provenance study of qumran pottery by neutron...

PROVENANCE STUDY OF QUMRAN POTTERY BY NEUTRON ACTIVATION ANALYSIS

PhD Dissertation

MÁRTA BALLA

BUDAPEST 2005

Table of contents Table of contents ........................................................................................................................ 0 Introduction ................................................................................................................................ 3 The scope of the work ................................................................................................................ 6 1. Science and archaeology .................................................................................................... 8 2. Archaeological chemistry................................................................................................... 9

2.1. Provenance Studies .................................................................................................. 11 2.2. Provenance studies of archaeological ceramics ....................................................... 12

2.2.1. “Best” elements ................................................................................................ 13 2.2.2. “Best” methods................................................................................................. 13

3. Neutron Activation Analysis............................................................................................ 15 3.1. Neutron Activation Analysis in archaeology ........................................................... 16

4. Principles of NAA............................................................................................................ 18 4.1. Irradiation ................................................................................................................. 18 4.2. Kinetics of activation ............................................................................................... 19 4.3. Standardization......................................................................................................... 20 4.4. Measurement and evaluation.................................................................................... 23

5. Performance capabilities of the INAA method ensuring privileged position among analytical techniques for provenance studies ....................................................................... 24

6. Analytical research and development .............................................................................. 26 6.1. “Strategic” developments......................................................................................... 26 6.2. Applied research....................................................................................................... 28 6.3. Operational activities................................................................................................ 28

7. Standard Operation Procedure for INAA of Archaeological Ceramics........................... 29 7.1. Analytical protocol ................................................................................................... 29 7.2. Estimation of uncertainty budget ............................................................................. 33 7.3. Method validation .................................................................................................... 34

7.3.1. Interlaboratory comparison and Proficiency Testing ....................................... 36 7.3.2. Intercalibration of laboratories ......................................................................... 37

8. Statistical evaluation of elemental data............................................................................ 39 8.1. Multivariate statistics for Qumran pottery data........................................................ 42

9. Qumran Pottery Project .................................................................................................... 44 9.1. The Dead Sea Basin ................................................................................................. 44 9.2. Scroll discovery........................................................................................................ 46 9.3. Excavations in Qumran ............................................................................................ 46 9.4. The function of the settlement.................................................................................. 49 9.5. The “Essene hypothesis”.......................................................................................... 50 9.6. Judean society in the Second Temple period ........................................................... 51 9.7. The Dead Sea Scrolls ............................................................................................... 53 9.8. Qumran pottery ........................................................................................................ 54

10. Chemical provenancing of Qumran pottery ................................................................. 57 10.1. Sample selection................................................................................................... 57 10.2. Reference material for Qumran............................................................................ 58 10.3. Analysis................................................................................................................ 59 10.4. Data processing .................................................................................................... 59 10.5. Analytical results.................................................................................................. 60

10.5.1. Chemical Group I. ............................................................................................ 61

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10.5.2. Chemical Group II............................................................................................ 62 10.5.3. Chemical Group III. ......................................................................................... 63 10.5.4. Chemical Group IV. ......................................................................................... 63 10.5.5. Chemical Group V. .......................................................................................... 63 10.5.6. Outliers ............................................................................................................. 64

10.6. Discussion ............................................................................................................ 65 10.6.1. West-East connection....................................................................................... 66 10.6.2. Inscriptions on Pottery (Ostraca)...................................................................... 67 10.6.3. Another source, providing complementary information .................................. 69

10.7. Summary .............................................................................................................. 69 Synthesis................................................................................................................................... 71 Tables ....................................................................................................................................... 74 List of samples ......................................................................................................................... 91 List of figures ........................................................................................................................... 96 Elemental data .......................................................................................................................... 97 Bibliography........................................................................................................................... 125 Acknowledgements ................................................................................................................ 133

2

Introduction

Introduction

Ancient manuscripts were discovered at various places during the last two centuries,

like e.g. Greek and Latin scrolls from under the lava of Herculaneum, Greek papyri and

Coptic Gnostic manuscripts from Egypt, but these never moved the Western world as did the

scrolls found in caves near Qumran, at the Dead Sea. These manuscripts, known today as the

Dead Sea Scrolls, dated to 300 BC-70 AD have over the last fifty-five years shed light on the

origins of Judaism and Christianity as well as providing insight into the political and religious

setting at a time of momentous importance.

To whom these manuscripts belonged, who wrote, copied, read these texts and hid

them into the caves, have always been controversial. The texts themselves do not give a

definite answer. Most part of the scrolls includes biblical texts, books of the Hebrew Bible,

another type is represented by apocryphal, and there are general writings, such as calendric

treaties or magical texts. A significant portion of the manuscripts however, of sectarian

character, belonging to a religious community: rules, exegeses and liturgical works.

Identification of this community is not clearly defined, but there is a consensus today,

that the Essenes, mentioned by the ancient authors, Flavius Josephus, Pliny the Elder, Philo of

Alexandria were the writers of the communal, sectarian texts, and the settlement, Khirbet

Qumran, excavated near the caves belonged to the Essene community. In the vicinity of the

settlement there is a cemetery of about 1200 graves that was also discovered.

The connection of the settlement with the cemetery and the caves, as well as the

function of the settlement, and the identity of the community have always been the object of

academic and religious debates. Generations of scholars have tried to answer the question:

who wrote the Dead Sea Scrolls? Were they written locally in Qumran, or were they taken

from other places? Do the descriptions of the ancient writers about the Essenes fit this

3

Introduction

community, and their description of the “wilderness” to Qumran? Do the settlers of Qumran

rest in the nearby cemetery? Were it the Essenes who used the caves and hid the scrolls there,

fearing the arrival of the Roman legions?

Scroll research was a continuous, dynamic process over the past fifty years, and

because of the very slow process of their publication, it always seemed mystical, nonetheless,

controversial. Archaeological research of the Qumran Complex (settlement, cemetery, caves)

however, led by Roland de Vaux, didn’t gain such a public attention. The excavation of

Khirbet Qumran was accomplished, investigation of the caves and the marl spur was

performed, material finds were placed into the vaults of the École Biblique et Archéologique

and in the Rockefeller Museum. Traditional archaeology finished its task.

The integration of flesh and spirit, archaeology and scroll research has been only a

recent endeavour, although Qumran provides a unique opportunity to the reconstruction and

understanding of the life of a community by

combining information from ancient authors, the

scrolls themselves, and archaeological evidences.

The texts and the antique literary sources provide

information that complement archaeology, while

archaeology establishes the direct connection

between the scrolls in the caves and the settlement at

Qumran.

The best evidence is provided by the pottery,

for the same unique ceramic types were discovered in

the settlement and in the scroll caves. In the first

season of Qumran excavations (1951) it was noticed

that “sunk into the floor of one of the rooms was a

jar, identical with most of those found in the Scroll

cave….We thus, even in the small area so far

excavated, have a direct connection with the Scrolls

“(Harding 1952). The most distinctive pottery-type associated with Qumran is, beyond doubt,

the cylindrical jar, the so-called scroll jar (Fig.1.).It represents a unique storage jar type,

frequent in Qumran, but completely unattested elsewhere. The ceramic assemblage shows a

Figure 1. Cylindrical scroll jar with lid (Davies 2002)

4

Introduction

number of peculiarities both in terms of types that are present and the types that are absent.

Most of the published papers on the pottery of Qumran are in agreement, that the pottery was

made at the site.

The study of pottery is always a powerful way to look into the life of early

civilisations. One can get a view into the technological level of pottery practice of a given

population, but one may learn about the development of trade, or simple human interaction

between groups of people. This applies to the Qumran settlement as it does to any other site.

Taking this into consideration, it seemed to be a logical step to study the ceramic

material unearthed at Khirbet Qumran and the surrounding caves, to cheque the validity of

this statement, by identifying specific characteristics of Qumran pottery, which give definite

answers concerning their provenance: chemical composition.

Archaeological ceramics all bear special chemical fingerprints which, appropriately

identified, can be used to trace the vessels back to where they were manufactured.

Instrumental Neutron Activation Analysis has been applied to Qumran pottery with a primary

objective of establishing their chemical composition and by that their provenience, thus

shading light on the closeness of the community, possible trade patterns and interregional

contacts.

5

Scope

The scope of the work

Within the past few years there has been a significant shift in the research interest

from classical archaeology to applying scientific techniques in an attempt to better understand

this ancient monastic community. This paradigm change has resulted in a new emphasis away

from the literary/historical emphasis of the distant past to an interdisciplinary synthesis

towards the human landscape.

The sciences provide archaeology with numerous techniques and approaches to

facilitate data analysis and interpretation, enhancing the opportunity to extract more

information from the material record of past human activities. Specifically, chemistry has as

much to offer as any other scientific discipline, if not more.

To determine the chemical profile of Qumran potteries and related materials, with a

special emphasis on trace element abundances, instrumental neutron activation analysis has

been applied. Reliable scientific information must be based on results produced by an

analytical technique, which has an appropriate accuracy, precision, sensitivity, resolution

power and fitness of purpose to be applied to the archaeological problem.

On the other hand, results of scientific provenance studies are irrelevant in themselves.

Where a vessel comes from is of limited value, unless it can be interfaced with an existing

social and economic structure, historical background, basic forms of human behaviour.

To meet the requirements of this twofold task, methodological as well as

archaeological research have needed, and the scope of the work summarized in the

dissertation was formulated as follows:

- to perform strategic (resource implementation) and applied (resource utilization)

research and development in the field of Instrumental Neutron Activation

Analysis, to fit the technique to provenance studies of archaeological ceramics

6

Scope

- to implement operational research, supporting investigations to improve the

performance and traceability of analytical work

- to accomplish a scientific approach to understand material culture with an

archaeologically coherent research design

- to trace the Qumran pottery by its chemistry to their place(s) of manufacture

- to establish the relation between the pottery found in the Qumran settlement and

the surrounding caves

- to study what pottery was locally made and which was brought in from elsewhere

to establish the cultural interactions with people near to or remote from Qumran.

7

Science and archaeology

1. Science and archaeology

Archaeology is one of the few disciplines that bridge the gulf between the humanities

and the sciences. The diversity of scientific analyses in archaeology can be summarized into

the following areas (Tite 1991):

- Physical and chemical dating methods which provide archaeology with absolute

and relative chronologies.

- Artefact studies incorporating provenance, technology and use.

- Environmental approaches which provide information on past landscapes,

climates, flora and fauna as well as diet, nutrition, health and pathology of people.

- Mathematical methods as tools for data treatment also encompassing the role of

computers in handling, analysing, and modelling the vast sources of data

- Remote sensing applications comprising a battery of non-destructive techniques

for the location and characterization of buried features at the regional, micro

regional, and intra-site levels.

- Conservation science, involving the study of decay processes and the development

of new methods of conservation.

It is easy to see, that chemistry is relevant to most, if not all of the areas.

Archaeological chemistry is not a straightforward application of routine methods, but a

challenging field of enquiry, making significant contributions.

8

Archaelogical chemistry

2. Archaeological chemistry

Chemical methods have been brought to bear archaeological importance ever since

chemistry became a recognizable science. At the end of the 18th century Klaproth determined

the composition of some Greek and Roman coins, and Roman glass pieces. H. Davy

examined ancient pigments from Rome and Pompei, Faraday proved the presence of lead in

Roman pottery glaze, and the list of the most eminent scientists could be continued (Pollard

1996). Since then, chemists in increasing numbers have been fascinated by the evidences that

chemical analysis can tell about ancient history, ancient ways of life, including technical

processes and the chemical substances, and patterns of trade in the ancient world.

In the middle of the 19th century, the Austrian scholar, J.E.Wocel first suggested that

correlations in the chemical composition could be used to trace the provenance, i.e. to identify

the source of archaeological materials. Some years later the Estonian Göbel made a

comparative study of a large number of metal objects from the Baltic region and that of

known artefacts of prehistoric, Greek and Roman date. With his work scientific analysis

progressed beyond the generation of analytical data on simple specimens to “establishing a

group chemical property” (Harbottle 1982).

The increasing number of archaeological objects soon called for restoration and

conservation methods. F.Rathgen established a laboratory at the State Museum of Berlin and

he published the first book on practical procedures for conservation of antiquities (Rathgen

1898). The end of the 19th century finally witnessed the first wet chemical investigations of

archaeological ceramics.

The beginning of the 20th century brought about instrumental measurement techniques,

like e.g. optical emission spectroscopy, and the scientific and technological developments

persuaded by the Second World War resulted in a wide range of scientific techniques to be

used for studying archaeological materials. The principles of neutron activation analysis

(NAA) had been set forth by this time too, but its widespread application was hindered by

technical and methodological difficulties.

9


The development of radiocarbon dating by W. Libby in 1949 is a real cornerstone

concerning the integration of hard sciences within archaeology (Libby 1952).

By the 1950s the new discipline of Archaeometry has been developed, covering the

involvement of chemical, physical and biological sciences within archaeology. A journal with

the same title started in 1958, illustrating the full potential of scientific endeavours in

archaeology. The term archaeometry is not favoured by now, as it has the danger of over-

emphasizing the “-metry” at the expense of the “archaeo-“, and has been modified to

archaeological science or scientific archaeology.

In the 1960s a wide range of scientific techniques was deployed to material remains.

The so-called golden era in archaeometry (Pollard 1996) brought about valuable contributions

in the determination of a wide range of chemical properties, including trace element

composition, scientific dating, mineralogy, isotopic distribution, biomarker composition, etc.

By the development of computers big data sets, generated by the measuring techniques could

be subjected to statistical treatment.

Sophisticated analytical techniques of the 80s-90s offered routine analysis of samples

in the milligram or smaller scale, running automatically under computer control, giving

information on any kind of physical and chemical properties of any kind of materials.

For quite a long time archaeology has paid more attention to the analysis of inorganic

materials – stone, metal, ceramics, glass, etc. Recently however, materials previously thought

to be lost, like ancient textiles, waxes and resins, food residues, human remains, including

bone, teeth, hair, protein, lipids and most recently DNA, are in the focus of research interest.

Organic chemistry, biochemistry, molecular biology has their techniques to offer to

archaeology.

As no analytical technique has “built-in interpretative value for archaeological

investigations” (DeAtley&Bishop 1991), the success in archaeological science, however, lies

in the degree of integration into relevant archaeological questions, in a contextually driven

research. Science and archaeology should focus on common objectives.

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2.1. Provenance Studies

Of all analytical work ever done on archaeological materials, provenance studies

undoubtedly account for the vast majority. The idea of diagnostic use of chemical

composition of artefacts for the characterization of the provenience, i.e. “chemical

fingerprinting” goes back to the second half of the 19th century, but widespread application on

ceramics, lithics, glasses and metals started in the 1960s-1970s.

The question of provenance in case of different rock-types, like e.g. obsidian, marble,

flint, jade etc., means the determination of the geographical source of the materials, quarries,

mines and deposits. In case of synthetic materials like ceramics, glass, or metals, where

production may result in significant changes in the chemical composition of the finished

objects with respect to the raw material, provenience is more complex and implies the place

of manufacture, production centre or workshop.

There are certain requirements for scientific provenance studies as summarized by

L.Wilson and A.M.Pollard (L.Wilson, A.M.Pollard 2001) as follows:

- The chemical characteristics of the geological raw material should be carried

through into the finished object.

- This fingerprint varies between the potential sources and this variation can be

related to the geographical occurrences of the raw material.

- Such characteristic fingerprints should be measured with sufficient precision in the

finished artefact, to enable discrimination between competing potential sources.

- It is essential to know that no mixing of raw materials, and no recycling has

happened.

- Post depositional processes either have negligible effect on the characteristic

fingerprint, or it can be detected.

- The interpretation of scientific provenance studies should be interfaced with an

existing appropriate socio-economic model. Any observed patterns of trade or

exchange are interpretable in terms of human behaviour.

11


2.2. Provenance studies of archaeological ceramics

Provenance studies of ceramics are a real success-story in archaeological chemistry.

Pottery was important in trade, and the composition of pottery is strongly related to the source

of clay and the recipe of the fabrication. This is highly site-specific and, although similar in

style and appearance, in critical cases it is possible to distinguish among products by

determining the chemical composition.

Clay deposits are extremely common and are found all over the world. The chemical

composition of a clay deposit is a complex product of the mineralogy of the rocks from which

the clay is derived, the weathering and transport processes effecting the production of given

deposit, and the chemical environment of sedimentation.

The basic constituents of pottery clays are clay minerals, i.e. hydrated aluminium

silicates. Within the basic phyllo-silicate structure some minor constituents, present to the

order of a fraction of 1 percent to several percents are also found. The raw clay used for

pottery contains, in addition to the clay minerals, residual components of the original rock,

and other materials that are picked up during the transport.

Ceramic producing procedures might involve washing, levigation, mixing clays from

different deposits, and adding temper, in order to obtain workable plasticity, to provide

porosity and diminish shrinkage during firing. Ceramics are fired at temperatures between

700-1400 oC, with a wide range of chemical reactions taking place during firing, depending

on the mineralogical composition of the clay and the temperature and condition of firing.

It is obvious that this anthropogenic manipulation of the raw material makes it highly

difficult to trace vessels back to raw clays, and usually it is not attempted. Ceramic

provenancing almost always means tracing potteries to production places, where both

geochemistry and potters’ practice are covered. The normal procedure is to compare the

finished pottery with fired pottery of certain, or assumed provenance. Most commonly

“control groups” are established from kiln wasters, or by comparison with material of

impeccable provenience.

12


Over the last twenty years there have been heated debates about the most informative

elements and the most appropriate analytical technique for source discrimination. A number

of instruments and analytical protocols may fulfil provenance objectives with the ability of

determining a wide range of elemental concentrations.

2.2.1. “Best” elements

Clay minerals are composed of the major structural elements Si, Al, and O. Minor

elements (0.1%-10%) such as Ca, Fe, K, Na, Ti and Mg can be both technological and

provenance discriminators. Trace elements (below 0.1%) are considered to be accidental, and

thus provenance-related. While changes in the concentrations of the main and minor

components are restricted by stoichiometrical rules, trace elements are more variable in clay

sources. Also, trace elements are less susceptible to anthropogenic control, than the major and

minor elements, which are more likely to influence the firing and performance characteristics

of the pot. The majority of chemical provenance studies carried out since the 1970s have

utilized trace element data.

2.2.2. “Best” methods

For scientific provenance analyses the following requirements have to be considered:

1. A logical demand is that analyses must give information on as many elements as

possible, so as to get an overall picture of the periodic system.

2. The method should be sensitive enough for the determination of trace elements.

3. Analyses, coming from the nature of the problem, should be carried out in series of

samples, too, so phases from the preparation of samples to the results received, should

not contain time-consuming processes.

The aim is to apply a well-automated measuring technique, which assumes a sensitive

determination of trace elements at the same time ensuring the objectivity, reliability and

reproducibility required by the task.

13


The most common methods of elemental analysis for ceramics are atomic emission

spectroscopy (AES), atomic absorption spectroscopy (AAS), X-ray fluorescence spectroscopy

(XRF), neutron activation analysis (NAA) and inductively coupled plasma spectrometry

(ICP).

Atomic emission spectroscopy is a simultaneous, selective technique, suitable to

measure virtually any element present in a powder sample of 10 mg, in concentrations

between 0.001% and 10%. It is quite difficult to standardize (photographic procedure) and the

reproducibility of the measurements is affected by some technical parameters.

Atomic absorption spectrometry provides a rapid and effective means of analysis, but

has the disadvantage of being sequential instead of simultaneous character. Sample

preparation is quite difficult, samples have to be dissolved. Reproductivity problems can be

significant as well.

X-ray fluorescence spectrometry is the most surface sensitive of the analytical

techniques, which can be a critical restriction. Although it can be non-destructive, for

unprepared samples standardization is quite problematic. For prepared, i.e. fusioned glass

bead samples and using a wavelength-dispersive system the method has the required trace

element sensitivity, but this protocol has relatively little use on archaeological materials.

Inductively coupled plasma atomic emission spectrometry (ICP-AES) is a quasi-

simultaneous multielemental technique, sensitive for the determination of trace elements. Its

main disadvantage is that it needs dissolved samples.

Connecting up the ICP torch to a mass spectrometer gives the powerful technique of

inductively coupled plasma mass spectrometry (ICP-MS). It makes possible to determine the

concentration of individual isotopes, or the ratios of specific isotopes of a given element. Its’

sensitivity is prominent, but still has the disadvantage of requiring a sample solution. There

are different approaches to overcome this problem, like slurry nebulization or laser ablation.

The following description will show that neutron activation analysis satisfies all the

mentioned requirements. This is the most widespread analytical technique applied in studies

on the provenance of archaeological ceramics.

14

Neutron Activation Analysis

3. Neutron Activation Analysis

Neutrons were discovered in 1932 and within four years the principles of neutron

activation analysis had been set forth by Hevesy and Levi (1936). They determined the

dysprosium content of an yttrium sample, using a radium-beryllium neutron source, Geiger-

Müller tube for beta-counting, while element identification was based on half-life. Because of

the lack of high-flux neutron sources and gamma ray spectrometry equipment the method was

slow in developing. Nevertheless, the initial development was combined with skilful

advancements in radiochemistry, as multi-element samples had to be treated via tedious post-

irradiation radiochemical separations (P.Guinn 1999).

The construction and rapid distribution of nuclear research reactors after the Second

World War has been of great help to the development of activation analysis. Radiochemical

separations were still essential, as counting was possible by Geiger or proportional counters.

The appearance of the NaI(Tl) scintillation detectors in the 1950s, coupled with the newly-

developed pulse-height analyzers paved the way to gamma-ray spectrometry. The electronic

revolution, with the development of transistors, computers and solid-state detectors has made

a real impact in the field.

In the early 1960s the lithium-drifted germanium semiconductor detectors were

invented, with an energy-resolution of some 20-30 times better, than was possible with a

NaI(Tl) scintillation detector. By 1970 Ge(Li) detectors with sensitive volumes approaching

1000 cm3 and multi-channel analyzers of 4096 channels had become commercially available.

Progress in the field of gamma-spectroscopy made possible the instrumental neutron

activation analysis (INAA) of multi-element samples. The method proved to be applicable in

a great variety of fields, the annual publication rate had risen to about 1000 (P.Guinn 1990)

During the 1980s the high-purity germanium detectors began to replace the Ge(Li)

detectors, the development in nuclear electronics proved to be a constant dynamic process,

just as the development of computers and computer programs to process the data.

15


It can be stated that up to the 1970s INAA was undoubtedly the only highly sensitive,

quantitative, multi-elemental analytical method available. Its unique position, nevertheless,

has been challenged by other increasingly sensitive and versatile analytical techniques, like

AAS, ICP-AES and ICP-MS, which today are used widely in applications that previously had

been a domain for NAA. A variety of activation analysis techniques have emerged, though,

that complements classical NAA and increases its capabilities. INAA still occupies a solid

position in analytical chemistry, it is competitive with or superior to most methods when

precise and accurate data are needed. It has the advantage that solid samples can be analysed

directly reducing the hazards of contamination that emerges during sample dissolution. The

highest competitor will be the ICP-MS with laser ablation in the future.

3.1. Neutron Activation Analysis in archaeology

NAA has been used on archaeological material from the early fifties. The earliest

publication is from Ambrosino and Pindrus (1953), they studied coins from the collection of

the Louvre. In 1956, at the suggestion of R.Oppenheimer, a conference was held in Princeton,

(Asworth 1966) to examine the possibility of the use of nuclear techniques to help solve

archaeological problems. As a result of this meeting, work started at the Brookhaven National

Laboratory and in the Research Laboratory for Archaeology at Oxford. E.Sayre made the

initial study on Mediterranean pottery (1957). In an evaluation of this work it was concluded,

that the results were encouraging, and that specific questions of archaeological analysis could

be answered by neutron activation analysis. V.M.Emeleus pioneered the technique in Britain,

and applied it mostly to terra sigillata (Emeleus 1958, 1960).

The first archaeological applications of INAA were primarily methodological in

nature, with the broadly posed archaeological question: Is this type of pottery chemically

different from the other one? By the development of the instrumentation the number of

elements, that could be determined and quantified, and the capabilities of the method

increased considerably. Main contributors of this period were Asworth and Abeles, Sayre and

Dodson. For more than two decades, the two major laboratories in this field were the

Brookhaven National Laboratory and the Lawrence Berkeley Laboratory.

16


This period culminated in the work of Isadore Perlman and Frank Asaro. With a

systematic theoretical as well as practical work of indisputable importance, they developed a

high precision INAA technique, making measurements accurate to the 1% level for most of

the elements, which should be good enough to make the distinctions between clay fingerprints

from different potteries. Protocols for the analysis and for a possible statistical data-treatment

are basic contribution to the field. Besides, they prepared and calibrated the first multi-

element standard of fired clay, called standard pottery, which became one of the most highly

regarded multi-element standards in the field of NAA. (Perlman 1969, 1971)

Perlman proved that the implementation of the newly developed method is not less

important than the accurate analysis. One of his major efforts was the development of a data

bank of reference clay-sources and groups of pottery of known origin, whose fingerprints

could be compared with those of ancient pottery. With his research group he tackled many

archaeological projects, mostly in the Mediterranean and in Palestine. (Perlman 1970, 1986)

Neutron activation laboratories specializing in the provenance of pottery with similar

procedures started in France (Widemann 1975, 1978, 1980), Israel (Perlman 1981,

Gunneweg 1983,1985, Yellin 1978,1985) and Germany (Mommsen 1987, 1988, 1992). The

most productive period of NAA laboratories in this field was the 1980-1990s, teams from the

University of Toronto (Hancock 1985, 1986), the Missouri University Research Reactor

(Glascock 1992, 1993., Neff 1992, 1993), the Demokritos Reactor Centre (Kilikoglou 1984,

1995), The University of Sofia (Kuleff 1986, 1996, 1998) reported valuable works on

different material remains of our cultural heritage, originating from the most different context

in space and time.

It can be stated that for at least two decades the standard analytical method for

producing multi-element analyses with detection limits at the ppm level or better has been

INAA, and in spite of the difficulties resulting from the decline in acceptance of nuclear

power, is still marketable. The two most competing techniques today are PIXE and ICP-MS.

INAA however is competitive with or superior to most methods when precise and accurate

data are needed.

17

Principles of NAA

4. Principles of NAA

A brief summary is given below on the theoretical aspects of NAA, to demonstrate

that its performance capabilities undoubtedly ensure its privileged position among trace-

element techniques implemented in archaeological science.

The basic idea of NAA is that irradiating a sample by neutrons high-probability (high

cross-section) nuclear reactions are induced, producing from stable isotopes of different

elements concerned radioactive nuclides, whose characteristic radiations can be used both to

identify and accurately quantify the elements of the sample.

The radioactive decay is characterized by its half-life, which can be on a wide scale

from the fraction of a second to several years. Most nuclides stabilize by β-decay, but the

emission of β-particles is often accompanied by discrete gamma radiation.

Determinations are based on the detection of the highly penetrating γ-photons of

discrete energies. Gamma energies of different nuclides are spread over the interval from

some keV to some MeV.

The measurable parameters for qualitative analyses are the energy of the emitted γ

quanta (Eγ) and the half-life of the nuclide (T1/2). For quantitative analysis the intensity (Iγ) is

used, which is the number of γ-photons of energy Eγ, measured per unit time.

4.1. Irradiation

There are various types of neutron sources according to the needs and availability.

Nevertheless, the most efficient neutron sources for high sensitivity activation analysis are the

nuclear reactors, operating in the maximum thermal power region of 100 kW – 10 MW, with

a thermal neutron flux of 1012 – 1014 neutrons cm-2 s-1.

18

Principles of NAA

4.2. Kinetics of activation

In the case of neutron induced nuclear reactions, the activity of the studied nuclide

depends, beside the number of target atoms, on the flux of the neutrons and the macroscopic

cross-section of the given nuclear reaction. Both cross-section and neutron flux depend on the

neutron energy, therefore the basic activation equation is:

∫0

)()( dEEENNR 4.2.1.

Where N is the number of interacting nuclides, σ(E) is the cross-section [in cm

∞

Φ(E) is the neutron flux per unit of energy interval [in cm-2s-1eV-1], and R is

the rea

lower limit of

e epithermal component of neutron spectra is 0.55 eV, the Cd cutoff energy:

Φ⋅⋅=Φ⋅⋅= σσ

2] at neutron

energy E[in eV] ,

ction rate.

When irradiation is performed in a nuclear reactor, the integral in Eq. 4.2.1. is replaced

by a sum of two integrals, separating the thermal and epithermal regions. The

th

)( 0INRRR eththepith ⋅Φ+⋅Φ⋅=+= σ 4.2.2.

s the resonance integral (cross-

ection in epithermal region) for the 1/E epithermal spectrum.

factor . Subsequent to the irradiation the nuclide decays exponentially. The decay

where Φth is the conventional thermal neutron flux, σth is the effective thermal neutron cross-

section, Φe is the conventional epithermal neutron flux, and I0 i

s

The activity (A) is time dependent. During irradiation the activity of the produced

radioactive nuclide grows according to a saturation characteristic, governed by a saturation

1 iteS λ−−=

factor is dteD λ−= .

DSINA ethth ⋅⋅⋅Φ+⋅Φ⋅= )( 0σ 4.2.3.

here t is the irradiation time and t is the decay time.

activity. The measured

arameter is the total peak area (Np) at a particular energy, given by:

w i d

The intensity of the measured gamma line is proportional to the

p

mp tfAN ⋅⋅⋅= γγ ε 4.2.4.

19

Principles of NAA

where εγ is the efficiency of a semiconductor detector (depends on gamma-energy), fγ is the

mission probability of a gamma photon at a given energy, and tm is the measuring time.

he unknown mass (mx) of element x can be expressed as follows:

e

T

mx = meththiAv

p

fN

MN

⋅

⋅

tDSIfx

⋅⋅⋅Φ+⋅Φ⋅⋅⋅ )( 0σεγγ

4.2.5.

here NAv is the Avogadro number, fi is the isotopic abundance and m is the mass of the

radiated element.

Absolu

n from literature, especially those on decay schemes and activation cross-

ections can sometimes be significant, comparative analysis with a standard sample is much

ften performed.

Classic

, followed by the measurement of the ratio of counts Npx / Npst . If the conditions for

oth irradiation and counting are identical, the ratio of masses mx / mst equals to the ratio of

w

ir

4.3. Standardization

te method

Equation 4.2.5. provides the basis for quantitative activation analysis. The unknown

mass can be determined if all other parameters are accurately known. By determining the

neutron flux and measuring the absolute gamma-ray activity, a direct calculation of

concentration can be done by applying the necessary nuclear constants. As uncertainties of

nuclear data take

s

o

relative method

A relative standardization can be performed by the simultaneous irradiation of the

sample with standards of known quantities of elements in question in identical reactor

positions

b

counts:

20

Principles of NAA

mx = mst stpN ,

4.3.1.

The accuracy of the relative standardization method depends on the standard

preparation pr

xpN ,

ocedure. The use of mono-elemental standards results in time consuming

easuring processes, but there are multi-elemental certified reference materials for different

ample types.

Single

f an experimentally determined composite nuclear constant k-factor.

As this

determination of the k-factors by

irradiating known quantities of the elements concerned together with the known quantity of

m

s

comparator method

This technique is based on the co-irradiation of the sample and of a neutron fluence

rate monitor and the use o

method has been used during this work, its description is more detailed here than for

the previous procedures.

The method has two phases, the first is the

the selected comparator element. k-factors are defined as

k = *spI

4.3.2.

I

spI

sp = N

mCDSp

⋅⋅⋅ and C =

λ

λ mte−−1 4.3.3.

here C is the counting factor which considers the decay during the time of the measurement

e parator. Theoreticall

equation:

k

w

(tm ) and the * refers to th com y the k-factors are calculated from the

= )()(

*0

****0

*

QfffMQfffM

thi

thi

+⋅⋅⋅⋅

+⋅⋅⋅⋅

γγ

γγ

εσεσ

4.3.4.

where e

thfΦΦ

= and th

IQ

σ0

0 =

21

Principles of NAA

This means that the k-factor depends on the thermal/epithermal neutronflux-ratio of

the irradiation position and on the efficiency curve (ε(E)) of the detector, that is they are valid

irradiation and measurement conditions. Valu -

factors are stored in a library.

ical phase, samples are irradiated together with the chosen comparator

lement (in most cases Au is used), and the mass of the element concerned is calculated by:

only under well-defined es of the defined k

In the analyt

e

m = *spIk

I cor

⋅ 4.3.5. and

CDSN

I pcor ⋅⋅

= 4.3.6.

k standardization 0

0 s

independent of the irradiation and measuring conditions. k0 factors are calculated according to

DeCorte (1987) defined the k -factors as a composite nuclear constant which i

the following equation:

***

*

0thi

thi

ffMffM

kσσ

γ

γ

⋅⋅⋅

⋅⋅⋅= 4.3.7.

The literature values can be checked by determining the k0-factors through measuring

the specific intensities, if the Φth / Φe ratio and the efficiency curve of the detector is known:

)()( *

0*

*0 QfQf

II

k sp

+⋅

+⋅⋅= γ

εε

0sp γ

4.3.8.

Using the commercially available k0 computer program the standardization procedure

plified. The program makes possible to avoid systematic errors during

the standardization procedure, like e.g. the gamma-attenuation effect, the changes of

ects, and epithermal flux deviations. This

method is a very promising contribution of NAA development.

can be avoided or sim

measuring geometry, the true-coincidence eff

22

Principles of NAA

4.4. Measurement and evaluation

Gamma-spectrometry systems are used to process the induced radiation of the

different nuclides produced in activated samples.

Gamma measuring systems are based on high-purity germanium semiconductor

detectors. The most important characteristics of the detector are its efficiency and resolution.

The detector is connected to a multi-channel analyser (MCA) by an appropriate electronic

system (preamplifier, spectroscopy amplifier, analogue-digital converter). MCAs are

computer based systems with the ability of spectrum evaluation. There are data acquisition

software for calculating the energies and the areas of the total energy peaks, enabling the

calculations of qualitative and quantitative characteristics of the nuclides.

23

Performance capabilities of NAA method

5. Performance capabilities of the INAA method ensuring privileged position among analytical techniques for provenance studies

Referring back to Chapter 2.2.2., outlining the requirements of analytical methods to

fulfil provenance objectives, the following conclusions can be drawn:

1. In order to take advantage of the differences resulting from different geological

layouts, it is logical that as wide an elemental range as possible should be measured,

encompassing great diversity in chemical properties.

Almost all elements subjected to neutron irradiation have a given probability of

interacting with neutrons, and at least one of the isotopes will be partially converted to a

radioactive form. By optimized irradiation and counting procedures about 30-35 elements can

be determined by INAA.

Nuclear reactions are independent of the chemical form of an element and their

chemical environment. Reaction probabilities (i.e. cross-sections) are functions only of the

energy of the bombarding neutrons and the characteristics of the nuclei. As a result, there are

no preferred chemical properties, all groups of elements of the Periodic Table are represented.

2. As trace element distribution of chemical pastes is site specific (see 2.2.1.), the

analytical method must be sensitive for their determination.

INAA does not measure all elements with equal sensitivity. Cross-section, isotope

abundance, half-life, emission probability of the given nuclide are the nuclear characteristics

determining sensitivity, but the measuring technique can influence it, too. INAA using

thermal neutrons can determine two thirds of the elements of the Periodic Table with

sensitivities at the ppm level or below, and these are mostly trace elements.

The method is not suitable however for some light elements. Concerning major

components of clayey materials, some either do not activate at all (e.g. O), they do poorly

(e.g. Fe), they have short-lived radionuclides which decay rapidly (e.g. Mg, Ca, Cl), or there

are interfering activation reactions making determinations difficult (e.g. Si, Al).

24

Performance capabilities of NAA method

3. In order to get a statistically meaningful data-set, analyses should be carried out in

series of samples.

The method is chemically non-destructive, samples do not have to undergo any

chemical treatment, neither prior, nor after activation, sample preparation involves only the

handling of representative samples, powdering, mass determination and packing. Phases of

analysis can be fully, or partly automated, so there are no laborious or time-consuming

processes. Standardization is potentially easy and accurate. Contamination hazard is easily

avoided by careful sample treatment.

Standardization is potentially easy and accurate.

Also objectivity is provided by the exploitation of automation, the risk of systematic as

well as random errors is reduced.

Summarizing the abovementioned points, it can be stated that INAA lends itself to a

successful provenance study by having different advantages inherent to the underlying

physical principle of the method.

25

Analytical research and developments

6. Analytical research and development

INAA technique is considered to be “mature”. The emphasis in this research program

has been shifted towards strategic developments and applied research (Bode 1996), to make

the existing knowledge on the technique available for utilization and to demonstrate its full

potential.

To go beyond the trivial level of applying INAA technique to archaeological ceramics,

laboratories have to develop and optimize the method, tailoring it to the special technical and

practical resources.

6.1. “Strategic” developments

Specific demands set by the task have been considered, theoretical and practical

aspects of resource implementation were studied as well.

The research reactor at our disposal is a low-flux reactor, with several irradiation

possibilities, characterized by different spectral variations of the neutron-flux. The

determination of the thermal neutron-flux, the Cd-ratio and the thermal/epithermal flux-ratio

has been performed by different methods through the years. Based on these data irradiation

channels with the highest thermal neutron-flux were chosen (G4 and G6 positions, see Fig.2.)

and the spatial and spectral variations of the neutron-flux in these positions has been

investigated. The optimal size of the irradiation vials, the number of samples, monitors and

standards per batches were defined.

Provenance studies require multi-elemental data of big sample sets, so standardization

must be simple, but accurate. Single comparator method has been chosen as standardizing

procedure, and proved to be appropriate for the accurate quantification of major, minor and

trace elements in pottery samples. By independent experiments k-factors for the most

important (n,γ) reactions and γ-ray energies of the resulting isotopes were determined. (Table

1.)

26


In the attempt to optimize the analysis of pottery, one of the primary questions was to

decide which elements provide the most important information for chemical discrimination of

ceramic materials. The diversity of the parent rocks and the complexity of geochemical

fractionations in the formation of clay beds result in specific distribution patterns of elements

in different sources of pottery clay. The fingerprinting process is usually not concerned with

any specific elements, but rather with an array, providing a pattern, which varies in a sensitive

manner. This sensitivity is provided by the trace elements (see 2.2.1.), their great variability

assumes more certain separation. To demonstrate this, in Table 2. trace element data of some

clay minerals from different regions of Hungary are presented.

Results showed that the kaolinites of the same structure but different genetics and

occurrence point to a wide diversity in respect of their trace-element composition. The

difference in the elemental concentrations sometimes can be greater than concerning two

structurally different clay minerals, e.g. illite and kaolinite. It is remarkable, that the trace-

element distribution of kaolinites from Szegi and Mád differ considerably, although they were

formed by the same rock-forming process, deposited geographically not far from each other.

Archaeological ceramics of different dates, pastes and fabrics have been analyzed in

great number, too, to get information on their trace-element composition.

To define the final set of elements to be determined in pottery samples, some specific

features of the nuclear measuring technique have also been considered. To ensure the lowest

detection limit and measuring uncertainty, the radioisotope, i.e. the gamma line of it which

yielded the greatest peak/background ratio free of spectral disturbance was chosen. These

conditions are significantly influenced by the choice of irradiation-, cooling and measuring

times, and measuring geometry, so care was taken to set the timing protocols and to fix the

counting geometry.

Different sampling techniques has been tested, and was found, that grinding by a

diamond-coated drill bit provides uncontaminated powder samples of appropriate particle

sizes. The amount of sample taken has to balance between limiting the damage to the

ceramics and the accurate and precise determination of a large number of elements.

On different ceramic types homogeneity studies were performed, to check, whether a

simple sample of about 50 mg can be considered representative for a whole vessel. Although

it proved to be true for fine wares (see Table 3.), a test is recommended for each pottery type

when starting a project.

27


6.2. Applied research

The implementation of the method, fitted by these experiments to the special

characteristics of the laboratory’s resources resulted in successful contributions in many

archaeological studies (Balla 1998, 1999).

The characteristic feature of radioanalytical work, i.e. sophisticated techniques on

special samples presumes a research oriented activity, with a dynamic method-development

and a constant improvement of effectiveness and reliability. A kind of quality culture has

always been involved in this field.

However, in the early 90s, by the appearance of ISO standards it was soon realized,

that there is a need and responsibility to implement a quality control and quality assurance

system, according to the guidelines and norms of an international standard.

Accreditation requires a transparent, high-level, and thoroughly documented analytical

activity, and decrees, that for non-standard test methods procedures should be developed,

containing full description of the given analytical process, with clear specifications of the

samples, standards, and equipment. The so-called standard operation procedure should cover

uncertainty budget estimation and should give criteria for approval or rejection.

During the accreditation process, procedures, instructions, forms (PIF) have been

defined for all the relevant equipment and the Standard Operation Procedure (SOP) for INAA

of Archaeological Ceramics has been prepared.

6.3. Operational activities

Performing these research tasks involves operational activities, to support

investigations and management work, so as to improve the performance and traceability of the

laboratory’s activity.

A five-year work of improvement, fulfilling scientific, technical and management

requirements, demonstrating the quality of work and crediting the methods, led to the

accreditation of the Radiochemistry Laboratory according to ISO/IEC 17025 International

Standard.

28

Standard Operation Procedure for NAA of Archaelogical Ceramics

7. Standard Operation Procedure for INAA of Archaeological Ceramics

This procedure, resulting from the strategic and applied research, which was supported

by operational activities, comprises the analytical protocol, the estimation of uncertainty

budget of pottery analysis and the validation of the method in Quality Control/Quality

Assurance system.

7.1. Analytical protocol

A detailed description of the procedure covers all phases of the analyses, and directs as

follows:

Sampling and sample preparation

Sampling is done by the use of a diamond drill-bit, on a freshly-cleaned surface of the

pottery, where no glaze or other type of finishing material is found. The sample should weigh

about 50-100 mg, if there is no constrain. In certain cases the sample may not be

representative, but it is determined by availability.

Powder samples then are fired in a furnace, for one hour duration, on 600 0C, so as to

get rid of moisture, organic materials, and to ensure identical starting conditions for all

samples. After cooling, samples are weighed into polyethylene irradiation capsules.

Gold is used as comparator element, and zirconium foils serve as flux-monitors. Three

pieces of 0.1%Au-Al alloy disc of 5mm diameter and two pure zirconium foils of the same

size are weighed, too, and packed together with fifteen ceramic samples and one sample of

reference material(RM) into one batch. RM type and analyte concentration range have to be

chosen as similar as possible to those of the samples. From our laboratory’s resources for

ceramics NBS SRM 1633a Coal Fly Ash, or GWB 07313 Marine Sediment are the most

appropriate.

29


Irradiation

Irradiations should be done

using either the G4 or the G6

vertical irradiation channels (Fig.

2.), with maximal 100 kW reactor

power, for eight hours. Irradiation

capsules are opened after a

cooling-time of five-six days.

Measurements

γ-spectrometric

measurements are performed on

one of the two gamma-

spectrometers of the Laboratory.

Each has a HPGe semiconductor

detector, connected through

appropriate nuclear electronic

devices to multichannel analyzers.

Measuring system specifications

are as follows: Figure 2. Horizontal cross section of the core of the nuclear reactor at the Institute of Nuclear Techniques

Gamma-spectrometer #1

Detector: HPGe-Well GCW 2022 Canberra, with a 2002CSL preamplifier

FWHM: 1.95 keV (1332 keV)

Rel.efficiency: 20.5%

HV Supply: NB-850 KT(ATOMKI) 5kV

Spectroscopic amplifier: 2020 Canberra

ADC: 8075 Canberra

MCA: S-100 Canberra, 2x8k

Software: SAMPO-90

30


Gamma-spectrometer #2

TOP

1.90 keV (1332 keV)

EC

anberra

lanned and documented quality control measurements are performed by both

equipm

nce the irradiation capsule is opened, samples and metal foils are unpacked. The first

measur

alculations

y the evaluation of Zr and Au spectra, corrected specific intensities are calculated,

and the

ed in Table 4.:

able 4. Nuclear data of Au and Zr isotopes

Eγ(k

Detector: HPGe POP

FWHM:

Rel.efficiency: 23%

HV Supply: NB-850 KT(ATOMKI)

Spectroscopic amplifier: 572 ORT

ADC: ND 579 Canberra

MCA: ACCUSPEC-B 8k C

Software: SAMPO-90

P

ent, control charts of resolution and efficiency values are recorded, action levels are

defined. The analyst has to be sure that γ-spectroscopic measurements are carried out using

equipment that is within specification, working correctly and adequately calibrated.

O

ements after 5-6 days-long cooling time are performed on the zirconium foils, then the

samples are counted for 5-8000 seconds each. An automatic sample changer ensures identical

measuring geometry not only for all samples but also for the comparators. A second

measurement after about one month is performed, the measuring geometry is kept unchanged.

C

B

thermal/epithermal flux-ratio is determined as well.

The most important nuclear data of Au and Zr are list

T

Isotope eV) T1/2 (s) Q0

198Au 411 232934 15,71 95 Zr 724 5532192 5,05 97Zr 743 60264 248,00

743 60264

31


According to Eq. 4.3. -facto depends on the thermal per epithermal ratio of the

irradiation position and on the efficiency curve of the detector. Using nuclides with different

I /σ va

4. the k r

0 0 lues (i.e. Zr) the flux ratio is controlled, and reference k-factors (kref), taken from the

library, are converted to an analytical (an) channel where the actual irradiation is performed:

)()()()(

00 refan*

00

QfQfkk refan

refan +⋅+⋅= 6.1.1.

*QfQf +⋅+

The evaluation of the saved sample-spectra is performed by SAMPO-90 software.

Peak identification by gamma-energies, and peak area determination by fitting an analytical

function to the peak is done interactively.

Using the k-factor library and the actual spectral parameters, calculation codes give

the elemental concentrations.

The set of elements determined through these processes are as follows:

As, Ba, Ca, Ce, Co, Cs, Cr, Eu, Fe, Hf, K, La, Lu, Na, Nd, Rb, Sb, Sc, Sm, Ta, Tb,

Th, U, Yb, Zn

Acceptance criteria

Results of analyses can be accepted if

- deviation of specific intensities of Au foils is below 10%

bigger value, especially when tendency is noticed, indicates a bad positioning

of the irradiation vial in the reactor core

- concentrations calculated from the first, and the second run agree within measuring

uncertainties

which justifies the qualitative determination (half-life), the use of a consistent

measuring geometry, and correct calculations

- calculated concentrations for the analysed reference material pass the u-test for

each element, where

29.3)(/ 22 ≤−−= refmrefm uuccu

by which the accuracy of the measurements can be verified

32


7.2. Estimation of uncertainty budget

The basic equation for the calculation of the concentration of the measurand, using

single comparator standardized INAA is

x

p

xxx

xp

spx

xspx

Ic =

kmCDS

N

CDSmIk1/ ****

*,

*, ⋅

⋅⋅⋅⋅⋅⋅=

⋅ 6.2.1.

etermined according to this equation,

based o

stimated, taking into account all recognised effects

influencing the results (Balla 2004).

inties due to sample preparation,

irradiation, gamma-ray spectrometry and standardization.

e the standard uncertainty of counting statistics is given by the gamma software SAMPO-

90.

N

Uncertainties of elemental concentrations are d

n the law of error propagation.

Although results, i.e. elemental concentration data, have never been sent out without

uncertainties, prior to the elaboration of this procedure uncertainty was not fully evaluated. In

most cases only counting statistics were given as measurement uncertainty. By now, a

combined standard uncertainty is e

INAA has unique sources of uncertainties which can be grouped according to the

individual steps of analysis into four categories: uncerta

Table 5. comprises and quantifies all investigated uncertainty components of INAA

and refers to uncertainties due to impurities of irradiation vials (Table 6.), varieties of sample

quantities (Table 7.), and the determinations of k-factors (Table 8. and 9.). There are

quantities (numerical values) ,which are estimated by statistical evaluation of measured data

(weighing, vial impurities, neutron-flux gradient, dead time effect, uncertainty of k-factors),

others taken from certificates (gold and zirconium foil concentration-purity- uncertainties ),

whil

33


Evaluating uncertainty budget it could be concluded, that the main components are :

the uncertainty of net peak areas, k-factors, sample masses, dead-time correction, and

standard deviation of intensities of gold foils. The combined standard uncertainty is calculated

according to the law of propagation of uncertainties.

is the p

ference materials proved to be appropriate, as RM type and

nalyte concentration range made it possible. Interlaboratory comparisons were performed,

o, as it will be reported later.

he following performance parameters were examined:

ove 10

pm, correction is needed for Ce, La, Ba and Nd. If the cobalt content is below 1 ppm, the

ite-specific background cobalt activity of our laboratory has to be taken into account.

7.3. Method validation

To meet the requirements of the ISO/IEC 17025 Standard, the laboratory has to

validate its non-standard, laboratory developed methods, i.e. it should be proved, that it is fit

for the particular, intended use. Method validation, by definition (EURACHEM Guide, 1998),

rocess of establishing the performance characteristics and limitations of a method and

the identification of the influences which may change these characteristics and to what extent.

Of the possibilities offered by the Standard for the determination of the performance

of the method the analysis of re

a

to

T

Selectivity:

The ability of the method to determine accurately and specifically the given nuclide in

the presence of other components in a sample matrix is good, due to high resolution gamma-

spectrometry. The proper analytical gamma lines have to be chosen, spectral interferences

should be avoided. Selectivity is violated, if e.g. the concentration of uranium is ab

p

s

34


D ion limit:

The detection limit dep ground and can be calculated

according to Currie’s equation:

etect

ends on actual gamma-back

BGD NL ⋅+= 29.371.2 where NBG is the background at

the given energy of the gamma-spectrum. Typical values for some elements are presented in

able 10.

ndependent of the

matrix) s ough:

amma self-absorption (e.g. determination of elements in lead)

- high dead-time

are available on

o detectors, results are controlled by measurements of reference materials.

b

with each batch of samples to check whether the results pass the accuracy

riteria, i.e.

T

Linearity:

Theoretical basis of NAA (the signal to concentration ratio is i

en ures linearity of the method, there are some exceptions th

- sample contains neutron absorber (e.g. boron, cadmium)

- in case of high g

Robustness:

The procedure is capable to remain unaffected by small, but deliberate variations in

method parameters. Intra laboratory studies were performed by measuring samples on both

gamma spectrometers. Results proved the reliability of the method. k-factors

tw

Accuracy:

Closeness of the agreement etween the results of a measurement and a true (accepted

reference) value of the measurand is characterized by u-test. Certified Reference Materials

are analysed

c

29.3)(/)( 22 ≤+−= refmmref uuccu 6.3.1.

Table 11. and Table 12. present the measured concentration data compared with reference

values for NBS SRM 1633a Coal Fly Ash and Perlman/Asaro Standard Pottery. As can be

seen, all results meet the acceptance criteria. It is stated in the SOP, that analytical results are

acceptable only if the concentration values of the reference sample pass the u-test, and with

no reasonable explanation to any discrepancy, the measurements have to be repeated.

35


Pr on:

Results of successive measurements of GBW 07313 Marine Sediment Certified

Reference Material samples are given in Table 13. Five sam

ecisi

ples were analysed under

peatability conditions. Precision index was defined as follows:

re

25.0)/()/( 22 ≤+= mmrefref cucuP 6.3.2.

The standard deviation of the concentrations in all five measurements is lower than the

calculated uncertainties, precision index is lower than 25% for all elements, the results are

s the method

suitable for providing accurate analytical data for ceramic provenance studies.

7.3.1. atory comparison and Proficiency Testing

terlaboratory

comparisons or proficiency programs. Examples for both are presented below.

(INCT-TL-1) and Mixed Polish herbs (INCT-MPH-2) were to be determined.

acceptable.

Summarizing the validation process, by taking all the investigated method performance

characteristics into account it can be stated that the INAA method, developed in the

laboratory fits for the intended use. By ascertaining a stable statistical control over the

necessary equipment, working according to well-documented standard procedure

is

Interlabor

For monitoring the validity of the analyses, to detect possible trends, or reveal reasons

for failures there are quality control procedures, like participation in in

An interlaboratory comparison was organized by the Institute of Nuclear Chemistry

and Technology, Warszawa, Poland with the intended goal of “Checking the accuracy of

analytical work of the laboratories engaged in the determination of trace elements”, and the

laboratory was invited to participate. Chemical profile of two plant samples, Tea leaves

Elemental data in qualitative sense were compatible with our prospectus, concerning

quantitative determinations, in many cases analyses were performed near detection limit

36


levels. In spite of this, for both materials the results passed the accuracy and precision criteria,

too, see Table 14. and Table 15.

es. Dust

materials on air filter samples originating from Vienna and Prague were subjected to INAA

analyses. Evaluation of the reported results is summarized in Table 16. and Table 17.

.3.2. Intercalibration of laboratories

cerami

ndard

Pottery

dards are used, based on the same primary standard, the uncertainty

compo

Participation in the Proficiency Test NAT-7, organized by the International Atomic

Energy Agency offered another challenge to control the method’s overall performanc

7

This kind of quality control activity has to be extended over a very important aspect of

c provenancing. During years, large amount of data have been accumulated in

laboratory’s data banks. Exchanging results and comparing data turned to be an actual need.

Achieving interlaboratory comparability requires a collaboration either in the analysis

of a common reference material, or in characterizing one another’s standards. As was shown

above, for method validation, among others, elemental data of the Perlman/Asaro Sta

was used. This reference material was widely used for several years in INAA

laboratories dedicated to pottery provenance studies, but now it is on very short supply.

When starting the Qumran pottery project, the first step aimed to investigate the extent

to which the data, generated during years, in the Archaeometry Unit of the Hebrew University

of Jerusalem could be compared with our results. The HU Laboratory used the P/A Pottery for

standardization, and we in the Radiochemistry Laboratory have used this reference material as

quality control material. When different laboratories are calibrated against the same primary

standards, the uncertainties in the reference values do not affect comparability. When

secondary stan

nents of this standard have to be considered in addition to the precision of the

measurement.

Validation proved the accuracy and precision of the analytical data obtained by us for

the P/A Pottery Standard. Samples of some clay samples (Motza 2) and also ceramics were

37


re-analysed in our laboratory, to assess the quality of the results in the sense of comparability.

The results indicated that the measured elemental concentrations, except for some outliers

a), are in good agreement, and with the necessary precautions, the exchange of pottery data

possible. Results are summarised in Table 18.

(N

is

38

Statistical evaluation of elemental data

8. Statistical evaluation of elemental data

Provenance studies generally aim to investigate the distribution of ceramic vessels in a

spatial dimension, make distinction between local and non-local products, try to find evidence

for production centres, and for the movements of goods or people. While elemental

concentrations, with their determinable degree of analytical precision have an inherent

objectivity, the incorporation of chemical data into a social, political or economic model is of

highly inferential nature. The bridge between analyses and interpretation is provided by

various statistical methods.

A considerable amount of analytical information can be obtained from elemental

concentrations and measuring uncertainties. There are different attempts to apply numerical

procedures to achieve partitioning of the data sets. Simple methods, such as bivariate scatter

plots and various pattern-recognition techniques are widely used, the well-quantified data-

matrices lend themselves to multivariate statistics.

There are several approaches, models and algorithms of multivariate statistics. The

primary point of view when choosing a procedure is that data processing should model the

questions arising from archaeological investigations and the results should directly answer the

questions.

In provenance studies elemental abundances are either used (1) to form statistically

meaningful compositional groups, or (2) to assign samples of unknown provenience to well-

defined existing groups. Samples to be treated are placed in a multidimensional space where

dimensionality is determined by the number of calculated concentrations. The samples lie

with varying point densities in this space. Problems are generally viewed in terms of

“distance” between different groups, groups and individual samples, or just among

individuals.

Data processing usually starts with a search for some kind of a structure, to define

statistically meaningful groups of chemically similar samples in the data set. The most widely

used, so-called “structure-imposing” (Bishop 2003) statistical methods for subdivision of

samples into groups are Cluster Analysis and Principal Component Analysis.

39


Cluster Analysis is designed to the classification of samples into more or less

homogeneous groups, in a way, that the relation between groups is also revealed. Clustering

process needs the definition of a measure of (dis)similarity, and an algorithm for defining

groups. As a measure of dissimilarity Euclidean distance, or its square, weighted Euclidean

distance, or Mahalanobis distance are the most used. Samples with the highest mutual

similarity are selected on the computed values, after which calculations are continued

according to hierarchical agglomerative algorithms, such as average-linkage method, Ward’s

method, or partitioning method. Calculations proceed until all samples are involved in one of

the clusters. The result is usually presented in the form of a dendrogram, characterizing and

illustrating the similarity relation of samples.

As elemental abundances are in most cases highly correlated, it is better to transform

the original data to uncorrelated components. The method working on this basis is Principal

Component Analysis.

Principal Component Analysis converts the original variables (i.e. elemental

concentrations) into new variables (principal components) that are linear combinations of the

originals. After this linear transformation similarity can be calculated by Euclidean distances.

At the same time the dimension of the problem is also reduced. The subspace of the first few

principal components, containing most of the variance, can be used to represent the structure

of the data set. Results can be presented in two-dimensional plots, where data-points are

projected into the plane of the first two principal components.

Another grouping method for elemental data is suggested by Beier and Mommsen

(1994) which surpasses the difficulties in Cluster Analysis and Principal Component

Analysis. As similarity measure between patterns a “modified Mahalanobis’ distance” based

on statistics is defined. It includes the consideration of elemental concentrations and

measuring uncertainties and a possible constant shift of the data caused by measurement

uncertainties or by dilution of the samples during manufacturing.

Once a structure has been identified in the data set, the subsets (groups) need further

investigation. Single-group, and/or between-group “structure-revealing” evaluative

procedures are needed to define the cohesiveness of a group and the “goodness” of separation

of the different chemical groups. For checking group cohesiveness the estimation of group

40


distribution parameters (mean and covariance matrix) are studied, by selecting the confidence

level.

As group separation approach, Discriminant Analysis can be applied. This

method also works with the uncorrelated linear combinations of the original variables (linear

discriminants) that reflect group differences as much as possible.

Several tests of significance are useful in conjunction with a discriminant function

analysis. In particular the T2 test can be used to test a significant difference between the mean

values for any pair of groups.

The structure of the data set usually reveals outliers as well, samples which cannot be

assigned to any of the subsets. The investigation of outliers can be performed e.g. by

Hotelling’s T2 test, with previously determined confidence level. χ2 test is also applicable.

Leaving out the outliers group distribution parameters are usually recalculated.

The separation of groups and the definition of outliers is followed by assigning

unknown samples to well-defined existing groups. One of the methods used for this kind of

problem is Discriminant Analysis mentioned above, another approach is based on

Mahalanobis distances.

The Mahalanobis distances of individual samples to previously defined group

centroids can be calculated, and each sample can be allocated to the group that it is closest to.

Significance tests can be also successfully applied for defining group membership

probabilities.

There are several further approaches and new methodologies of multivariate statistics,

like e.g. the Bayesian statistics (Buck 1966), which works on a model-based methodology,

where archaeological knowledge can be incorporated into statistical analysis. Model-based

clustering, classification trees, as well as neural networks offer future challenges in clearing

archaeological problems. A summary of statistical and computational methods used in

archaeology can be fined in Brothwell and Pollard (2001).

41


8.1. Multivariate statistics for Qumran pottery data

The following is the summary of the iterative classification treatment applied for

Qumran ceramics. Calculations were performed by L.Balázs, and the detailed description is

given in Qumran II. Volume (Balázs 2003).

In the Qumran pottery study 225 samples were analyzed, generating a statistically

meaningful data set. There were no predetermined groups, so parameters of group distribution

function could have been estimated only by iteration, i.e. by repeated selection and parameter

estimation phases. Steps of data treatment are given below:

Scaling

Raw data (sample concentration vector co-ordinates) were standardized, using the

average measurement uncertainties as scaling factors.

Determination of preliminary group centres

The dimension of measurement space were reduced using Principal Component

Analysis, sample vectors were projected to the subspace expanded by the dominant principal

component vectors (PCs with high/large eigenvalues). Then the proper equidistant grid was

generated in this subspace (first few PC space) and the sample probability density function

values at the grid points were approximated by the multidimensional Parzen-Rosenblatt

procedure. In this treatment each sample vector is regarded as a centre of multidimensional

Gaussian function, and after proper normalization the probability density function can be

estimated anywhere, by the summation of

these Gaussians. The group centres are

defined by the local maxima of these

estimated density functions. Fig. 3. shows

a two dimensional section of the three

dimensional density function of Qumran

pottery samples. The two local maxima are

related to the main groups.

-433 -389.4 -345.8 -302.2 -258.6 -215 -171.4 -127.8 -84.2 -40.6 3-54

-43.2

-32.4

-21.6

-10.8

0

10.8

21.6

32.4

43.2

54

centers for the iteration

Figure 3. Parzen-Rosenblatt density functions in Principal Component subspace

42


Preliminary group selection

In this step the group samples are selected around the preliminary centres, offering

further on the determination of group mean and covariance matrix as starting value of

iterations. Selection may be based on the Euclidean distance, proper statistical criteria cannot

be defined, only an arbitrary critical value. For the proper group selection the sequence of

critical values must be used, and the variation (trends and stability) of calculated group

parameters need to be analysed. The preliminary group boundaries are determined by given

critical levels regarding to the decrement of estimated density function from the local

maximum. For each preselected group mean vector and sample covariance matrix are

calculated.

Classification

Using the calculated group distribution functions, all sample points are classified by

the group conditional probability, or equivalently, by the related Mahalanobis distances.

Classification is performed on different confidence levels. By extending the confidence level

the number of group points increases, in the same time the outliers are filtered. The

subsequent estimation of group distribution parameters and selection of confidence level leads

to the convergence of the result.

The determination of group membership probabilities can be carried out by applying

the Hotelling’s T2 test to the Mahalanobis distances.

Although all these techniques offer empirical solutions, and can provide only

statistical probability of the provenance, statistics provides a powerful interpretative tool,

bridging the gap between chemistry and archaeology.

43

Qumran Pottery Project

9. Qumran Pottery Project

9.1. The Dead Sea Basin

The Dead Sea basin, a prominent morphotectonic depression along the Dead Sea Rift,

is the most famous of all the world’s depressions, having figured prominently in the events of

the Old Testament. Situated on the critical land bridge between the continents of Africa and

Asia, it has influenced the course of human history.

The Dead Sea is not only the lowest continental depression on Earth (-409m mean sea

level), but also has one of the highest salinities of any lake. The hypersaline, terminal sea is

inhabited only by highly specialized green algae and red archaeobacteria. The extreme

negative elevation is combined with tectonically elevated mountains flanking the basin,

resulting in a very arid environment. The western fault escarpment, up to 400m high is

composed of dolomite and limestone of Cenomanian and Turonian age. The area between the

fault escarpment and the lakeshore is covered by lacustrine sediments, known as the Lisan

Formation. Lisan marl, consisting of marl and unconsolidated alluvial fan deposits erodes

easily, but hosts many ancient sites along the Dead Sea, including Qumran (Fig. 4.). (Niemi

1977).

Contrary

to the idea that

the Dead Sea

area is an

uninhabitable

wasteland, the

region has a

large number of

archaeological

settlements, from

prehistoric times

Figure 4. Qumran settlement

44


to later periods (Fig.5) The special terrain, deep wadis,

tory served as a

many caves and topographic havens

provided an ideal environment for

anyone seeking isolation, whether for

ideological reasons, or for escape

from enemy. Beside that, the natural

resources of the Dead Sea area, like

e.g. salt, asphalt, fruit crops and

freshwater, provided unique raw

materials needed in the ancient world

(Beit-Arieh 1997).

The area around Qumran

many times in his

place of refugee and hiding- for

people, treasure and documents. In a

cave at Nahal Mishmar, called “The

cave of the treasure” Chalcolitic

people hid a spectacular copper

treasure of about 400 finely worked

artefacts, including crowns, mace-heads, scepters and standards. Bar Kochba warriors of the

Second Jewish Revolt used the cave at Nahal Hever (Cave of Letters), leaving documents and

some of their wartime correspondence there. Human remains as well as documents of

Samaritan refugees were found in a cave in Wadi Daliyeh, north of Jericho. These examples

show, that it is not unusual to find documents hidden in caves in this arid environment.

Figure 5. Archaeological sites around the Dead Sea (Beit-Arieh 1997)

45


9.2. Scroll discovery

The first scrolls, today known as

the Dead Sea Scrolls, were discovered in

1947, in Cave 1, North of Qumran

(Fig.6.). The seven scrolls, found by

Bedouins turned up for sale on the

antiquities market without

archaeological context, but their

authenticity was soon proved by Eleazar

Sukenik of the Hebrew University of

Jerusalem. He dated them to about the

time of Jesus, and he was the first to

suggest a connection with the Essenes.

The seven scrolls were: two copies of the

book of Isaiah, the Genesis Apocryphon,

the Habakkuk Commentary, the Hymn

Scroll, the War Scroll, and the Rule of

the Community. This latter one, but also

the War Scroll, the poetic work of the Thanksgiving Hymns, or the Commentary on

Habakkuk, are not biblical texts, but undoubtedly belonged to a certain community, and

provide information on their lives, beliefs and religious practices.

Figure 6. Cave 1 (Davies 2002)

9.3. Excavations in Qumran

In 1949 Roland de Vaux of the École Biblique et Archaéologique of Jerusalem and

Lankaster Harding, the chief inspector of antiquities in Jordan excavated Cave 1, and

surveyed the Qumran settlement and cemetery. At that time they had found no evidence for

the connection with the scrolls and the caves.

46


In 1951 however, excavations were started in Qumran and de Vaux found a jar, similar

to those, found in Cave 1, dated by a nearby coin to ca.10 BC. It was also recognized that the

same types of pots and lamps that was found in Cave 1 were represented in the settlement.

Based on this, these pottery types were dated to the 1st century BC and 1st century AD.

The first season of excavations finished with the conclusion, that the people who lived at

Qumran deposited the scrolls in the cave.

de Vaux conducted excavations on the site for four further seasons, between 1953 and

1956. Based on his observations he distinguished several different periods of occupation and

assigned dates to them. The history of the settlement can be summarized as follows (de Vaux

1973):

The site was first

inhabited in the late Iron Age

(8th-7th century BC). A

rectangular building with a

row of rooms, a large round

cistern and a wall, running

southward belong to this

phase. This settlement was

destroyed in around 586 BC,

and was abandoned for quite

a long time. Under the reign

of John Hyrcanus (135-104

BC) a new population lived

there, but only for relatively

short period of time. The Iron

Age buildings were rebuilt,

rooms were constructed around the big cistern and two rectangular pools were dug. Two

potters’kilns in the south-east part

Figure 7. Plan of Khirbet Qumran (Gunneweg 2003)

(L66) were in use in this period.

The settlement acquired its definitive form, and became an impressive complex of

buildings during the reign of Alexander Jannaeus (103-76 BC).(Fig.7.)

47


In the middle of the north side of the settlement a squared tower stood at the main

entry, the settlement was divided into two main parts: an eastern part with the tower, and a

western sector centred around the round cistern (L110). A highly developed water system,

channelling rainfalls from the hill-foot to the farthest south-east spot, through several pools

and cisterns, was developed, which is perhaps the most striking characteristic of the site. de

Vaux stated, that this carefully constructed water system supposes a group, “which was

relatively numerous, which had chosen to live in the desert, and for which, accordingly, the

problem of how to ensure a supply of water was vital- or more than this”, they needed it for

purification rites.

In a room (L

86,87,89) more than a

thousand vessels were

found (Fig.8.) comprising

every types of wares

needed for meals: plates,

bowls, jars, jugs, beakers,

dishes. It was identified

as a crockery, storing

vessels for common

meals of about 200-250

people, which were held in the big hall beside it (L77). In the south-east area there was a

potters’workshop, with two kilns (L64, 84). Peculiar finds of L30, like broken parts of a big

table made of mud-bricks, two inkwells, fragments of two smaller tables led de Vaux identify

this hall as a scriptorium, where the scrolls were written. The nearby small room, with low

benches all around was defined as council room. In the western sector different workshops,

storerooms and industrial installations were excavated. The deposition of animal bones

between pots, placed in jars, or covered by plates is a striking feature of L130 on the north-

west part (corner). This occupational phase is dated of the Hasmonean rule (134-37 BC) and

to the first years of Herod the Great (37-4BC). An earthquake and a fire destroyed the

settlement, which is dated by de Vaux to 31BC, based on Flavius Josephus, who tells (Bellum

1.370-380) that at the time of the battle at Actium, which happened to be at the 7th year of

Figure 8. The “Crockery” at L.89. (Magness 2002)

48


Herod’s rule, there was the most serious earthquake ever in Judea. (Traces of evidence is not

convincing though.)

After a period of abandonment the same community reoccupied the site. The general

plan remained, buildings were used for the same activities as before. The potters’workshop

remained in use, the rite of animal bone deposits continued. The tower was reinforced by a

stone rampart, the water system was modified, but the broken crockery was left in its place.

This period is dated to the first century AD, from Herod Archaleos (4-6 BC) to the

First Jewish Revolt. In 68 AD the settlement suffered a violent destruction by Vespasian’s

Legio X Fretensis.

9.4. The function of the settlement

As written above, de Vaux

soon stated that Khirbet Qumran is not

a village, or group of houses, it is the

establishment of a community. This

idea very early determined the historic

–archaeological characterization of the

site. Alternative interpretations (villa-

Donceel (1994), fortress-Golb (1995),

commercial entrepot- Crown (1994),

cultic centre) can account for some of

the evidence, but most scholars still

agree, that Qumran was the home of

an isolated religious community.

It has too many features that

are unparalleled at other sites, like e.g.

the water system with pools and

cisterns, crockery and dining hall,

scriptorium tables and inkwells,

animal bone deposits, or the pottery.

Figure 9. Cave 4.

49


Between 1951 and 1956 ten other caves hiding scrolls were discovered, among them

Cave 4, (Fig.9.) containing thousands of fragments, and Cave 11, with several complete

scrolls. Cave 4 and 5 are located within a stone-throw from the buildings of the settlement, so

the connection of the scrolls from the caves and the settlement was generally accepted. Scrolls

were found in association with potteries in almost all cases, the only exception is Cave 5,

where not a single shard of pottery was recognized.

Next to the site, about 50 meters to the east, there is a cemetery of about 1200 graves,

arranged in neat rows, most of them in the same orientation, with heads pointing south.

Tombs are marked by heaps of stones on the surface.

The magnitude of the cemetery and the careful arrangement of individual graves

suggest people of similar religious rite. Out of the 43 graves opened, four were identified as

women or children.

By 1955, all the seven scrolls of Cave 1 have been published. Based on paleography,

epigraphy and archaeology, it was determined that the scrolls can be dated to the last centuries

of the Second Temple era: 2nd century BC-1st century AD. Already in 1951(!) a piece of

textile, attached to one of the scrolls was subjected to C-14 dating, and later on eight scroll

fragments from different caves were analysed by Accelerator Mass Spectrometry, confirming

the previous dates.

9.5. The “Essene hypothesis”

1st century ancient authors, Flavius Josephus, Pliny the Elder, Philo of Alexandria all

have passages in their books about a Dead Sea community, the Essenes. Flavius Josephus in

Bellum 2.119-61 gives a long and detailed description of their ascetic life style, their religious

beliefs. Pliny’s Historia Naturalis (5.73) provides information about the location of the

settlement, writing that they live on the western shore of the Dead Sea, somewhere above the

town of En Gedi. He wrote, that the Essenes didn’t marry and lived in isolation, “with only

the palm trees for company”. Most of Philo’s information on the Essenes (Every Good Man is

Free 75-79) corresponds with that of Josephus’s, but it is less specific.

50


Although the only place on the west side of the Dead Sea north of En Gedi, where

archaeological remains of a communal centre were found is Qumran, there has been a

constant debate regarding the identification of this group with the Essenes. That the site was

probably a religious communal settlement, does not necessarily identify it as Essene.

9.6. Judean society in the Second Temple period

In the 2nd century BC Palestine was ruled by the Ptolemies until 198 BC when

Antiochus III took control. During Seleucid era there was a continuous force to destroy

Jewish religious and national autonomy. The conflict, caused by the Hellenizing program of

Antiochus IV Epiphanes (175-164 BC), imposing edicts against the Jewish religion, forcing

the Jews to sacrifice to the Greek gods, culminated in 167 BC with the outbreak of

Maccabean Revolt.

The Maccabees, with a group of people called Hasidim, purified the Temple,

reinstituted the sacrifices and liberated Judea. The Hasidim left the political battlefield. The

Maccabees, although they were not descendents of Zadok, ruled as High Priests, which was

considered to be illegitimate by the conservative Jews. Later Judas united the priestly and

civil authority in himself and thus established the line of Hasmonean priest-rulers and for 100

years governed an independent Judea. Under the Hasmonean kings the political, as well as

ethnic and religious authority was stabilized. In these times new thoughts and theories

enriched Jewish theology: belief of immortality of the soul, messianic hopes and apocalyptic

views.

Different philosophies, different political and religious intentions resulted in separate

socio-religious classes or parties. The three main policies, first mentioned by Flavius Josephus

(Ant. 13.171) under the reign of Jonathan the Maccabee are the Sadducees, Pharisees and the

Essenes.

The Sadducees represented the aristocratic upper class of Judean society, most of them

were priests, or members of priestly families. They derived themselves from Zadok, the high

priest of the First Temple and as his descendents served as high priests through the First and

Second Temple periods. Although the purity of the cult was the most important for them, they

adopted political changes and realities.

51


The Pharisees belonged mostly to the middle and lower classes of Judean society and

opposed the adoption of Hellenization. Pharisees are regarded as an attractive and powerful

faction, with an ascetic lifestyle, who could effectively control the state. They were the most

rigid defenders of the Jewish religion and traditions, and were very scrupulous in their

observance of Jewish law.

The third main religious group of the Jews of Second Temple Palestine was the sect of

the Essenes. The history of essenism goes back to the Hasidic movement of the 2nd century

BC. It is rooted in the conflict between the Wicked Priest and an unknown priest, the spiritual

leader of the community, the teacher of Righteousness. Surviving Hasidim became the

founding-members of the community. They were more ascetic and more esoteric than the

Sadducees or the Pharisees. One of the most striking characteristics of this group was their

communal life. Their ascetism, moral principles, apocalyptic outlook, eschatologic

philosophy and messianic hopes are mostly known to us from Josephus’ writings.

There were other smaller and less powerful factions, like the Zealots/Sicarii or the

early Christians, and the evolvement of all these groups marks a tendency of separation from

mainstream Judaism.

At 63 BC the rivalry between Hyrcanus II and Aristobulus II over the control of

Palestine brought about a civil war, which led to Roman intervention by Pompey. Different

administrative districts of Palestine were ruled and governed by Roman procurators or

governors.

The rule of the Hasmonean dynasty ended in 37 BC, when Herod the Great became

king of the Jews. Herod become the ruler with Roman help, and was a dependent client-king.

Nevertheless, his building projects, the development of economic resources, the establishment

of a sound bureaucracy undoubtedly enhanced the standing of the country. Many of his

projects won him the bitter hatred of orthodox Jews though. After his death in 4BC, the

kingdom was divided among his sons, Archeleaus, Philip and Antipas.

Roman control had grown more and more onerous. Rome took over the appointment

of the High Priest, proved unconcealed contempt for Judaism, and this in combination with a

financial exploitation brought about the Great Revolt of 66-70 AD, leading to one of the

greatest catastrophes in Jewish life, the destruction of the Temple.

The settlement of Qumran was destroyed by the Roman legions, while the loss of

Masada, defended by a group of Zealots in 73 BC marked the end of the rebellion.

The history of Qumran should be viewed in this historical background.

52


9.7. The Dead Sea Scrolls

Classical sources and archaeology both are consistent with putting the Essenes to

Qumran and the “Essene hypothesis” can be corroborated by the scrolls themselves. The

scrolls are the only extensive contemporary documentation that we have, all other sources

being retrospective. This group of documents provides a detailed picture of a socio-religious

entity. It is a self-portrait, not a description by others. Although there are a few cases in which

historical figures (Shalomzion, Amaelius) are mentioned, they provide almost no information

on Jewish history proper.

The origin of the community is depicted by cryptic statements. The founder of the

community was the “Teacher of Righteousness”, who had to suffer persecution by the

“Wicked Priest” of the Jewish rulers. The teacher and his followers had to flee to the

wilderness to wait for the coming event: the victory of the Lord above the evil and dark, the

Sons of the Light above the Sons of Darkness. The conflict written in the scrolls is the conflict

between the head of the community and the political-religious Jewish ruler, Jonathan or

Simon Maccabee. (Vermes 1998)

The number of documents counts more than 800, with Cave 4 giving 555. Most part of

them is written in Hebrew, there is a smaller portion in Aramaic, and some of them are

written in Greek. Before their discovery, no Jewish documents written in Hebrew or Aramaic,

dated to pre-Christian time was known.

Among the scrolls, in complete or fragmentary form, all books of the Hebrew Bible

(except the book of Esther) can be found. Beside biblical literature apocryphals (e.g.

Ecclesiasticus), and pseudo-epigraphical texts (e.g. Jubilees, Henoch) are also represented.

Communal documents, probably written in Qumran by members of the community,

like rules, exegeses, religious poetry, liturgical texts stress the deliberate and selective policy

of isolation, pursuit for purity. The split with the Temple is embedded into calendrical

treatises, alighting the use of the solar calendar. The basic laws of communal life are written

in these texts, and although these group characteristics may be true for some other

contemporary Jewish groups, neither of the hypotheses identifying the Qumran community

53


with the Pharisees, Sadducees, Zealots or early Christians are provable, the Essene theory

seems to be the most probable and acceptable.

Contrary to the claims made by some scholars, no traces for copies of the New

Testament are represented among the scrolls. Highlighting the internal diversity of Judaism at

the height of Second Temple Palestine, they help fill the blank page between the Hebrew

Bible and the early rabbinic literature, rather than the blank page between the two testaments.

After fifty years of scroll research, based on paleography, epigraphy, archaeology and

scientific analyses the scrolls are dated to 2nd century BC-1st century AD. The general

hypothesis is that part of them were written in the settlement, but there are also others, that

came in from somewhere else, and all of them constitute a library of a religious community.

Concerning the function of the scroll caves, the most probable explanation is that some

of the remote scroll caves (1,2,3,11) could have been an archive for the scrolls, while the

man-made nearer caves (4,5) were serving as a fast answer to a sudden danger (Gunneweg

2003).

Whether or not the Essenes were the authors of the sectarian literature of the scrolls,

the settlers of Qumran were flesh and blood people, simple human beings whose traces

remained after they disappeared, and we have to find them.

9.8. Qumran pottery

The study of pottery from any archaeological sites offers valuable information that is

not provided by any other remains. This is valid to the pottery of Qumran, too. de Vaux died

in 1971 without publishing a final report of his excavations. His overview of the archaeology

of Qumran, that is the book of the so-called Sweich-lectures (de Vaux 1973), and the volume

containing his field notes and photographs from the excavation were published (J-B.Humbert,

A.Chambon 1994) later. A summary of published Qumran pottery is given by J.Magness

(Magness 2003).

54


According to these, the ceramic types represented in Qumran include bowls, plates,

cups, jars, lids, jugs, juglets, kraters, flasks, cooking pots and oil lamps. The pottery from the

caves is identical with that of the settlement, the same fabrics and the same forms recur here.

The vessel types reflect the activities carried out on the place. The ceramic assemblage

shows important peculiarities, with respect to other archaeological sites of this period.

A number of pottery types represented at contemporary Judean sites are absent from

Qumran’s ceramic assemblage. No amphoras, Roman mold-made oil lamps, or Terra Sigillata

sherds were unearthed. The fine, thin-walled, painted Nabatean pottery is also absent.

The most distinctive type of pottery is undoubtedly the cylindrical jars, the so-called

scroll jars.

Cylindrical jars are common in

Qumran both in the caves and the

settlement, proving the organic connection

between them, but no other places outside

Qumran have this type of ceramic ware

(Fig. 10). According to the Bedouins,

scrolls wrapped in linen were stacked in

these pottery jars in the caves, but there

were quite some pieces in the settlement,

too, without any fragmentary piece of

parchment. In nearby caves which didn’t

contain scrolls, pottery sherds, including

scroll jars were also recognized.

Storing scrolls in jars was an ancient

practice, that is known to us from

Jeremiah, 32:14, where there is an advice,

that sealed and unsealed books and

purchase contracts are best placed in pottery containers if one wants to preserve them for a

long period of time.

Figure 10. Sroll jars at Qumran exhibition

The pseudepigraphical work of the Assumption of Moses (1:16-18) also refers to

storing scrolls in jars. Moses who is about to die, gives Joshua certain books of prophecies,

which Joshua is supposed to treat with cedar oil and store in jars in a place appointed by God.

55


Ancient authors, like e.g. the Christian scholar Origen, the church historian Eusebius,

and later Timotheus I, the Nestorian patriarch of Seleucia mention biblical texts found in jars

near Jericho.

Whether or not the scrolls were stored in jars, they were manufactured to suit special

needs and they are undoubtedly site-specific. Lids are associated with them, some of them can

be attached with a string to pierced ledge handles on the shoulder of the jars. Lids are

common both in caves and the settlement.

Other types of jars, like ovoid jars, bag shaped jars are also common, but also these

represent a regional type (Magness 2002, p.101.).

The other unusual, but not without parallels, pottery type is represented by the

inkwells. Different sources give different numbers, but at least five inkwells made of

earthenware and one of bronze were found in the settlement.

All pottery is plain, undecorated, the vessels are made of well-levigated, light red, or

grey clay, often with a white slip on the surface. The presence of a potters’workshop

indicates, that at least part of the ceramic material was manufactured locally.

de Vaux stated that this workshop produced the large number of vessels discovered at

Khirbet Qumran, and that the monotony of pottery and its unique character at the same time

can be explained by the local manufacture.

If all the Qumran pottery was locally made we have a “hapax” settlement which had

no connection with its environment. This closeness of the community needs a thorough study

though, as with all groups of people during history, material remains of basic human relations

are always found. Where people have lived, one is bound to find its traces among the

population itself and those with others. If Qumran had relations with other sites, we have to

find these. Concerning pottery, in spite of de Vaux’s statement, there remains the uncertainty

which pottery is Qumranic for sure, which is dubious, and which has to be excluded as locally

made, and from where did it come instead. Scroll jars are of special interest, perhaps even part

of the scrolls can be traced by the provenience of the jars.

56

Chemical provenancing of Qumran pottery

10. Chemical provenancing of Qumran pottery

This pottery project, initiated by Jan Gunneweg of the Hebrew University started in

1998, in co-operation with Jean-Baptiste Humbert of the École Biblique et Archaeologique,

Jerusalem.

The main goals of the research were:

- to trace the Qumran pottery by its chemistry to their place(s) of manufacture

- to establish the relation between the pottery found in the Qumran settlement and

the surrounding caves

- to study what pottery was locally made and which was brought in from elsewhere

to learn the interregional trade between Qumran and its surroundings.

10.1. Sample selection The main objective in sample selection was to analyse a representative portion of the

original de Vaux’s assembly of pottery of

all sorts of household ware and site-

specific pottery from the settlement and

the caves.

34 samples were taken from

materials thought to serve as Qumran

reference materials, as well as 166 other

samples were taken from pottery that

consisted of a variety of styles, including

scroll jars. Ceramic material from further

archaeological sites, such as Jericho,

Jerusalem, Hebron, Callirhoe, EnGedi,

Masada and ‘Ain Feshkha were also

sampled and involved into the research

57Figure 11. Map of the sites (Gunneweg 2003)


(Fig. 11). The total number of analysed samples reached 225. The complete list of samples is

given in the Appendix.

10.2. Reference material for Qumran

To start a provenancing process it is of great help to construct a reference group, that

is to get the chemical profile of ceramic materials, definitely local to the site. For Qumran

reference material samples of kiln linings, clay balls, mud-bricks, oven covers and jar

stoppers, local marl and Dead Sea mud samples were chosen.

Besides, two kiln wasters, i.e. collapsed or misfired pottery, whose trade can be

excluded, were found and analyzed with great expectation. An extra set of six samples

coming from the Motza Clay Formation, Hebron and Jericho was also involved.

To get the local chemical fingerprint it seems obvious to sample raw clay used by the

local potter. The problem is, that no real clay is found at, or near the site that could have been

used for the pottery under study. de Vaux claimed that “…the marl terrace of Qumran can be

made into excellent mud bricks but it is too calcareous and not malleable enough to be used as

potter’s clay. Nor are there any beds of clay in the immediate environment of Khirbet

Qumran. There is clay on the plateau above the Dead Sea and the winter rains carried it down

to Wadi Qumran. These deposits are still far calcareous.” (de Vaux 1973). Zeuner performed

chemical analysis on two samples from L75 Potter’s basin, and on two further samples from

cisterns, defining their CaCO3, MgCO3 and CaSO4 content (Zeuner 1960). His results are

comprised in Table 19.

To test the suitability of local marl and Dead Sea mud for making pottery vessels some

experiments were performed: the upper layer of a dried up puddle after the first rain in

Qumran was taken and a vessel was formed and fired. Another pot was made of Dead Sea

mud. The tests succeeded, the final products looked as good as any ceramic material in

Qumran. Their analytical results are involved in the pottery data.

There are some theories for transporting raw clay to Qumran from other locations. Up

till now, however, there is no decisive evidence for the movement of clay prior to the

58


industrial era. The proximity of raw materials to production sites is a major issue in ancient

procurement patterns. According to Arnold’s notes (Arnold 1985) on 111 ethnographic cases,

33 per cent of potters obtained clays within a 1km radius of their workshops, and 84 per cent

within 7km. (Whitebread 2001).

There should be clays to be found around Qumran, or further away: but we have to

find those. A Polish team surveyed the site and the nearby wadis and took 22 clay samples

from different places, the Judean Mountains, Jerusalem, En Gedi, El-Jib, Hebron, Cave 4,

Qumran aqueduct, Wadi Qumran. Laboratory tests (colour, texture, porosity) as well as

petrographic and geochemical investigation were performed not only on these clay samples

but also on 55 ceramic jars from Qumran caves. They concluded that Qumran jars were made

of a raw material, which is not present in the vicinity of the site, and most of the jars were

probably produced from the Motza Formation clays, known and widely utilized in Judea

(Michniewicz 2003).

10.3. Analysis

Selected samples were analysed by instrumental neutron activation, according to the

validated standard operation procedure detailed in Chapter 7.

Due to the implemented quality control/quality assurance system accurate and precise

data has been generated in an organized, transparent and thoroughly documented system.

10.4. Data processing

Elemental concentrations and combined standard uncertainties were processed by the

multivariate statistical procedure given in Chapter 8.1.

Scraping samples of QUM 222, 223, 230, 233, 235 were not analyzed but were saved

to be investigated by other methods.

To avoid problems caused by missing values, big measuring uncertainties, or other

practical reasons (e.g. volatility of As and Br during firing) some elements were subtracted

59


from calculations. The data matrix processed thus was determined by 16 elements and 220

samples.

10.5. Analytical results

Data treatment has resulted in five chemically distinct groups of samples. (Fig. 12) and

Table 20.

Data points in PC1-PC2 space

-40

-20

0

20

40

60

80

100

0 50 100 150 200 250 300 350

PC1

PC2

outlayers

group 5

group 1

group 2

group 3

group 4 ?

group 5 ?

group 2 - subgroup ?

group 3 ?

Conf. ellip. - group 5





PC1-PC2-PC3

-433 -389.4 -345.8 -302.2 -258.6 -215 -171.4 -127.8 -84.2 -40.6 3-54

-43.2

-32.4

-21.6

-10.8

0

10.8

21.6

32.4

43.2

54

centers for the iteration

Co - La projection

0

1020

3040

50

0 10 20 30

Figure 12. Chemical groups of Qumran pottery samples

60


Fig 12. exhibits different approaches for the representation of the subdivision of

Qumran pottery samples. The basis is a two-dimensional plot, where data points are projected

into the plane of the first two principal components, containing the maximum variance of the

related data. The upper left segment shows the projection of sample points to the PC space,

determined by the first three principal components. The bottom left figure is a bivariate plot

the Parzen-Rosenblatt density functions with local

aximums as iteration centres are presented.

10.5.1

d ceiling (146), and mortar samples of the “scriptorium table” (175-178). Three

oven c

5) and perforated clay balls

(127, 1

p makes it highly

probab

however, didn’t live up to the expectations, they do

not ma

aterial failed in the firing, because the composition was not adequate, or that these

sherds

ains many types of household vessels of daily use, cups, bowls,

lids, a l hem ten scroll jars.

of raw data, while in bottom right

m

Columns of Table 17. comprise code numbers of samples belonging to the different

chemical groups defined. The separation of different pottery types within the groups proved to

be useful in the interpretation of the results.

. Chemical Group I.

A large group of pottery (44 samples) comprises most of the samples that were

thought to produce Qumran’s local chemical fingerprint: samples of the inner and outer lining

of the kiln (101, 103, 104), the puddle-marl and Dead Sea mud (225, 226), a piece from a

stucco-line

overs (150-152) and two clay-balls (128, 130) were certainly made of material

available on the site.

All these samples are highly calcareous, with an average calcium content of 24

percent. However, there are other samples of crude covers (142, 14

30) with a calcium content around 7 percent, which means that law calcium clay was

also available. The great number of Qumran reference samples of this grou

le that this unique chemical fingerprint corresponds the local pottery production of

Qumran.

The two kiln-wasters (140, 197),

tch anything in the data set. They are different also from each other. It either means

that their m

represent earlier (Iron Age) or later (Late Roman) pottery.

The local group cont

amp, a juglet and different kinds of jars, among t

61


Out of the ten scroll jars six come from caves (132, 139, 163, 186, 231, 240) and four

from the settlement (120, 156, 162, 187). All of them are typical cylindrical jars, but the

settlement pieces are all of smaller size.

even nto this local assembly, but none of them comes from

caves.

ttery made of this clay has been published in several papers

erlm

two samples of Hebron clay (228, 229) found a statistical match with this

roup, giving the confirmation for the provenance of this group of pottery being the Hebron-

eit’Ummar type Motza clay.

Twenty out of the 41 samples constructing this group are scroll jars, six from various

of t n from caves. This means that the majority of the

analysed

El storage jars are grouped i

Two ovoid jars are made of the local makeup, one unearthed in the settlement (133)

and one from Cave 7 (134).

The cups and bowls are all from the settlement.

10.5.2. Chemical Group II.

Based on the similarities of their chemical pattern 41 samples are grouped together,

forming the second largest subset of the data matrix. The distinction is characteristic, so it is

fair to say that these vessels are not locally made, or made from not local raw material. The

unique high potassium values proved to be useful in tracing the provenance of ceramics

belonging to this group to the Motza Clay Formation.

This Cenomanian geological formation is one of the few levels of clay rocks that

occurs in the area of the Jerusalem Hills and Hebron Mountains and was employed in

different periods of history. Po

(P an 1986, Gunneweg 1985b, 1994). It was found, that the Motza clay source chemically

is not homogeneous, although homogeneous enough to be recognized. A slightly different

chemical composition can be seen regionally and also vertically, concerning its different

concordant layers. Based on these previous studies it became very probable that Qumran

Group II. potteries have a Motza clay connection, which could be confined to Beit ‘Ummar,

near Hebron. The

g

B

locations he settlement and fourtee

scroll jars were manufactured of this material. Lids and storage jars from the

settlement and the caves as well, a funnel, three bowls and a lamp also belong to Chemical

62


Group II., which means that this kind of raw material was not used specifically for making

scroll jars only.

10.5.3. Chemical Group III.

41 ceramics of the Qumran settlement and Caves analyzed as local Jericho pottery.

ent is based on the results of four samples analysed from the Hasmonean and

in Jericho. In 1989, Yellin and Gunneweg published a study,

t of Jericho pottery found in these sites.

Two scroll jars, found in Cave 1 and Cave 3, can be traced back to the Jericho local

akeup

on the comprehensive studies on Edomite and Nabatean pottery of

unneweg (1988, 1991) and Gunneweg and Mommsen (1990, 1995).

0.5.5. Chemical Group V.

samples clustered together are considered to be originated from Jericho, but this

group is different from Chemical Group III. The six Qumran samples analyse as QUM 224, a

bowl from Jericho itself.

Assignm

Herod’s winter palaces

determining the local chemical fingerprin

m , both of them are of the so-called bulging cylindrical type. QUM 198 (Cave 1) is one

of the two complete scroll jars exhibited in the Shrine of the Book at the Israel Museum.

Storage jars as well as ovoid jars of Jericho provenance are also represented here,

together with six cups, fourteen bowls and nine jugs.

10.5.4. Chemical Group IV.

A small group of nine samples, a large cup, an ovoid jar and a storage jar, two jugs

and four bowls refers to Qumran’s connection with the other side of the Dead Sea, i.e. Edom.

The conclusion is based

G

1

Seven

63


10.5.6

s

ithstand great temperature differences when in use. Although

no quality criteria is known for producing a good cooking pot, it is very probable, that the

clay us

nous limestone

An oil shale sequence is found in the Judean Desert uplands, providing a black

mesto

ated and proved to be chemically similar, with about 30 percent calcium content and a

lative low lanthanide and high uranium concentration.

s

any other pottery, as was mentioned

bove.

. Outliers

There are quite some samples which cannot be associated with any of the five group

given above.

Cooking pots

Cooking wares have to w

ed for the manufacture of cooking ware is different from that used for other vessels.

Four cooking pots, QUM 168, 169, 195 and 196 were analyzed, and all of them were

found to be without identifiable provenience.

Bitume

li ne, which is widely used in Qumran as filler in the plasters of the many pools.

According to the analysis of samples 181 and 285 this material is enriched in a number of

metals, e.g. chromium, molybdenum, uranium and zinc.

Stucco

Plaster pieces of the “scriptorium table” and a sample from a stuccoed ceiling were

investig

re

Waster

The two kiln wasters (140, 197) had no match with

a

Ceramics

There are some pieces of pottery, like QUM 148,155, 208, 209, 211, 215, 219, 232 and 277

for which a chemical parallel has not been found yet.

64


10.6. Discu

ssion

ical fingerprint of the Hebron (Beit ‘Ummar)

ostly in the caves, but were found in the

settlem

ho jars are slightly different in shape, a bit

bulging opposed to the cl

chemically to the group of scroll

ade and dominate on the settlement, although

some were found in caves, too. All four groups have ovoid jar representatives.

ux as “Crockery”. L 86 is adjacent to L 77,

According to the analytical results, about 33 percents of the analyzed pottery has a

provenience local to Qumran. A relatively large part of pottery has connection with Jericho,

and another bigger group of vessels have a chem

type Motza Clay. There are quite some pottery wares alighting a possible Edom connection.

No difference in the chemical composition of pottery analyzed from the settlement and

that of the caves was found, each chemical groups have representative pieces in both contexts.

The elongated cylindrical jars appear m

ent as well. In the caves they are associated with scrolls, but no scrolls were found

with them in the settlement. Of the 34 scroll jars analysed ten represent the local manufacture,

twenty are related to Hebron, two originate from Jericho, while the provenance of a scroll jar

from Cave 4 remained unidentified. The two Jeric

assic cylindrical type.

Lids are grouped into Group I. and II., which is quite reasonable, they belong

jars. Jars and lids should have been made simultaneously so

as to fit to each other.

Most of the storage jars are locally m

Ceramic assemblage of the caves consisted mostly of the cylindrical jars, other types

of storage jars, lids and lamps, but some bowls and jugs were also found. Pottery was found

also in caves which didn’t contain scrolls. This implies that the caves were used by people on

more than one occasion of hiding the scrolls.

A great number of cups, bowls and jugs were unearthed on the settlement. Locus 86

contained 279 shallow, carinated bowls, 798 hemispherical cups, 150 deep cups, 37 large

bowls, 11 jugs and 8 jars and was called by de Va

65


the biggest room of Khirbet Qumran, called the Assembly Hall, or p

stock of pottery beside, the “Refectory”. The large number as we

robably because of the

ll as the

dishes points to communal meals with many participants, and a con

cups and bowls analysed from the crockery proved to have originate

This part of the settlement was destroyed, the broken vesse

area was sealed off.

kraters and oil lamps

were found. Samples

analysed from this and

the surrounding rooms

were either locally made

or represent the Hebron-type Motza com

nfamiliar to the rest of Qumran pottery. Another trial was made to establish Qumran’s

ossible relation to another site on the Eastern shore of the Dead Sea: ‘Ain ez-Zara

allirhoe). Balsam juglets were chosen for analysis, in the hope of defining their provenance.

The four balsam juglets (QUM 295-299) proved to be chemically different. Two of them were

ourth one remained unparalleled.

Nevertheless, the connection of Ez-Zara with Qumran and Jericho became highly probable.

uniformity of the

cern of purity as well. All

d in Jericho.

ls were left in place, the

There was

another store of dining

dishes in L 114,(Fig. 13.)

next to the round cistern.

Bowls, more than one

hundred hemispherical

and deep cups, jugs and

Figure 13. Dishes in Locus 114 (Magness 2002)

position. This information needs further studies,

mostly into the different time periods of the settlement.

10.6.1. West-East connection

Some bowls, cups and jars mark the connection with Edomite sites with types quite

u

p

(C

produced in Qumran, one came from Jericho, the f

66


traces of writing on them (Gunneweg

ls, or on sherds with ink or paint, on

after firing. Fifty-five sam

bearing signs of measurement, names, students’excercises, dated ‘deeds’, fragm

ent

ity. The

decipherment and interpretation of

the writings is given by Lemaire

ples were treated

togethe

criptions were

proved to be locally made in Qumran

10.6.2. Inscriptions on Pottery (Ostraca)

ples were found

ents of letters,

or just incised lines. Forty-one of

them have been analyzed by NAA.

The primary goal of these analyses

were to define the provenance of the

shards with inscription, which in

special cases gives the origin of the

script, too, to corroborate the

connection of caves and settlem

A special study was performed on potteries with

and Balla 2003b). Writing was found on whole vesse

pottery engraved before firing, or scratched

through writing activ

(2001).

These samFigure 14. The R

r with all the ceramic samples

by the analytical and statistical

procedures given above.

Four jars (121, 134, 311, 315)

and a jug (312) with ins

OMA jar (Lemaire 2003)

Figure 15. The “Roma” insription (Lemaire 2003)

and it seemed obvious that also a local scribe wrote the inscriptions. The most interesting

vessel in this group is a jar (QUM 134) with two ROMA inscriptions in black ink or paint.

(Fig. 14-15.)

67


The jar was found in Cave 7 together with many Greek papyri of various texts. Some

fragments of papyri were identified as the Gospel of St. Mark, and those thought to be the

earliest written Christian documents ( Thiede 1992), although most biblical scholars refute the

theory. Thiede suggests, that the inscription ROMA on the jar might indicate the provenance

of its c

leven ostraca have been found, ten in the settlement and one in Cave 6, with a

chemic

which is of special interest. QUM 205 is the “Eleazar” bowl, with the name inscribed before

inscribed in Jericho and brought to Qumran.

ied time

there is another ostraca found in Qumran, menti

ions as

Nabate

Qumran living quarters and its caves, through scribal links: certain

scribal remains appeared on pottery that was made locally in Qumran and found in the caves.

As Lem ire (2001) claims, the type of writing in given scrolls as well as some on pottery is

ontents, i.e. the scrolls had been identified as coming from Rome (Thiede 1996). This

New testamentary connection has to stand or fall only on the texts themselves as the jar was

proved to be locally manufactured in Qumran (Gunneweg and Balla 2001).

E

al composition that can be traced to the Hebron-type Motza clay. Where the

inscriptions were born, cannot be localized, they could have been written in Qumran, or in the

place where the pottery was manufactured.

The Jericho chemical group includes ten jugs, a plate, a handle and two bowls, one of

firing, which means that the bowl was made and

The name Eleazar is quite common in the stud period, but it is still interesting, that

oning Eleazar and Jericho (Cross and Eshel

1997).

Two jugs with inscription on their

shoulder were assigned to Chemical group

IV, i.e. coming from Edom (Fig. 16).

Lemaire deciphered the inscript

an names, thus corroborating the

results of provenance studies, putting the

place of manufacture as well as the writing

to the eastern side of the Dead Sea.

In conclusion, provenance studies of

ostraca furnished further evidence for the

connection betweenFigure 16. The Edom jug QUM 201 Lemaire 2003

a

68


similar, too. Besides, the Jericho, as well as the Edom/Nabatea connection is corroborated by

written evidences.

iring temperature

(Rasmu

onclusion was supported by the determination of

firing tem th

timated firing temperature of Qumran ceramics under study varies between

710 C and 860oC. It is interesting, that for the waster sample (QUM 196), which is one of the

outliers, it proved to be much lower, 570oC.

is conclusion of the results of TL dating is that “there is nothing in the data of the

remaining eleven samples that speaks against a date in the 3rd century BC to the second

de Vaux’s view, however, claiming that pottery serves as connecting link between the

settlem

10.6.3. Another source, providing complementary information

K.Rasmussen has attempted a fairly new method for provenance determination on

Qumran pottery and a completely new approach for determining their f

ssen 2003). He measured magnetic susceptibility and thermoluminescence sensitivity

on twelve samples, the same of which were analysed by neutron activation analysis. Three

samples were identified as imports, and this c

peratures of the samples too. One of the outliers was TL dated to the 20 century,

while the two others remained unparalleled also in the INAA data set.

The eso

H

century AD”.

10.7. Summary

As a conclusion of the provenance study it can be stated, that the main goals were

reached: by its chemistry Qumran pottery was traceable to their places of manufacture. The

widely accepted standpoint of de Vaux, that all the pottery was locally manufactured has

proved to be insupportable. It was possible to determine five chemically different groups of

pottery and to localize their probable provenance.

ent and the caves has been corroborated. It can be stated with some confidence, that

there is no difference in chemical composition between the pottery from the settlement and

69


that of the caves. A new evidence, connecting the settlement to the habit of scribal activity,

and by this to the caves has also been provided.

the analytical results, can help understand who the people were who lived in Qumran and with

whom they were in contact.

Because a diverse interrelation is traceable trough the ceramic material, not only with

sites quite near to Qumran, like Jericho, but also with the farther Eastern side of the Dead Sea.

A careful inquire in the settlement’s setup, the study of the distribution of pottery

types and possible functions of the different rooms, as well as cave materials in the light of

70

Synthesis

Synthesis

Qumran’s unique cultural heritage has been the object of intense fascination and

extreme controversy. Thousands of research studies focused on the better understanding of

the spiritual, as well as material inheritance of the Dead Sea community. Nevertheless,

Qumran research evokes innumerable questions, much more than we can answer reliably.

Part of these questions cannot be answered by the own conventional methods of

archaeology. Science provides a different and less subjective approach. Within the past few

years Qumran research has received a new dimension: a multidisciplinary project has been

started, aiming the study of the site and its people by scientific means, among them neutron

activation analysis.

Instrumental neutron activation analysis has been applied to Qumran ceramics with the

primary objective of establishing the chemical composition of potteries that can be traced to

site-specific manufacture centres and so translated into trade patterns and interregional

contacts. Reliable scientific information must be based on results produced by an analytical

technique, which has an appropriate accuracy, precision, sensitivity, resolution power and

fitness of purpose to be applied to the archaeological problem.

Neutron activation analysis is a highly developed analytical method, where

fundamental research has been limited for some time. Nevertheless, the inherent

characteristics of nuclear analysis justify studies of, and with INAA. To make the existing

knowledge on the technique available for utilization, i.e. a kind of “strategic” research, is an

obvious demand in each laboratory. To offer long-term opportunities for the multi-element

analysis of archaeological ceramics, the following developments have been directed:

Irradiation channels with the highest thermal neutron flux were chosen and spatial and

spectral variations of the neutron-flux were monitored. By independent experiments k-factors

for the most important (n,γ) reactions and γ-ray energies of the resulting isotopes were

determined. A systematic analysis of different clays, as well as archaeological ceramics of

different dates, pastes and fabrics was performed to define the most informative elements.

Sampling technique, necessary and sufficient sample masses, the optimal number of samples,

monitors and standards per batches were defined. Timing protocols were set, counting

geometry was fixed. On different ceramic types homogeneity studies were performed, to

71

Synthesis

check, whether a simple sample of about 50 mg can be considered representative for a whole

vessel.

To demonstrate the full potential of the technique, a Standard Operation Procedure has

been elaborated for the analysis of archaeological ceramics. This procedure comprises the

pottery-optimized analytical protocol, the estimation of the uncertainty budget of the

measurements, performance capabilities of the technique and the validation of the method in a

quality control/quality assurance system.

Aiming to improve the laboratory’s overall performance, a quality assurance program

has been accomplished, which resulted in the accreditation of the laboratory according to the

ISO/IEC 17025 International Standard.

The power of the technique has been proved, but to exploit its great potential to

address cultural and social issues, involving ceramics, an archaeologically coherent research

design was elaborated. It must be applied within a clearly formulated archaeological context,

where questions can be posed knowing the given socio-economic structure, historical

background, basic forms of human behaviour.

The Qumran pottery project meets these requirements. On the basis of the immense

knowledge built up by the means of exegesis, historical research and archaeological evidence

concerning the cultural heritage of the Dead Sea Scrolls and Qumran, definite questions have

been formulated to answer them by scientific means. In all of the many research studies

focused on Qumran the primary objective has always been to establish a connection between

the finds of Qumran settlement with those of the caves. Pottery can provide the best evidence

for proving the contact as the same unique ceramic types were discovered in the building

complex and in the caves. Peculiarities of Qumran’s ceramic corpus led to a general opinion

that all the pottery was made at the site, propping the idea of a closed ascetic community as

Qumran’s inhabitants. Stylistic approach however has its shortcomings, style is a cultural

trait, without geographical specificity. Nevertheless, pottery has a specific characteristic

giving definite answer concerning its provenience: chemical composition. By determining the

chemical fingerprint of pottery pieces they can be traced back to their place(s) of manufacture,

thus enabling us to establish trade links or find proofs for human relations.

The main goals of this project were to uncover the interrelations between the

Qumranites and the ceramic remains in the caves, and also to establish Qumran’s relations to

other people and sites by the Dead Sea and farther remote.

Systematic sampling and subsequent analysis of clay and mud samples, inner lining of

kilns, unfired and fired clay-balls, oven stoppers, kiln wasters served as reference material for

72

Synthesis

defining Qumran’s local chemical fingerprint. Clay and ceramic samples from other places,

like Jericho, Jerusalem, Hebron, Callirhoe and ‘Ain Feshkha were also sampled and analysed

to help workshop assignment. The Qumran pottery set consisted of 166 samples, representing

a variety of styles including the unique scroll jars, found in the settlement as well as the caves.

As a result of the analysis of all these samples, a data-bank of ceramic materials has

been developed, comprising the chemical profile of different pottery types of Qumran and the

Dead Sea region, in the time period of 200 BC-70 AD.

To help place the derived analytical data into archaeological context different

procedures of multivariate statistics have been applied. By an iterative classification treatment

the partitioning of the data-set has been achieved, compositional groups were created and

placed into spatial perspective.

The main goals of the provenance study were reached: by its chemistry Qumran

pottery was traceable to their places of manufacture. According to our results, about 33

percents of the analysed pottery were produced locally, in Qumran. A relatively large part of

pottery has connection with Jericho, and another bigger group of vessels has a chemical

fingerprint of the Hebron (Beit ‘Ummar) type Motza Clay. There are quite some pottery

wares enlightening a possible Edom/Nabatea connection.

The idea, claiming that pottery serves as a connecting link between the settlement and

the caves has been corroborated, there is no difference in the chemical composition between

the pottery from the settlement and that of the caves.

The question of the settlement’s closeness has got a different new light: through the

ceramic material a diverse interrelation is traceable, not only with sites and people near to

Qumran, but also with people of the Eastern side of the Dead Sea.

The intention to enrich Qumran studies by the application of methods of analysis from

the field of natural sciences proved to be fruitful. The extent to which these results can

contribute to the wider historical and archaeological narrative is difficult to asses, but

different methodological and intellectual approaches can provide complex and more accurate

explanations, and the impact of a joint acquisition of knowledge can be considerable.

73

Tables.

Tables Table 1. k-factors for the two detectors Isotope Eg [keV] T1/2 [s] I/s Kwell Kpop uncertaintySm-153 103,18 168120 14,40 4,909E-01 4,60E-01 3 Ce-141 145,44 2808000 1,20 5,266E-03 5,27E-03 3 Lu-177 208,36 579744 0,55 1,769E-01 1,87E-01 3,7 Np-239 228,18 203472 103,40 1,593E-02 1,62E-02 3,5 Np-239 277,60 203472 103,40 1,286E-02 1,30E-02 3,5 Pa-233 311,98 2332800 11,53 2,832E-02 2,86E-02 2,8 Cr-51 320,08 2393453 0,53 2,192E-03 2,21E-03 3 Yb-175 396,32 362016 0,46 2,036E-02 2,24E-02 3 Hf-181 482,03 3663360 2,52 2,454E-02 2,42E-02 3 La-140 487,03 145008 1,24 3,303E-02 3,26E-02 2,5 La-140 1596,50 145008 1,24 2,370E-02 2,16E-02 2,5 Ba-131 496,00 1019520 14,80 4,954E-05 4,88E-05 4,5 Nd-147 91,00 948672 2,00 1,231E-03 1,64E-03 7 Nd-147 531,00 948672 2,00 1,728E-04 2,54E-04 7 As-76 559,10 94752 13,60 3,246E-02 3,17E-02 3 Sb-122 563,93 233280 33,00 4,090E-02 4,00E-02 2,5 Sb-124 602,71 5201280 28,80 2,433E-02 2,37E-02 3 Sb-124 1691,00 5201280 28,80 4,757E-03 4,33E-03 4 Cs-134 604,70 65166444 11,80 2,757E-01 2,86E-01 3 Cs-134 795,84 65166444 11,80 1,966E-01 2,01E-01 3 Tb-160 879,36 6246720 17,90 4,573E-02 4,33E-02 5 Sc-46 889,25 7239456 0,43 3,611E-01 3,64E-01 2,2 Sc-46 1120,30 7239456 0,43 2,963E-01 2,94E-01 2,2 Rb-86 1076,60 1612224 14,80 3,032E-04 2,84E-04 6 Fe-59 1099,20 3845664 0,97 1,827E-05 1,79E-05 3 Fe-59 1291,50 3845664 0,97 1,224E-05 1,19E-05 3 Zn-65 1115,50 21072960 1,91 1,708E-03 1,59E-03 4,6 Ta-182 1221,40 9886752 33,30 2,602E-02 3,14E-02 5 Co-60 1332,50 166352733 1,99 2,895E-01 2,67E-01 3 Co-60 1173,10 166352733 1,99 3,232E-01 3,01E-01 3 Na-24 1368,50 53852 0,59 9,880E-03 9,11E-03 3 Eu-152 1408,00 422871840 0,61 1,678E+00 1,54E+00 3 K-42 1524,70 44496 0,97 2,107E-04 1,93E-04 3

74

Tables.

Table 2. Trace element concentrations in different clay-minerals Element Kaolinite Kaolinite Kaolinite Kaolinite Illite Bentonite Halloysite Mád Szegi Budakeszi Sárisáp Fűzérradvány Istenmezeje Cserszegtomaj

Sc 7,6 13,7 10,3 15,9 7,0 4,3 4,4 Cr 12,3 480,0 58,5 39,5 7,9 35,2

Fe% 0,2 3,02 1,19 0,89 0,29 1,89 0,14 Co 0,6 5,7 3,3 0,17 0,9 0,8 Rb 47,4 51,2 477,0 Sb 19,5 48,9 2,1 4,2 Cs 1,02 5,6 10,1 3,2 53,6 0,9 1,8 Ba 200 195 175 566 91 188 La 12,6 62,2 39,0 13,0 18,0 12,1 1,8 Ce 31,1 66,0 18,9 28,4 31,3 29,9 10,2 Nd 26,2 21,3 13,3 16,7 Sm 6,1 21,5 32,9 2,5 2,6 7,3 10,2 Eu 0,3 3,2 0,4 0,4 0,7 Tb 1,0 6,5 5,0 0,6 1,1 0,5 Tm 3,2 3,4 0,6 1,3 Yb 1,8 9,7 10,5 1,0 0,5 1,5 0,6 Lu 0,35 1,8 2,0 0,21 0,14 0,3 0,7 Hf 4,0 14,0 11,1 2,8 6,0 1,8 Ta 1,5 4,6 2,0 0,8 1,3 3,3 Th 23,1 91,7 41,8 8,2 9,3 12,0 0,7 U 2,8 4,0 16,6 2,0 1,8 7,0 20,7

Table 3. Homogeneity study of Terra Sigillata pottery (10 samples from one sherd)

Element Mean value STDEV ppm %

Sc 12,1±0,2 1,8 Cr 94±14 14,4

Fe% 3,34±0,14 4,2 Co 12,3±0,4 2,9 Rb 271±30 11,1 Cs 55,9±2,5 4,4 La 46,6±1,9 4,0 Ce 102±17 16,0 Eu 1,15±0,10 8,4 Yb 2,2±0,2 9,4 Lu 0,36±0,04 12,0 Hf 3,4±0,3 8,5 Th 19,4±0,9 4,5 U 4,9±1,0 20,0

75

Tables.

Table 5.Uncertainty components of INAA Uncertainty components Typical value Sample preparation Balance: standard deviation of 3x10 measurements.

0.016 mg

Mass determination of the sample 0.05-0.1g Mass determination of gold foil 5-10 mg ≈0.3% Mass determination of zirconium foil 30-40 mg, ≈0.03% Concentration of gold foil: according to certificate 0.02% Moisture determination: depends on sample type; can be evaluated by repetitive measurements.

Generally negligible

Variation of isotopic abundance: in our case only for uranium it may be important.

Negligible

Impurities of irradiation vials: concentration of some elements in PE vials is high comparing to measurand .(See Table 6.)

below 1%

Irradiation Irradiation geometry: neutron gradient practically very low, but using 3 gold foils in sandwich type geometry, can be minimised

0.1-0.5 %

Neutron self-shielding: in most cases negligible 0.1% Irradiation time: samples and gold foils are irradiated together, uncertainty is max. 5 min compare to 8 hour of duration.

Negligible,

Nuclear reaction interference: in case of high uranium concentration correction is needed.

in most cases negligible

Neutron spectrum variation: using Zr foils correction can be derived. Calculated by Spread Sheet Method.

after correction negligible

Gamma spectrometry Counting statistic: standard uncertainty is calculated by Sampo90 evaluation software.

0.2-30%

Gamma self-absorption: Negligible Dead time effect: up to 10% dead time

after correction less then 2%

Random coincidences: standardisation performed in the same geometry there is no difference between coincidences.

Negligible

Decay timing: 5 min/week or month Negligible Counting time: 0.2 sec/5000-10000 sec Negligible Background correction: in our laboratory correction for Co-60 is needed. in most cases negligible Counting geometry differences: the measurement is done at least 5 cm from the detector; the sample and the comparator are measured in the same geometry (see Table 7).

2-3% mainly from sample volume differences

Gamma interference: should be minimised by using more gamma lines and by repeating the counting. In special cases correction is needed.

Negligible

Uncertainty of standardisation: Uncertainty of the k-factors had been estimated by repeated measurements of different RMs. (see Table 8.and 9.)

2-10%

76

Tables.

Table 6. Impurities of polyethylene vials: [µg]

Sm 10-5-10-6

Mo 10-2-10-4

Cr 0,1-0,01 Au 10-4-10-5

Sb 10-3-10-4

Sc 10-4-10-5

Fe 0.1-1 Zn 0.1-0.01 Co 10-2-10-3

Na 0.01-0.3

Table 7. Counting geometry: uncertainty was determined by measuring samples with different quantities (20 and 60 mg respectively)

Samples with 60 mg

Samples with 20 mg

Element

Av. conc. Ppm

STDEV of 3 samples

Av. conc. ppm

Deviation

Ce 86.3 0.7% 88.27 2.2% Co 72.87 2.2% 76.00 3.0% Cr 57.07 1.9% 59.40 1.5% Eu 4.74 2.6% 4.84 0.4% Fe 44800 2.0% 46500 2.6% La 65.43 0.9% 68.60 3.4% Lu 1.33 1.3% 1.44 5.1% Na 32300 0.5% 33500 2.8% Sc 26.57 1.1% 27.90 3.6% Sm 17.90 2.1% 19.09 4.2% Th 13.37 1.9% 14.40 5.9%

STDEV: standard deviation of repeated measurements Deviation: deviation between the results in case of sample with low (20 mg) and high (60 mg) mass. Average deviation is around 3%.

77

Tables.

Table 8. Results of measurement of RMs: FA: NBS SRM 1633a Coal Fly Ash; S7: IAEA Soil 7; MS: GBW 07313 Marine Sediment:

FA S7 MS FA S7 MS FA S7 MS No. of measurements

9 3 15 9 3 15 9 3 15

As As As Ba Ba Ba Ce Ce Ce Cert. val.[ppm] 145 13.4 5.8 1500 159 4400 180 61 92

u 15 0.8 0.8 30 200 7 8 Meas. Val.[ppm] 138 13.30 6.18 1422 170 4455 170 61.0 93.6

σ 2.6 0.36 0.71 91 8.02 192 9.8 1.0 4.3

Co Co Co Cr Cr Cs Cs Cs Cert. val.[ppm] 46 8.9 76.7 196 58.4 11 5.4 9.4

u 0.9 1.2 6 1.3 0.76 0.7 Meas. Val.[ppm] 42 8.67 71.1 193 58.5 10 5.43 8.66

σ 0.51 0.38 2.1 6.2 2.3 0.21 0.21 0.32

Eu Eu Eu Fe% Fe% Fe% Hf Hf Hf Cert. val.[ppm] 4 1 5.3 9.4 2.57 4.6 7.6 5.1

U 0.2 0.3 0.1 0.1 0.4 Meas. Val.[ppm] 3 0.94 4.84 10 2.69 4.43 7.16 5.13 4.45

σ 0.10 0.09 0.14 0.20 0.08 0.13 0.49 0.47 0.20

FA S7 MS FA S7 MS FA S7 MS La La La Lu Lu Lu Na Na % Na %

Cert. val.[ppm] 28 67.8 0.3 1.46 1700 0.24 3.568 u 2.0 2.9 0.19 100 0.04

Meas. Val.[ppm] 77.6 25.7 65.5 0.98 0.29 1.32 1730 0.22 3.21 σ 1.97 0.70 2.34 0.04 0.01 0.07 80.09 0.01 0.09

Nd Nd Nd Rb Rb Rb Sb Sb Sb Cert. val.[ppm] 30 91.8 131 51 97.3 7 1.7 1.85

u 5 3.9 2 4.5 2.6 0.2 0.35 Meas. Val.[ppm] 58.1 29.0 81.6 128 48 84 6.43 1.70 2.08

σ 11.6 11.3 12.8 11.4 5.5 13 0.10 0.20 0.08

Sc Sc Sc Sm Sm Sm Ta Ta Ta Cert. val.[ppm] 40 8.3 25.6 5.1 21.5

u 1.1 2.9 0.36 1.3 Meas. Val.[ppm] 38.5 8.47 26.5 16.4 4.84 20.0 2.0 0.96 1.11

σ 0.71 0.12 0.76 0.29 0.20 0.59 0.2 0.08 0.13

Tb Tb Tb Th Th Th U U U Cert. val.[ppm] 2.53 3.4 24.7 8.2 13.9 10.2 2.6 1.98

u 0.04 0.3 1 1.1 1.1 0.3 0.55 0.47 Meas. Val.[ppm] 2 0.67 3.18 24.45 8.07 13.45 10.1 2.63 1.83

σ 0.3 0.07 0.20 0.53 0.47 0.58 0.18 0.15 0.43

Yb Yb Yb Zn Zn Zn Cert. val.[ppm] 7.5 2.4 9.8 220 104 160

u 0.13 0.4 1.1 10 6 3 Meas. Val.[ppm] 8 2.29 9.88 241 106 194

σ 0.2 0.11 0.37 45 15 25 σ: standard deviation of the results [ppm]

78

Tables.

Table 9. Uncertainty of k-factors:

Radionuclide Energy

keV Uncertainty of Radionuclide Energy

keV Uncertainty ofk-factors % k-factors %

As-76 559.1 3 Na-24 1368.5 3 As-76 657.0 5 Nd-147 91 7

Au-198 411 2 Nd-147 531 7 Ba-131 496 4.5 Np-239 228.2 3.5 Ce-141 145.4 3 Np-239 277.6 3.5 Co-60 1173.1 3 Pa-233 312 2.8 Co-60 1332.5 3 Rb-86 1076.6 6

320.1 3 Sb-122 563.9 2.5 Cr-51 Cs-134 604.7 3 Sb-124 602.7 3 Cs-134 795.8 3 Sb-124 1691 4 Eu-152 1408 3 Sc-46 889.3 2.2 Fe-59 1099.2 3 Sc-46 1120.3 2.2 Fe-59 1291.5 3 Sm-153 103.2 3

Hf-181 482 3 Ta-182 1221.4 5 La-140 487 2.5 Tb-160 879.4 5 La-140 1596.5 2.5 Yb-175 396.3 3 Lu-177 208.4 3.7 Zn-65 1115.5 4.6

Table 10. Typical values of detection limit

Det. limit Det.

Limit Element ppm Element ppm

As 2,80 Nd 25 Ba 300 Rb 35 Ce 4,5 Sb 0,4 Co 2 Sc 0,06 Cr 9 Sm 0,1 Cs 0,9 Ta 0,2 Eu 0,12 Tb 0,6 Fe 600 Th 0,7 Hf 0,8 U 1,7 La 0,5 Yb 0,7 Lu 0,1 Zn 20 Na 80

79

Tables.

Table 11. Results of NBS SRM 1633a Coal Fly Ash. Reference values from Bode (1992)

Element Measured Reference Relative Value[ppm] STDEV[ppm] Value[ppm] STDEV[ppm] deviation As 138,0 2,6 145 15 -0,048 Ba 1422 91 1420 100 0,001 Ce 170,0 9,8 175 7 -0,029 Co 42,0 0,5 43 3 -0,023 Cr 193 6 196 6 -0,015 Cs 10,0 0,2 10,5 0,7 -0,048 Eu 3,50 0,10 3,7 0,2 -0,054 Fe % 10,00 0,200 9,4 0,1 0,064 Hf 7,16 0,49 7,4 0,3 -0,032 La 77,6 2,0 84 8 -0,076 Lu 0,98 0,04 1,12 0,18 -0,125 Na % 1730 80 1700 100 0,018 Nd 58 11 Rb 128 11 131 2 -0,023 Sb 6,43 0,10 6,8 0,4 -0,054 Sc 38,5 0,7 39 3 -0,013 Sm 16,4 0,3 17 1,5 -0,035 Ta 2,0 0,2 2 0,2 0,000 Th 24,5 0,5 24,7 0,3 -0,010 U 10,1 0,2 10,2 0,1 -0,010 Yb 8,0 0,2 7,4 0,7 0,081 Zn 241 45 220 10 0,095

Element u result P% Result As 0,46 passed 10,5 passed Ba 0,01 passed 9,5 passed Ce 0,42 passed 7,0 passed Co 0,33 passed 7,1 passed Cr 0,35 passed 4,4 passed Cs 0,68 passed 7,0 passed Eu 0,89 passed 6,1 passed Fe % 2,68 passed 2,3 passed Hf 0,42 passed 8,0 passed La 0,78 passed 9,9 passed Lu 0,76 passed 16,6 passed Na % 0,23 passed 7,5 passed Nd Rb 0,27 passed 8,7 passed Sb 0,90 passed 6,1 passed Sc 0,16 passed 7,9 passed Sm 0,39 passed 9,0 passed Ta 0,00 passed 14,1 passed Th 0,41 passed 2,5 passed U 0,49 passed 2,0 passed Yb 0,82 passed 9,8 passed Zn 0,46 passed 19,2 passed Accuracy criteria (u-test acceptance): u<=3.29 Precision criteria: P<=25%

80

Tables.

Table 12. Results of Perlman/Asaro Standard Pottery

Element Measured Reference Relative Value[ppm] STDEV[ppm] Value[ppm] STDEV[ppm] Deviation As 28,0 2,1 30,8 0,22 -0,093 Ba 738 43 712 32 0,036 Ce 75,8 5,4 80,3 3,9 -0,056 Co 13,7 0,5 14,06 0,15 -0,024 Cr 108 7 102 4 0,055 Cs 7,9 0,7 8,31 0,55 -0,045 Eu 1,30 0,13 1,29 0,03 0,005 Fe % 1,015 0,040 1,017 0,012 -0,002 Hf 6,06 0,23 6,23 0,44 -0,027 La 44,5 1,9 44,9 0,45 -0,008 Lu 0,38 0,03 0,402 0,036 -0,060 Na % 0,243 0,006 0,261 0,04 -0,068 Nd 26 3 Rb 73 12 70 1 0,037 Sb 1,73 0,06 1,71 0,05 0,014 Sc 18,6 1,1 20,55 0,03 -0,095 Sm 6,0 0,3 5,78 0,12 0,038 Ta 1,6 0,2 1,55 0,04 0,015 Th 13,8 0,8 13,96 0,04 -0,011 U 5,1 0,7 4,82 0,14 0,059 Yb 2,5 0,4 2,96 0,06 -0,151 Zn 60 5 59 1 0,023

Element u result P% Result As 1,37 passed 7,4 passed Ba 0,48 passed 7,3 passed Ce 0,68 passed 8,6 passed Co 0,68 passed 3,6 passed Cr 0,73 passed 7,3 passed Cs 0,40 passed 11,4 passed Eu 0,05 passed 10,2 passed Fe % 0,05 passed 4,1 passed Hf 0,34 passed 8,0 passed La 0,20 passed 4,3 passed Lu 0,50 passed 12,3 passed Na % 0,44 passed 15,5 passed Nd Rb 0,22 passed 16,1 passed Sb 0,31 passed 4,4 passed Sc 1,80 passed 5,8 passed Sm 0,67 passed 5,5 passed Ta 0,12 passed 12,7 passed Th 0,18 passed 5,9 passed U 0,38 passed 14,5 passed Yb 1,11 passed 15,9 passed Zn 0,26 passed 8,5 passed Accuracy criteria (u-test acceptance): u<=3.29 Precision criteria: P<=25%

81

Tables.

Table 13. Reproducibility measurements of GBW 07313 Marine Sediment

(five samples) Element Average conc.

ppm STDEV

ppm Uncertainty

ppm Precision index %

As 5.42 0.63 0.60 17.7 Ba 4400 235 250 7.3 Ce 89.9 1.4 3.30 9.4 Co 73.8 1.81 2.50 3.7 Cr 58.5 2.33 3.00 5.6 Cs 8.50 0.31 0.40 8.8 Eu 4.82 0.16 0.18 6.8 Fe 45300 1000 1500 4.0 Hf 4.38 0.13 0.22 La 66.3 1.46 2.20 5.4 Lu 1.37 0.06 0.06 13.7 Na 32600 561 1100 3.6 Nd Rb 93.0 10 10 11.1 Sb 2.05 0.06 0.10 19.5 Sc 26.94 0.62 0.70 11.6 Sm 18.32 0.64 0.60 6.8 Ta Tb 3.24 0.09 0.21 10.9 Th 13.60 0.48 0.50 8.7 U 0.30

Yb 9.75 0.25 0.40 12 Zn 224 15 25 11.3

Conclusion: Standard deviation of 5 measurements are lower then the calculated uncertainty.

Acceptance criteria: Precision index is lower then 25% for all elements.

82

Tables.

Table 14. Results of “Tea leaves”

Intercomparison 2002 INCT-TL-1 Element Unit Results Reference Relative Abs. % Measured Unc. Unc. Ref value Unc. deviation As ppb 93,0 8,0 8,6 106,0 21,0 -0,123 Ba ppm 45,9 7,2 15,7 43,2 3,9 0,062 Br ppm 12,5 0,6 5,0 12,3 1,0 0,012 Ca ppm 6820,0 886,6 13,0 5820,0 520,0 0,172 Ce ppb 847,0 31,3 3,7 790,0 76,0 0,072 Cl ppm 573,0 48,0 Co ppb 383,0 16,9 4,4 387,0 42,0 -0,010 Cr ppm 2,12 0,1 5,9 1,9 0,2 0,110 Cs ppm 4,0 0,1 3,3 3,6 0,4 0,094 Cu ppm 20,4 1,5 Eu ppb 116,0 10,0 8,6 49,9 9,4 Fe ppm 513 16,9 3,3 432,0 0,188 Hg ppb 4,9 0,7 Hf ppb 28,0 K % 1,77 0,1 5,2 1,7 0,1 0,041 La ppb 983,0 32,4 3,3 1000,0 70,0 -0,017 Lu ppb 18,3 0,9 4,9 16,8 2,4 0,089 Mn ppm 1733,0 60,7 3,5 1570,0 110,0 0,104 Na ppm 26,3 0,9 3,3 24,7 3,2 0,065 Rb ppm 85,9 5,5 6,4 81,5 6,5 0,054 Sb ppb 52,7 2,3 4,4 50,0 0,054 Sc ppb 257,0 6,7 2,6 266,0 24,0 -0,034 Sm ppb 190,0 6,3 3,3 177,0 22,0 0,073 Th ppb 31,7 5,5 17,3 34,3 4,8 -0,076 Ti ppm 30,0 V ppm 2,0 0,4 -1,000 Yb ppb 107,0 4,9 4,6 118,0 13,0 -0,093 Zn ppm 35,5 1,7 4,8 34,7 2,7 0,023

83

Tables.

Table 14. continued

INCT-TL-1 Element Unit Accuracy Precision u Result P% Result As ppb 0,58 passed 21,6 passed Ba ppm 0,33 passed 18,1 passed Br ppm 0,13 passed 9,5 passed Ca ppm 0,97 passed 15,8 passed Ce ppb 0,69 passed 10,3 passed Cl ppm Co ppb 0,09 passed 11,7 passed Cr ppm 0,83 passed 12,9 passed Cs ppm 0,87 passed 10,8 passed Cu ppm Eu ppb 4,82 Error 20,7 passed Fe ppm Hg ppb Hf ppb K % 0,46 passed 8,8 passed La ppb 0,22 passed 7,7 passed Lu ppb 0,59 passed 15,1 passed Mn ppm 1,30 passed 7,8 passed Na ppm 0,48 passed 13,4 passed Rb ppm 0,52 passed 10,2 passed Sb ppb 1,16 passed 4,4 passed Sc ppb 0,36 passed 9,4 passed Sm ppb 0,57 passed 12,9 passed Th ppb 0,36 passed 22,3 passed Ti ppm V ppm Yb ppb 0,79 passed 11,9 passed Zn ppm 0,25 passed 9,1 passed Accuracy criteria (u-test acceptance criteria): u<=3.29 Precision criteria : P<=25%

84

Tables.

Table 15. Results of “Mixed Polish Herbs” Intercomparison 2002 INCT-MPH-2 Element Unit Reference Relative abs. % Measured Unc. Unc. Ref.value Unc. deviation As ppb 200,0 11,8 5,9 191,0 23,0 0,047 Ba ppm 32,5 2,5 Br ppm 7,4 0,4 5,0 7,7 0,6 -0,047 Ca % 1,3 0,1 7,0 1,1 0,1 0,204 Ce ppm 1,2 3,3 1,1 0,1 0,045 Cl % 0,3 0,0 Co ppb 220,0 7,3 3,3 210,0 25,0 0,048 Cr ppm 1,94 0,1 3,7 1,7 0,1 0,148 Cs ppm 88,0 7,3 8,3 76,0 7,0 0,158 Cu ppm Eu ppb 22,0 1,5 6,8 15,7 1,8 0,401 Fe ppm 518 17,1 3,3 460,0 0,126 Hg ppb 17,6 1,6 Hf ppb 236,0 20,0 K % 1,95 0,1 5,2 1,9 0,1 0,021 La ppb 583,0 19,2 3,3 571,0 46,0 0,021 Lu ppb 8,0 0,5 6,3 9,0 1,5 -0,111 Mn ppm 202,0 7,1 3,5 191,0 12,0 0,058 Na ppm 458,0 31,1 6,8 350,0 0,309 Rb ppm 11,8 0,7 6,2 10,7 0,7 0,103 Sb ppb 64,0 2,4 3,7 65,5 9,1 -0,023 Sc ppb 127,0 3,3 2,6 123,0 9,0 0,033 Sm ppb 96,3 3,2 3,3 94,4 8,2 0,020 Th ppb 160,0 5,8 3,6 154,0 13,0 0,039 Ti ppm 34,0 V ppm 952,0 163,0 Yb ppb 52,5 3,4 6,5 52,7 6,6 -0,004 Zn ppm 36,7 1,8 4,8 33,5 2,1 0,096

85

Tables.

Table 15. continued INCT-MPH-2 Element Unit Accuracy Precision u Result P% Result As ppb 0,35 passed 13,4 passed Ba ppm Br ppm 0,51 passed 9,4 passed Ca ppb 1,92 passed 9,5 passed Ce ppb 0,50 passed 8,9 passed Cl ppm Co ppb 0,38 passed 12,4 passed Cr ppm 1,68 passed 8,5 passed Cs ppm 1,19 passed 12,4 passed Cu ppm Eu ppb 2,69 passed 13,3 passed Fe ppm Hg ppb Hf ppb K % 0,25 passed 8,2 passed La ppb 0,24 passed 8,7 passed Lu ppb 0,63 passed 17,8 passed Mn ppm 0,79 passed 7,2 passed Na ppm 3,47 passed 6,8 passed Rb ppm 1,09 passed 9,0 passed Sb ppb 0,16 passed 14,4 passed Sc ppb 0,42 passed 7,8 passed Sm ppb 0,22 passed 9,3 passed Th ppb 0,42 passed 9,2 passed Ti ppm V ppm Yb ppb 0,03 passed 14,1 passed Zn ppm 1,17 passed 7,9 passed Accuracy criteria (u-test acceptance criteria): u<=3.29 Precision criteria : P<=25%

86

Tables.

Table 16. Results of “Vienna Dust” NAT-7 Vienna dust V-25 Element Unit Measured Reference Relative Value Unc. Value Unc deviation As mg/cm2 Ca mg/cm2 21320 2550 22060 4007 -0,034 Co mg/cm2 12,4 0,6 14,63 2,62 -0,152 Cr mg/cm2 312 9 486 57 -0,358 Cu mg/cm2 2270 160 1443 159 0,573 Fe mg/cm2 48000 1600 50660 6664 -0,053

Mn mg/cm2 570 30 566,7 130 0,006 Accuracy Precision Element u result P% Result

As Ca 0,16 passed 21,75 passed Co 0,83 passed 18,55 passed Cr 3,02 passed 12,08 passed Cu 3,67 failed 13,08 passed Fe 0,39 passed 13,57 passed Mn 0,02 passed 23,54 passed Accuracy criteria (u-test acceptance): U≤3.29 Precision criteria: P≤25% Table 17. Results of “Prague Dust” NAT-7 Prague dust P-76 Element Unit Measured Reference Relative Value Unc. Value Unc. deviation As mg/cm2 31 4 29 4 0,069 Ca mg/cm2 Co mg/cm2 16,7 0,8 16,15 2,16 0,034 Fe mg/cm2 58000 1940 58830 5949 -0,014 Mn mg/cm2 660 30 621 84 0,063 Sb mg/cm2 179 6 171,9 16,2 0,041

Ti mg/cm2 3600 330 3486 451 0,033 Accuracy Precision Element u result P% result As 0,36 passed 18,6 passed Ca passed passed Co 0,24 passed 14,2 passed Fe 0,13 passed 10,7 passed Mn 0,44 passed 14,3 passed Sb 0,41 passed 10,0 passed Ti 0,20 passed 15,9 passed Accuracy criteria (u-test acceptance): U≤3.29 Precision criteria: P≤25%

87

Tables.

Table 18. Analysis of “Motza Clay” samples Element Measured Hebrew University Relative Value[ppm] STDEV[ppm] Value[ppm] STDEV[ppm] deviation As 7,43 0,8 7,79 0,66 -0,046 Ba Ce 44,4 5,8 45,2 1,45 -0,018 Co 11,2 1,1 11,8 0,23 -0,053 Cr 94 6 93,8 2,07 -0,001 Cs 5,1 0,3 5,68 0,16 -0,102 Eu 1,15 0,17 1,08 0,02 0,065 Fe % 3,13 0,32 3,01 0,01 0,040 Hf 3,52 0,25 3,3 0,01 0,067 K% 3,65 0,19 4,04 0,01 -0,097 La 22,8 1,9 21,09 0,16 0,081 Lu 0,29 0,02 0,3 0,02 -0,033 Na % 650 180 490 100 0,327 Nd Rb 95,30 8 113,5 2,2 -0,160 Sb 0,40 0,03 0,4 0,01 0,000 Sc 14,63 1,02 16,16 0,06 -0,095 Sm 4,94 0,50 4,27 0,06 0,157 Ta 0,69 0,14 0,63 0,07 0,095 Th 6,60 0,69 6,91 0,1 -0,045 U 2,57 0,38 2,17 0,05 0,184 Yb 1,98 0,15 2,02 0,11 -0,020 Zn 76,10 9,35 Element u result P% Result As 0,35 passed 13,7 passed Ba Ce 0,13 passed 13,5 passed Co 0,55 passed 10,2 passed Cr 0,01 passed 7,1 passed Cs 1,90 passed 5,8 passed Eu 0,41 passed 14,9 passed Fe % 0,37 passed 10,2 passed Hf 0,88 passed 7,1 passed La 0,88 passed 8,5 passed Lu 0,35 passed 9,6 passed Na % 0,78 passed 34,4 failed Nd Rb 2,25 passed 8,4 passed Sb 0,00 passed 7,9 passed Sc 1,50 passed 7,0 passed Sm 1,33 passed 10,2 passed Ta 0,38 passed 23,1 passed Th 0,44 passed 10,6 passed U 1,04 passed 15,0 passed Yb 0,22 passed 9,3 passed Zn Accuracy criteria (u-test acceptance): u<=3.29 Precision criteria: P<=25%

88

Tables.

Table 19. Zeuner’s results Zeuner's analysis of Qumran samples List of samples: 1. L 75 2. L75 3. L B2 4. Cistern 58 5. Lisan Marl Sample 5.Lisan Marl unleached leached Silica, clay minerals 41.7% 48.7% Limestone + dolomite dust 43.9% 51.3% Soluble salts 14.4% Sample CaCO3% MgCO3% CaSO4% silica+clay%

1. 14,8 16,9 0,3 68,0 2. 18,1 16,0 2,6 63,4 3. 64,4 16,7 0,9 18,0 4. 56,0 16,1 1,9 26,1

89

Tables.

Table 20. Chemical Groups of Qumran Pottery

I.

Local to Qumran II.

Hebron type MotzaIII.

Jericho IV.

Jordan connection V.

Jericho 2

Scroll jars 120, 132, 139, 156 115, 116, 117, 118, 198, 256 162, 163, 186, 187, 119, 122, 123, 124, 231, 240 125, 138, 153, 166, 164, 165, 199, 238, 245, 250, 255, 257 Store jars 121, 126, 127, 131 160, 184, 212, 241 234, 251, 267, 102 158 135, 136, 183, 210 236, 237, 276 142, 211, 284 265, 268, 284

Ovoid jars 133, 134 244 220, 239 237 242, 243

Lids 154, 161, 182 137, 246, 247, 248, 249, 279

Bowls 112, 190, 191, 213 173, 264, 188, 179 113, 170, 171, 172 180, 189, 269, 270 109, 253

263, 271, 151, 152 204, 253, 261, 262 275, 110, 111, 114 252 Jugs 203, 206, 207, 214 201, 202 216, 218, 266, 200 217 Cups 105, 106, 108, 273 107, 205, 258, 259, 272 260, 274

Various 193, 225, 150, 185 194, 228, 229 281, 283, 286, 290 266, 224

288, 289, 130, 150 291, 292 293, 294, 275

Ostraca 121, 134, 311, 312 120, 131, 212, 304 200, 203, 204, 205 201, 202 315 310, 313, 314, 318 206, 207, 211, 213 319, 320, 321 214, 216, 218, 220 309, 316, 308

90

Samples

List of samples QUM 100 Clay taken from Jericho brick QUM 101 Kiln inner lining L.84 QUM 102 Sherd from kiln make-up QUM 103 Kiln outer lining L.84 QUM 104 Kiln inner lining (other side of QUM 101) QUM 105 KHQ 1057 Cup L.59 QUM 106 KHQ 1055 Cup L.59 QUM 107 KHQ 1286 Cup L.65 QUM 108 KHQ 733 Cup L.39 lower floor, early QUM 109 KHQ 1624 Bowl, large, warped QUM 110 KHQ 1079 Bowl L.61 QUM 111 KHQ 1080 Bowl L.44 QUM 112 KHQ 1052 Bowl L.59 upper corner of L.44 QUM 113 KHQ 24 Bowl L.1 QUM 114 KHQ 1574-6 Decanter L.89 QUM 115 CAVE 8 Lump of clay on bottom of jar QUM 116 CAVE 8 Scroll jar of QUM 115 itself QUM 117 KHQ 27 Scroll jar L.2 QUM 118 KHQ 768 Scroll jar L.13 QUM 119 KHQ 764 Scroll jar L.13 QUM 120 KHQ 2553 Scroll jar L.124 QUM 121 KHQ 621 Jar with inscription L.34 QUM 122 CAVE 8 Scroll jar XVII (reddish fabric) QUM 123 CAVE 8 Scroll jar 11 (reddish fabric) QUM 124 CAVE 8 Scroll jar 3 (greyish fabric) QUM 125 CAVE 8 Scroll jar 1 QUM 126 KHQ 522 Silo QUM 127 KHQ 800 Funnel-filter L.45A QUM 128 KHQ 1301 Clay ball L.66 multiple perforation QUM 129 KHQ 2574 Clay ball L.131 whitish clay QUM 130 KHQ 2209 Clay ball L.130 reddish clay QUM 131 KHQ 1401 Jar with inscription in ink L.84 kiln QUM 132 CAVE GQ8 Scroll jar with blisters QUM 133 KHQ 1486 Ovoid jar L.81 QUM 134 CAVE 7Q6 Jar with ROMA inscription QUM 135 KHQ 49 Two handled cloche-storage jar L.4 QUM 136 KHQ 2107 Torpedo jar L.116 QUM 137 Q7 Bowl/lid on top of scroll jar QUM 138 Q7 Scroll jar as above, white wash QUM 139 GQ7 39 Scroll jar QUM 140 KHQ 2114 Real waster of pottery L.104 QUM 141 KHQ 2296 Oval lump oven lid L.130 QUM 142 KHQ 2045 Oval flat oven lid L.105 ins. oven QUM 143 KHQ 377 Round ball-like oven lid L.10A QUM 144 KHQ 2271 Round ball-like oven lid L.130 QUM 145 KHQ 1669 Oven cover with handle

91

Samples

QUM 146 KHQ 130 Roof stucco QUM 147 KHQ 376 Cover of oven L.10A QUM 148 KHQ 2622 40cm vat with fingerpierced handles QUM 149 KHQ 2465 Large handle QUM 150 KHQ 2046 Lid from oven lid+hillshaped handle L.105 QUM 151 KHQ 638 Miniature footbath lid L.31 QUM 152 KHQ 1139 Oval lid with bas. Relief cut handle QUM 153 GQ 29-25 Scroll jar QUM 154 GQ8 Q7 347742 Lid of scroll jar QUM 155 11 Q13 Chalcolitic crude pot (fishgrade design) QUM 156 KHQ 2504 Storage jar QUM 157 CAVE 11 „Negev” S-shape + fingerpr. Rim QUM 158 Feshka 256 Storage jar (Villa Locus 5.) QUM 159 GQ 29-22 Scroll jar QUM 160 KHQ 1492 Small scroll jar & lid L.81 QUM 161 KHQ 1466 Lid with 4 pierced handles L.80 QUM 162 KHQ 1465 Small scroll jar with 4 pierced handles QUM 163 GQ 39-1 Large scroll jar QUM 164 GQ8 Large scroll jar QUM 165 KHQ 2561A (2661A) larger scroll jar L.120 QUM 166 Q 39-7 Scroll jar QUM 167 Kiln lining QUM 168 KHQ 2050 Cooking pot carinated shoulder L.101 QUM 169 KHQ 2342 Cooking pot large L.130 QUM 170 KHQ 365 Pseudo Nabatean base QUM 171 KHQ 2611 Pseudo Nabatean base QUM 172 KHQ 501 Pseudo Nabatean dish L.28 QUM 173 Ein Feshka 203 Pseudo Nabatean base QUM 174 KHQ 891 Small bowl red slip buff circ. On red slip QUM 175 KHQ Scriptorium table large mortar piece QUM 176 KHQ Scriptorium table small mortar piece QUM 177 KHQ Scriptorium yellow inner clay mould of QUM 175 QUM 178 KHQ Scriptorium grey clay mold of QUM 175 QUM 179 KHQ 2576 Incurved low dish L.28 QUM 180 KHQ 2577 Incurved low dish L.28 QUM 181 KHQ Bitumenous rock from Qumran quarry QUM 182 KHQ 2463 Lid paint + brown paint L.100 fill QUM 183 KHQ 2091 Jar for 182 painted+pierced holes L.115 QUM 184 KHQ 2507 Small jar 25cm round base carinated shoulder QUM 185 KHQ 2596-1 Small juglet(Afarsimon) buff L.114 deposit QUM 186 GQ8:11 Highest scroll jar QUM 187 KHQ 2548 Small scroll jar QUM 188 KHQ 2591-2Deep small bowl L.114 of JB QUM 189 KHQ 2600-2 Deep small bowl L.114 of JB QUM 190 KHQ 1620 Carinated dish as NABPF no paint L.40 QUM 191 KHQ 1621 Carinated dish as NABPF no paint L.40 QUM 192 KHQ 2595 High pinch rim dish L.114 JB QUM 193 Ein Feshka 15 Inkwell QUM 194 KHQ2093 „Herodian” lamp with two crc on nozzle L.115 QUM 195 KHQ 2265 Cooking pot red upstanding rim

92

Samples

QUM 196 KHQ 954 Cooking pot dark gray everted rim QUM 197 KHQ Waster of high handleless krater QUM 198 KHQ Cave 1 5582 Scroll jar (Roitman) rounded QUM 199 KHQ Cave 1 5584 Scroll jar (Roitman) long, narrow QUM 200 KHQ 192 Jug engraved TA* KW QUM 201 KHQ 2416 Jug QUM 202 KHQ 2417 Jug jamzadoza QUM 203 KHQ 979 L.54 QUM 204 KHQ 1110 Bowl, aleph painted in red inside bowl QUM 205 KHQ 1650 carved before firing QUM 206 KHQ 2609 MTMPP QUM 207 KHQ 635 sherd with greek „OG” QUM 208 Cave 7 Q1 painted „S” QUM 209 KHQ 2575 carved cross, even length QUM 210 KHQ 2108 store jar PNWWM QUM 211 Feshka 255a Greek carved letters QUM 212 KHQ 2507 Small holemouth jar QUM 213 KHQ 2587 Small hemispherical bowl, black paint QUM 214 KHQ 680 Jug QUM 215 KHQ provenance unknown Tah QUM 216 KHQ 681 Jug as 214 „chi-nun-quf” QUM 217 KHQ 682 Jug as 214 L.34 engraved QUM 218 KHQ 387 Jug as 214 engraved „TWN” QUM 219 KHQ Sherdwith painted letter L.111 QUM 220 KHQ 3759 Handle with 4 parallel lines incarved L.4 QUM 221 KHQ 4638 Inkwell bottom QUM 222 KHQ 4638 Inkwell ink-scraping QUM 223 KHQ 2989 Scraping from jar L.41 east, oil, bitumen, ink QUM 224 KHQ Terra 26 Jericho painted pseudo-nabatean QUM 225 KHQ Qumran puddle fored made into inkwell QUM 226 KHQ Fired Dead Sea mud made into an inkwell QUM 227 KHQ Terra 45? Jericho painted pseudo nabatean QUM 228 Hebron 1 Ummar 25 Landgraf QUM 229 Hebron 2 Ummar 26 Landgraf QUM 230 KHQ 1465 Scraping from inside small storage jar QUM 231 Cave 6 39:7 Scroll jar QUM 232 Cave 4 Q3 (length 30.8) QUM 233 Cave X:2 Storage jar, hor. Comb band, dripping, purple color QUM 234 Cave X:2 Jar of 223 itself QUM 235 Cave X:2 Jar (234-dripping outs. as cement) QUM 236 KHQ 908 Ovoid jar scraping, fine wash ourside L.45c QUM 237 KHQ 908 Ovoid jar itself with two handles L.45c QUM 238 KHQ 758 Scroll jar L.13 QUM 239 KHQ 2494 Ovoid jar L.61 QUM 240 Cave IX Scroll jar (green dot) 6b QUM 241 Cave 7:Q5 Ovoid as Roma jar 12b QUM 242 KHQ 1404 Ovoid shaped jar two vert. handles L.61 QUM 243 KHQ 2649 Ovoid shaped jar two vert. handles L.133 QUM 244 KHQ 2657 Ovoid shaped jar with 2 handles L.114 QUM 245 Cave 29:3 Scroll jar

93

Samples

QUM 246 Cave 7-1 Lid scroll jar, red ware 1 QUM 247 Cave 12-5 Lid scroll jar, grey ware QUM 248 Cave 3-5 Lid scroll jar QUM 249 Cave 8-15 Lid scroll jar grey ware QUM 250 Cave 28-1 Scroll jar with blisters QUM 251 KHQ 1239 Store jar QUM 252 KHQ 1601 Small deep hemisph. bowl L.89 QUM 253 KHQ 1601 Small deep hemisph. bowl L.89 QUM 254 KHQ 2563 Afaesimon Juglet QUM 255 Cave 29-24 Scroll jar in 6a QUM 256 Cave 3-1 Scroll jar in 6c QUM 257 KHQ 42 Scroll jar 4 small vert. handles L.2 QUM 258 KHQ 1587 Cup 11a L.89 QUM 259 KHQ 1587 Cup 11b L.89 QUM 260 KHQ 1587 Cup 11c L.89 QUM 261 KHQ 1591 Dish 10a L.89 QUM 262 KHQ 16 Sharp carinated dish flat base L.1 QUM 263 KHQ 795 Sharp carinated dish flat base L.45 QUM 264 Cave 8 Q8 Hemispherical bowl stringcut base QUM 265 KHQ 1627 Outflaring jar without handles L.91 QUM 266 KHQ 1237 Lagynos QUM 267 Cave 001 Jar with two loop handles QUM 268 KHQ 917 Store jar with 4 piercing L.44 QUM 269 KHQ Q4 Small platter stringcut base L.1 QUM 270 Cave 31-3 Small hemisph. bowl QUM 271 Cave 1 Q1 Hemisph. bowl QUM 272 KHQ 1270 Large cup, ringbase L.65 QUM 273 KHQ 216 Small cup, stringcut L.8 QUM 274 KHQ 1050 Large cup, ringbase L.59 QUM 275 KHQ 179 Platter(very flat) QUM 276 KHQ 1452 Funnel&soot&clean piece L.86 QUM 277 Cave 8 Q11 Lid, sharp carination QUM 278 Cave 3 Lid (had before) QUM 279 KHQ 3000 Lid rounded with purple dye QUM 280 KHQ 3000 Scraping of purple. Mercury? QUM 281 KHQ 582 Long pipe QUM 282 Jericho bowl 28 QUM 283 Jericho bowl 29 QUM 284 Large storage jar QUM 285 Bituminous limestone QUM 286 KHQ Q43 Oil lamp Cave 1 QUM 287 KHQ 10151 Hellenistic lamp L.44 QUM 288 KHQ 1009 Bowl QUM 289 KHQ 5084 Lamp L.62 QUM 290 KHQ 5085 Lamp L.66 QUM 291 KHQ 2206 Hellenistic lamp L.130 QUM 292 KHQ 5087 Lamp L.130 QUM 293 KHQ 2093 Herodian lamp QUM 294 KHQ q2541 Herodian lamp QUM 295 Ez-Zara L.043/682 balsam juglet

94

Samples

QUM 296 Ez-zara L. 206/96 balsam juglet QUM 297 Ez-Zara L. 114/104 balsam juglet QUM 298 Ez-Zara L.329/435 balsam juglet QUM 299 Ez-Zara L. 336/483 cream ware bowl (white ware) QUM 300 Ez-Zara L. 202/24 cream ware bowl (white ware) QUM 301 KHQ Scraping inside pipe L.51 QUM 302 KHQ Pipe itself L.51 QUM 303 KHQ 935 Jar with shin inscribed before firing QUM 304 Cave 6Q1 Ovoid jar with inscription in ink QUM 305 No.11 Pipe cistern 110 (dark grey soil) QUM 306 No. 11 Pipe deposit at inside of round cistern 110 QUM 307 KHQ 2419 Funnel vessel, white ware QUM 308 KHQ 461 Grafitto QUM 309 KHQ 711 Grafitto QUM 310 KHQ 1236 Grafitto QUM 311 KHQ 2556 Grafitto QUM 312 KHQ 386 Grafitto QUM 313 KHQ 425 Grafitto QUM 314 KHQ Grafitto QUM 315 KHQ 2176 Grafitto QUM 316 KHQ 426 Grafitto QUM 317 KHQ 734 Grafitto QUM 318 KHQ 2554 Grafitto QUM 319 KHQ 1313 Grafitto QUM 320 KHQ 2109 Grafitto QUM 321 KHQ 2125 Grafitto QUM 322 Roof tile, Legio X Fretensis QUM 323 Curved roof tile QUM 324 Aquaba city kiln waster QUM 325 Other sample of QUM 324

95

List of figures

List of figures FIGURE 1:CILYNDRICAL SCROLL JAR WITH LID (DAVIES 2002)............................................................. 4 FIGURE 2 : HORIZONTAL CROSS SECTION OF THE CORE OF THE NUCLEAR REACTOR AT THE

INSTITUTE OF NUCLEAR TECHNIQES................................................................................................ 30 FIGURE 3 PARZEN-ROSENBLATT DENSITY FUNCTION IN PRINCIPAL COMPONENT SUBSPACE . 42FIGURE 4 QUMRAN SETTLEMENT................................................................................................................ 44 FIGURE 5 ARCHAEOLOGICAL SITES AROUND THE DEAD SEA (BEIT-ARIEH 1997).......................... 45 FIGURE 6 CAVE 1 (DAVIES 2002) ................................................................................................................... 46 FIGURE 7 PLAN OF THE KHIRBET QUMRAN (GUNNEWEG 2003)........................................................... 47 FIGURE 8 THE “CROCKERY” AT L.89. (MAGNESS 2002) ........................................................................... 48 FIGURE 9 CAVE 4. ............................................................................................................................................. 49 FIGURE 10 SROLL JARS AT QUMRAN EXHIBITION .................................................................................. 55 FIGURE 11 MAP OF THE SITES (GUNNEWEG 2003).................................................................................... 57 FIGURE 12 CHEMICAL GROUPS OF QUMRAN POTTERY SAMPLES ...................................................... 60 FIGURE 13 DISHES IN LOCUS 114 (MAGNESS 2002)................................................................................... 66 FIGURE 14 THE ROMA JAR QUM 134 (LEMAIRE 2003) .............................................................................. 67 FIGURE 15 THE “ROMA INSRIPTION” (LEMAIRE 2003)............................................................................. 67 FIGURE 16 THE EDOMJUG QUM 201 LEMAIRE 2003................................................................................. 68

96

Elemental data

Elemental data QUMRAN SAMPLES Concentrations in ppm

100 101 102 103 104 105 106 107

As 9.4±0.2 12.6±0.3 9.6±0.3 7.9±0.3 11.1±0.22 5.9±0.2 7.6±0.3 9.3±0.4 Ba 285±26 246±37 460±46 307±43 233±30 284±48 Br 15±0.2 16±1 34±0.4 27±1 17±0.3 7.1±0.2 8.5±0.3 11.4±0.3 Ce 49.6±1.0 45.8±0.9 79.3±1.6 40.2±1.2 47.6±1.0 62.3±2.0 61.5±1.2 71.0±2.0 Co 11.2±0.2 11.5±0.4 13.5±0.4 9.3±0.4 10.9±0.3 12.8±0.4 10.6±0.6 14.9±0.5 Cs 2.55±0.13 0.6±0.09 2.0±0.2 3.87±0.27 4.26±0.3 3.61±0.3 Cr 88.9±1.8 164±3 157±3 133±3 190±4 111±2 121±4 163±3 Eu 0.92±0.06 0.89±0.07 1.82±0.1 0.89±0.1 1.0±0.1 1.4±0.1 1.49±0.1 1.56±0.11

Fe% 2.59±0.03 2.68±0.05 4.87±0.05 2.03±0.04 2.84±0.03 3.74±0.04 4.32±0.04 4.76±0.05Hf 4.2±0.1 4.1±0.2 7.5±0.2 3.9±0.2 4.06±0.16 5.02±0.2 5.2±0.3 7.24±0.3

K% 0.86±0.1 1.03±0.1 1.98±0.1 1.11±0.1 0.72±0.06 2.10±0.10 2.4±0.12 2.08±0.15La 23.2±0.1 22±1 37.7±0.4 20.8±0.2 24.6±0.3 25.6±0.3 28.0±0.3 32.5±0.3 Lu 0.23±0.01 0.27±0.01 0.39±0.02 0.27±0.01 0.31±0.01 0.34±0.01 0.35±0.01 0.39±0.01Mo

Na% 0,299±0.001 0,062±0.001 0,999±0.001 0,462±0.001 0.47±0.01 0.476±0.01 0.46±0.01 0.76±0.01Nd 18±4 21±3 24±4 12±3 21±4 Rb 36.9±4.1 50.7±7.1 86.0±7.0 91±9 63±10 Sb 1.38±0.03 1.11±0.04 0.7±0.05 0.91±0.05 1.29±0.04 0.35±0.03 0.54±0.04 0.74±0.05Sc 8.4±0.1 8.7±0.1 14.6±0.2 6.60±0.1 8.63±0.1 16.3±0.1 16.5±0.1 14.9±0.2 Se 4.4±0.9 6.1±1.4 3.95±0.8 2.8±1 2.54±0.8 6.4±1.3 Sm 4.96±0.1 4.97±0.1 8.03±0.1 4.33±0.1 5.39±0.1 6.43±0.1 6.78±0.1 6.67±0.07Ta 0.72±0.1 0.71±0.09 1.33±0.12 0.61±0.09 1.0±0.1 1.13±0.14Tb 0.78±0.1 0.91±0.1 0.93±0.16 0.7±0.1 0.57±0.12 1.06±0.20Th 5.55±0.11 5.03±0.2 8.9±0.3 5.5±0.2 5.85±0.18 8.2±0.2 8.26±0.25 8.83±0.26U 6.9±0.1 11.3±0.2 3.1±0.2 9.9±0.3 11.8±0.2 3.7±0.2 3.61±0.22 3.92±0.27

Yb 1.696±0.05 1.91±0.04 2.89±0.09 1.85±0.09 1.98±0.06 2.41±0.1 2.5±0.1 2.83±0.06Zn 90±5 250±8 177±9 169±8 300±10 75±6 108±8 142±8

97

Elemental data

QUMRAN SAMPLES Concentrations in ppm

108 109 110 111 112 113 114 115

As 7.9±0.3 10.1±0.3 9.3±0.4 9.4±0.3 5.8±0.4 9.4±0.4 7.8±0.4 5.6±0.2 Ba 1170±120 230±32 357±36 271±30 300±30 256±36 Br 9.7±0.3 10.2±0.3 17.2±0.3 7.7±0.2 33.2±0.3 21±1 14.6±0.5 15.5±0.2 Ce 64.4±1.3 75.0±1.5 71.1±1.4 74.5±1.5 57.3±1.2 75.7±0.8 68.5±1.4 57.8±1.2 Co 10.2±0.3 15.0±0.3 14.8±0.4 15.4±0.3 10.4±0.4 15.1±0.3 13.6±0.3 17.3±0.4 Cs 3.6±0.3 3.72±0.26 3.28±0.26 4.12±0.25 4.81±0.2 3.98±0.24 1.86±0.13 6.7±0.3 Cr 112±2 158±3 153±3 168±4 99.0±2.0 153±3 146±3 97.0±3.0 Eu 1.36±0.1 1.47±0.07 1.77±0.10 1.76±0.07 1.40±0.07 1.64±0.08 1.58±0.05 1.34±0.10

Fe% 4.13±0.04 5.13±0.05 4.92±0.05 5.19±0.05 3.87±0.04 5.10±0.05 4.63±0.05 4.22±0.04Hf 4.87±0.19 6.34±0.19 6.12±0.24 6.0±0.2 4.76±0.19 5.36±0.16 6.64±0.13 3.95±0.28

K% 2.25±0.11 2.29±0.14 2.20±0.15 2.06±0.12 2.51±0.18 1.98±0.14 2.24±0.2 3.54±0.11La 28.2±0.2 36.3±0.3 36.0±0.2 37.7±0.3 26.6±0.2 35.9±0.3 33.2±0.3 26.9±0.3 Lu 0.35±0.01 0.4±0.02 0.35±0.03 0.41±0.02 0.34±0.02 0.41±0.02 0.35±0.02 0.29±0.01Mo 3.3±0.7

Na% 0.54±0.01 0.83±0.01 0.71±0.01 0.57±0.01 0.86±0.01 0.55±0.01 1.19±0.01 0.42±0.01Nd 24±4 27±4 25±4 34±5 18±3 28±4 23±3 16±2 Rb 80±7 66±7 71±9 77±8 78±7 79±7 49±7 116±8 Sb 0.52±0.1 0.57±0.04 0.63±0.04 0.89±0.13 0.42±0.04 0.62±0.04 0.72±0.05 0.52±0.03Sc 16.2±0.1 17.1±0.1 16.5±0.1 17.4±0.1 15.9±0.1 16.6±0.1 14.4±0.1 16.7±0.1 Se 3.2±0.9 2.2±1 2.1±0.6 3.9±1.1 Sm 6.82±0.1 7.77±0.1 7.85±0.1 8.12±0.1 6.56±0.1 7.98±0.1 7.30±0.1 5.59±0.1 Ta 0.76±0.08 1.28±0.10 1.0±0.1 1.08±0.10 0.64±0.10 1.24±0.10 1.14±0.07 0.77±0.09Tb 0.87±0.12 0.94±0.14 0.99±0.14 0.97±0.13 0.85±0.12 0.75±0.13 0.99±0.09 0.92±0.16Th 8.10±0.16 9.42±0.19 8.65±0.26 8.93±0.09 7.16±0.21 8.88±0.18 8.06±0.16 7.56±0.23U 3.17±0.19 4.04±0.2 3.68±0.22 4.39±0.22 3.33±0.2 3.89±0.19 3.69±0.26 2.94±0.21

Yb 2.49±0.07 2.79±0.03 3.08±0.03 3.25±0.06 2.52±0.08 2.96±0.06 2.67±0.05 1.99±0.08Zn 106±10 133±8 141±6 165±5 76±8 161±8 129±6 68±8

98

Elemental data


116 117 118 119 120 121 122 123

As 5.8±0.2 8.1±0.2 7.2±0.2 14.8±0.2 7.2±0.4 7.6±0.2 5.97±0.24 5.9±0.2 Ba Br 12.7±0.3 17.3±0.2 9.2±0.2 9.05±0.18 16±5 14.8±0.2 4.45±0.22 6.5±0.2 Ce 58.3±1.2 65.1±0.7 60.2±1.2 52.5±1.0 53.3±1.6 68.5±1.4 55.9±1.7 56.8±1.1 Co 18.5±0.4 17.1±0.3 18.8±0.4 17.8±0.4 14.4±0.6 13.6±0.4 19.7±0.4 18.1±0.4 Cs 6.15±0.31 2.94±0.23 4.92±0.25 4.49±0.22 3.13±0.41 3.95±0.28 6.30±0.31 6.26±0.31Cr 108±3 107±2 110±2 120±2 88±4 119±4 102±3 104±3 Eu 1.15±0.07 1.37±0.07 1.22±0.07 1.32±0.07 1.18±0.13 1.64±0.10 1.17±0.08 1.18±0.08

Fe% 4.42±0.04 4.48±0.05 4.57±0.05 4.37±0.04 4.18±0.08 4.46±0.05 4.47±0.05 4.40±0.04Hf 4.63±0.23 5.02±0.2 4.02±0.2 4.54±0.18 4.35±0.39 6.24±0.31 4.15±0.25 4.26±0.26

K% 3.38±0.10 3.19±0.1 3.77±0.11 2.34±0.1 1.40±0.15 2.51±0.15 3.70±0.18 3.47±0.17La 27.0±0.22 28.1±0.2 25.1±0.2 22.6±0.2 26.7±4 28.2±0.3 27.1±0.3 26.9±0.3 Lu 0.32±0.01 0.34±0.01 0.33±0.01 0.33±0.01 0.27±0.03 0.34±0.01 0.32±0.02 0.30±0.01Mo 3.8±1.0 7.6±0.9 4.8±0.9 4.8±1.2 3±1 6.6±1.1 4.1±0.9 1.6±0.5

Na% 0.96±0.01 0.80±0.01 0.69±0.01 1.08±0.01 0.66±0.01 0.66±0.01 0.52±0.01 0.41±0.01Nd 13±2 12±3 16±4 14±3 18±5 18±5 18±5 Rb 120±10 72±8 104±8 69±8 65±8 95±10 112±10 Sb 0.5±0.03 0.59±0.03 0.56±0.03 0.67±0.03 0.39±0.05 0.7±0.03 0.56±0.04 0.50±0.03Sc 17.6±0.1 16.0±0.1 18.1±0.1 18.3±0.1 16.8±0.1 16.9±0.2 17.9±0.1 17.6±0.2 Se Sm 5.51±0.1 6.13±0.1 5.48±0.1 5.36±0.1 5.43±0.1 6.56±0.1 5.43±0.1 5.22±0.1 Ta 1.46±0.12 1.78±0.11 0.98±0.10 0.81±0.10 0.86±0.11 0.94±0.11 0.86±0.09Tb 1.17±0.14 0.83±0.16 0.87±0.14 0.97±0.16 Th 7.29±0.22 7.58±0.23 8.07±0.24 6.36±0.19 6.86±0.34 7.46±0.22 7.61±0.23 7.18±0.22U 2.19±0.2 4.18±0.21 3.26±0.2 2.13±0.15 2.32±0.35 3.76±0.26 3.04±0.24 2.51±0.23

Yb 2.25±0.14 2.54±0.08 2.19±0.11 2.24±0.07 2.12±0.11 2.71±0.08 2.30±0.05 2.27±0.09Zn 108±11 123±14 87±10 113±14 98±13 120±17 72±10

99

Elemental data


124 125 126 127 128 129 130 131

As 5.7±0.3 5.87±0.23 10.3±0.3 7.6±0.4 2.5±0.3 8.5±0.4 4.4±0.4 7.6±0.2 Ba 232±30 Br 12.8±0.3 5.6±0.2 19.2±0.2 13.1±0.3 36.2±0.4 41.8±0.4 51.2±0.5 24±0.2 Ce 58.5±1.2 56.0±1.1 57.8±1.2 61.3±1.2 45.2±1.4 46.1±1.4 57.4±1.7 51±1 Co 19.8±0.4 17.7±0.7 13.4±0.4 12.5±0.4 10.4±0.3 9.20±0.37 11.2±0.5 14.2±0.3 Cs 6.08±0.3 5.80±0.29 2.46±0.25 4.31±0.3 0.53±0.15 1.36±0.2 4.74±0.3 4.04±0.2 Cr 103±3 99±3 105±3 121±4 110±3 208±4 105±4 100±2 Eu 1.29±0.08 1.14±0.07 1.18±0.08 1.31±0.08 0.90±0.07 1.01±0.1 1.16±0.10 1.10±0.07

Fe% 4.25±0.04 4.17±0.04 4.91±0.05 4.20±0.04 1.98±0.04 2.58±0.05 4.05±0.08 3.55±0.04Hf 4.77±0.24 4.17±0.25 5.03±0.25 5.75±0.3 7.49±0.22 6.34±0.25 4.50±0.3 4.8±0.2

K% 3.27±0.16 3.07±0.18 2.95±0.21 2.88±0.23 1.29±0.22 1.99±0.08La 26.3±0.3 25.7±0.3 22.2±0.2 26.03±0.3 21.8±0.2 24.2±0.2 26.7±0.3 21.8±0.2 Lu 0.28±0.02 0.27±0.01 0.33±0.01 0.35±0.01 0.28±0.01 0.30±0.02 0.34±0.01 0.25±0.01Mo 3.4±0.9 4.8±1.2 9.7±1.2 6.6±1.2 7.7±1.3 21±1 7.8±1.2 6±1

Na% 0.37±0.01 0.42±0.01 1.85±0.01 0.81±0.01 1.06±0.01 0.84±0.01 0.89±0.01 0.63±0.01Nd 17±2 15.7±4.4 20±2 16±4 13±8 19±3 21±5 15±2 Rb 116±9 93±9 74±10 72±9 65±6 Sb 0.41±0.03 0.44±0.03 0.52±0.04 0.57±0.04 0.39±0.03 0.95±0.05 0.42±0.04 0.4±0.04 Sc 17.2±0.1 17.1±0.2 16.8±0.1 17.5±0.2 7.1±0.1 8.6±0.1 16.8±0.2 14.8±0.1 Se Sm 5.13±0.1 4.94±0.1 6.05±0.1 6.04±0.1 4.37±0.1 4.91±0.1 5.93±0.1 4.95±0.1 Ta 0.72±0.08 0.86±0.10 0.88±0.10 0.92±0.10 0.75±0.10 0.62±0.10 0.65±0.08Tb 0.79±0.17 0.99±0.17 1.0±0.2 0.86±0.18Th 7.44±0.22 6.87±0.20 7.35±0.22 8.10±0.2 4.88±0.20 4.99±0.20 7.06±0.3 7.3±0.2 U 2.13±0.06 3.1±0.1 3.46±0.24 3.65±0.29 5.83±0.23 10.6±0.3 3.08±0.34 3.0±0.2

Yb 2.12±0.15 2.15±0.09 2.69±0.08 2.44±0.05 1.89±0.04 2.09±0.1 2.28±0.09 1.72±0.05Zn 45±7 58±9 176±12 90±9 100±7 235±9 60±10 97±6

100

Elemental data


132 133 134 135 136 137 138 139

As 6.9±0.3 8.2±0.3 6.3±0.3 7.5±0.2 6.4±0.2 5.9±0.2 6.2±0.3 5.7±0.3 Ba 116±25 265±40 Br 18±1 25±1 16±0.5 22±1 6±0.5 22±1 16±0.3 80±2

Ca% 6.00±1.5 4.60±1.0 9.09±1.5 1.82±0.5 6.25±1.5 4.89±1.0 4.29±1.0 7.52±1.5 Ce 55±2 57±2 49±2 56±2 61±1 64±1 61±1 61±2 Co 9.9±0.3 13.3±0.3 11.1±0.3 10.8±0.2 10.8±0.2 20.0±0.4 17.9±0.4 12.0±0.2 Cs 4.4±0.2 3.8±0.2 5.2±0.3 4.2±0.2 5.06±0.15 6.4±0.3 6.9±0.2 3.0±0.2 Cr 114±2 123±2 108±2 112±2 115±2 115±5 111±2 98±2 Eu 1.26±0.06 1.20±0.07 1.02±0.07 1.29±0.05 1.40±0.06 1.55±0.08 1.22±0.06 1.49±0.06

Fe% 4.12±0.04 4.31±0.04 3.79±0.04 3.94±0.04 4.26±0.03 4.62±0.04 4.52±0.04 3.91±0.04Hf 4.80±0.14 6.56±0.20 3.8±0.5 4.77±0.14 5.34±0.16 4.40±0.20 4.80±0.1 6.02±0.18

K% 2.21±0.09 2.34±0.09 2.09±0.10 2.50±0.10 2.16±0.06 4.09±0.16 3.73±0.15 2.37±0.14La 25.0±0.5 24.2±0.4 22.3±0.2 24.7±0.3 26.7±0.3 29.0±0.4 27.2±0.3 27.3±0.2 Lu 0.31±0.01 0.33±0.01 0.28±0.01 0.32±0.01 0.34±0.01 0.30±0.01 0.31±0.01 0.33±0.01Mo 7±1 8±1 7±1 5±1 4±1 5±1 5±1 6±1

Na% 0.65±0.01 1.06±0.01 0.41±0.01 0.50±0.01 0.37±0.01 1.13±0.01 0.76±0.01 1.00±0.01Nd 22±3 20±3 16±4 19±3 19±3 24±6 19±4 21±3 Rb 75±7 77±7 85±7 70±6 79±5 108±8 118±7 68±6 Sb 0.7±0.05 0.4±0.05 0.5±0.05 0.5±0.03 0.4±0.03 0.5±0.05 0.4±0.1 0.5±0.04 Sc 16.6±0.1 16.1±0.1 15.4±0.1 15.8±0.1 17.8±0.1 18.2±0.1 18.1±0.05 16.2±0.1 Se Sm 6.02±0.06 5.94±0.12 5.07±0.10 6.03±0.06 6.57±0.13 6.36±0.13 5.88±0.12 6.58±0.13Ta 0.60±0.07 0.86±0.09 0.78±0.09 0.67±0.06 0.80±0.06 0.90±0.09 0.84±0.08Tb 0.73±0.13 0.61±0.12 0.95±0.11 1.06±0.10 0.84±0.13 0.91±0.10Th 7.9±0.2 7.9±0.2 6.9±0.2 7.2±0.1 8.2±0.2 8.1±0.2 8.3±0.2 7.6±0.2 U 3.3±0.2 3.6±0.3 3.6±0.2 3.1±0.2 3.0±0.2 2.6±0.2 3.7±0.2 3.4±0.1

Yb 2.36±0.05 2.03±0.08 1.93±0.06 2.23±0.04 2.43±0.02 2.09±0.08 2.06±0.06 2.49±0.07Zn 102±7 117±8 95±8 160±10 97±8 96±8 90±6 80±8

101

Elemental data


140 141 142 143 144 145 146 147

As 13±1 4.1±0.3 7.0±0.1 4.1±0.2 6.0±0.2 5.6±0.5 4.9±0.2 2.4±0.1 Ba 280±20 660±30 100±18 Br 16±1 84±2 48±1 82±1 36±1 40±1 39±1 40±0.5

Ca% 21±5 12.5±2 37.9±5.0 30.2±5.0 14.3±3.0 26.8±3.0 39.7±5.0 Ce 97±2 32±2 65±2 12.7±0.3 27.5±0.8 76.9±1.5 26.1±0.5 12.3±0.3 Co 26.8±0.3 7.4±0.3 12.8±0.4 2.01±0.08 5.35±0.27 16.2±0.5 5.42±0.11 2.19±0.09 Cs 2.16±0.11 2.5±0.3 2.56±0.23 1.87±0.28 0.8±0.07 0.2±0.03 Cr 115±2 115±2 140±3 163±2 130±3 167±3 115±2 141±1 Eu 1.62±0.03 0.84±0.07 1.30±0.08 0.34±0.02 0.54±0.06 1.33±0.09 0.62±0.03 0.37±0.03

Fe% 6.13±0.02 1.89±0.04 3.89±0.04 0.41±0.01 2.03±0.04 4.47±0.05 1.49±0.01 0.37±0.04 Hf 12.6±0.1 4.64±0.19 8.18±0.25 0.47±0.05 1.88±0.17 8.81±0.26 3.4±0.1 8.9±0.2

K% 0.92±0.04 1.09±0.09 2.07±0.15 0.25±0.03 1.47±0.12 1.51±0.17 0.59±0..05 0.29±0.045La 41.2±0.2 17.0±0.2 32.7±0.3 9.4±0.1 14.8±0.2 37.1±0.4 14.7±0 9.6±0.1 Lu 0.44±0.01 0.37±0.01 0.15±0.01 0.17±0.02 0.43±0.02 0.19±0.01 0.17±0.01 Mo 67±2 14±1 19±1 15±2 18±2 13±1 17±2

Na% 0.56±0.01 1.05±0.01 1.35±0.01 0.30±0.02 0.40±0.02 1.62±0.01 0.35±0.01 0.248±0.10Nd Rb 45±4 58±8 50±6 48±8 16±3 Sb 0.78±0.08 0.47±0.05 0.8±0.06 0.72±0.03 0.6±0.02 0.7±0.1 0.48±0.02 Sc 15.0±0.1 6.12±0.06 13.3±0.13 2.42±0.03 8.01±0.08 13.27±0.13 4.83±0.02 2.39±0.02 Se 4.0±0.6 3.8±0.4 3±1 Sm 8.26±0.17 3.48±0.10 6.66±0.13 1.87±0.09 2.60±0.08 7.34±0.22 3.06±0.09 2.03±0.1 Ta 1.7±0.05 0.52±0.08 0.97±0.11 1.06±0.13 0.37±0.04 Tb 1.12±0.07 0.44±0.10 1.07±0.15 0.20±0.03 0.99±0.16 0.39±0.05 0.23±0.08 Th 10.8±0.2 3.75±0.15 7.30±0.22 0.91±0.04 4.3±0.2 8.3±0.3 3.10±0.1 0.81±0.05 U 4.1±0.1 4.8±0.2 4.6±0.3 11.8±0.2 2.89±0.26 4.6±0.4 7.5±0.08 12.9±0.1

Yb 3.15±0.03 1.43±0.10 2.62±0.1 0.97±0.04 1.0±0.1 3.37±0.13 1.31±0.04 1.08±0.04 Zn 110±7 143±9 149±9 207±5 121±8 150±7 134±8

102

Elemental data


148 149 150 151 152 153 154 155

As 7.2±0.3 5.4±0.5 8.6±0.8 7.6±0.5 14±1 6.5±0.4 5.9±0.5 8.5±0.3 Ba 360±30 310±30 Br 43±1 22±1 34±1 65±2 36±2 25±1 29±1 44±1

Ca% 10.02±2.0 12.9±2.0 11.2±1.5 9.6±2.0 10.7±2.0 3.72±1.0 8.23±1.5 3.85±1.0 Ce 64±2 66±1 65±1 56±2 53±2 60±2 54±2 90±2 Co 16.6±0.3 13.3±0.1 11.2±0.5 11.6±0.4 12.7±0.4 18.0±0.4 11.9±0.4 16.0±0.3 Cs 2.0±0.2 1.94±0.16 4.0±0.3 2.9±0.2 3.1±0.3 7.2±0.2 4.7±0.3 4.1±0.2 Cr 125±3 126±3 142±4 109±2 123±3 113±3 111±2 97±2 Eu 1.32±0.05 1.30±0.06 1.97±0.14 1.31±0.08 1.22±0.07 1.35±0.07 1.21±0.08 1.10±0.04

Fe% 3.87±0.04 3.37±0.04 3.81±0.08 3.51±0.04 4.15±0.04 4.58±0.04 4.24±0.04 4.77±0.05Hf 9.22±0.18 10.9±0.2 5.19±0.30 4.23±0.21 4.19±0.21 4.91±0.15 4.37±0.22 8.65±0.17

K% 1.60±0.12 1.24±0.14 2.60±0.01 2.62±0.18 2.98±0.21 3.90±0.23 1.97±0.28 1.26±0.14La 30.0±0.2 30.0±0.3 30.8±0.6 24.4±0.2 24.4±0.2 28.1±0.3 25.0±0.3 40.7±0.4 Lu 0.35±0.02 0.39±0.02 0.42±0.02 0.30±0.02 0.32±0.017 0.33±0.01 0.29±0.01 0.39±0.01Mo 12±1 10±1 21±2 10±2 11±2 5±1 4±1 5±1

Na% 0.84±0.04 0.56±0.01 2.17±0.02 0.76±0.01 0.41±0.01 0.64±0.05 0.45±0.01 0.25±0.01Nd 36±5 20±2 22±2 27±2 Rb 40±5 41±6 53±6 54±8 120±10 82±9 58±5 Sb 0.6±0.04 0.6±0.04 0.8±0.1 0.45±0.05 0.75±0.06 0.4±0.04 0.4±0.05 0.5±0.05 Sc 11.2±0.1 10.1±0.1 16.4±0.2 14.4±0.1 15.5±0.2 18.3±0.1 15.9±0.2 12.8±0.1 Se Sm 6.38±0.13 6.45±0.13 8.06±0.16 6.18±0.19 5.91±0.12 6.14±0.12 5.70±0.11 6.83±0.14Ta 1.23±0.07 1.14±0.22 0.59±0.09 0.72±0.10 1.02±0.08 0.82±0.10 Tb 0.87±0.12 1.04±0.11 0.86±0.13 1.02±0.16 0.70±0.11 1.04±0.17 0.69±0.09Th 7.2±0.1 8.5±0.1 7.5±0.3 6.7±0.2 7.3±0.2 8.7±0.2 7.4±0.2 12.2±0.2 U 3.8±0.2 4.2±0.2 4.0±0.5 4.7±0.2 3.8±0.3 3.9±0.2 2.7±0.3 3.6±0.2

Yb 2.56±0.08 2.72±0.08 2.85±0.14 2.25±0.09 2.16±0.06 2.19±0.07 2.08±0.08 2.97±0.06Zn 120±6 100±5 130±10 103±6 92±8 98±8 85±7 160±10

103

Elemental data


156 157 158 159 160 161 162 163

As 4.9±0.2 7.5±0.5 6.2±0.3 6.4±0.3 9.0±0.4 7.2±0.3 5.5±0.3 6.7±0.3 Ba 470±40 250±40 200±40 Br 16±1 30±0.3 40±0.4 17±0.4 62±1 26±0.3 21±0.4 100±1

Ca% 6.57±1.5 28.16±2.0 4.74±1.5 4.61±1.0 9.87±1.5 6.77±1.5 7.62±1.5 9.94±1.5 Ce 51.4±1.0 36.4±0.7 50.3±1.0 54.4±1.1 58.7±1.2 55.8±1.1 51.0±1.0 54.0±1.1 Co 10.5±0.2 9.7±0.3 17.5±0.4 17.4±0.4 19.0±0.4 10.8±0.3 10.5±0.2 12.2±0.2 Cs 4.0±0.2 1.9±0.2 5.5±0.3 6.0±0.2 3.9±0.3 4.35±0.22 2.9±0.2 3.9±0.2 Cr 92±2 80±2 141±3 108±2 114±2 108±2 115±2 100±2 Eu 1.03±0.04 0.84±0.06 1.16±0.07 1.17±0.06 1.26±0.06 1.24±0.06 1.20±0.06 1.22±0.06

Fe% 3.68±0.04 3.27±0.04 4.51±0.05 4.25±0.03 4.07±0.04 3.65±0.04 3.72±0.04 4.35±0.04Hf 4.08±0.12 2.49±0.15 4.44±0.18 4.08±0.16 5.2±0.2 5.05±0.15 5.3±0.2 4.38±0.18

K% 1.94±0.06 1.27±0.04 2.91±0.09 3.75±0.11 2.88±0.12 2.32±0.02 2.56±0.13 2.23±0.13La 24.5±0.3 17.6±0.2 22.1±0.2 26.5±0.3 28.4±0.3 26.0±0.3 24.7±0.3 25.4±0.3 Lu 0.29±0.01 0.21±0.01 0.29±0.01 0.32±0.01 0.33±0.01 0.31±0.01 0.27±0.01 0.31±0.01Mo 2.5±0.6 3.8±0.6 5.0±0.8 5.1±0.8 9.5±1.0 6.0±0.5 4.7±0.8 4.4±0.9

Na% 0.24±0.01 0.83±0.01 1.12±0.01 1.07±0.04 0.87±0.01 0.81±0.01 2.04±0.01Nd 20±4 15±4 16±2 14±3 22±4 19±3 18±2 21±4 Rb 70±5 90±6 118±6 70±8 80±5 58±5 76±6 Sb 0.44±0.03 0.37±0.04 0.47±0.04 0.45±0.04 0.69±0.05 0.46±0.04 0.54±0.04 0.53±0.05Sc 15.1±0.1 10.3±0.1 18.8±0.1 17.0±0.1 14.9±0.1 14.3±0.1 13.5±0.05 15.6±0.1 Se Sm 5.42±0.05 3.80±0.08 5.72±0.06 5.62±0.06 6.24±0.06 6.55±0.07 5.49±0.05 5.90±0.12Ta 0.60±0.05 0.86±0.08 0.80±0.07 1.03±0.08 0.85±0.07 0.72±0.08 0.75±0.08Tb 0.64±0.08 0.58±0.10 0.66±0.11 0.80±0.12 0.91±0.12 0.85±0.13 0.51±0.11 0.71±0.11Th 6.7±0.1 4.9±0.2 6.79±0.14 7.9±0.2 7.71±0.15 6.7±0.1 7.1±0.1 7.2±0.1 U 2.81±0.14 2.2±0.2 2.18±0.20 2.9±0.2 4.3±0.2 3.4±0.2 3.3±0.2 3.2±0.3

Yb 2.06±0.06 1.44±0.03 2.24±0.07 2.24±0.02 2.25±0.09 2.41±0.05 2.29±0.05 2.13±0.09Zn 61±5 190±10 84±7 86±7 114±7 90±6 100±6 80±6

104

Elemental data


164 165 166 167

As 4.6±0.3 5.2±0.3 4.8±0.3 8.4±0.5 Ba 135±30 Br 20±0.4 20±0.4 12±0.4 44±2

Ca% 6.07±1.5 5.24±1.5 5.67±1.5 23.4±2.0 Ce 58.3±1.2 61.2±1.2 52.4±1.1 27.7±0.6 Co 17.9±0.4 17.5±0.4 18.4±0.4 7.09±0.3 Cs 5.9±0.2 5.9±0.2 4.54±0.23 Cr 112±2 125±3 124±2 116±2 Eu 1.25±0.06 1.22±0.1 1.4±0.07 0.54±0.05

Fe% 4.37±0.04 4.47±0.03 4.35±0.04 1.55±0.03 Hf 4.13±0.17 4.83±0.14 4.16±0.17 2.81±0.14

K% 3.87±0.15 3.55±0.14 2.60±0.26 2.20±0.15 La 28.2±0.3 29.5±0.3 23.7±0.2 14.2±0.1 Lu 0.31±0.01 0.33±0.01 0.31±0.01 0.14±0.02 Mo 4.6±0.7 5.3±0.8 2.3±0.6 45±2

Na% 0.71±0.01 0.77±0.01 0.70±0.01 3.26±0.02 Nd 21±4 19±3 18±3 Rb 118±7 108±5 73±7 Sb 0.43±0.04 0.42±0.04 0.7±0.1 Sc 17.7±0.1 18.1±0.1 18.2±0.1 5.07±0.05 Se Sm 5.95±0.06 6.11±0.06 5.88±0.06 3.04±0.09 Ta 0.81±0.08 0.89±0.07 0.55±0.08 0.39±0.06 Tb 0.81±0.13 0.78±0.09 0.76±0.11 0.37±0.08 Th 7.9±0.2 8.1±0.2 6.7±0.1 3.1±0.1 U 3.3±0.2 3.9±0.2 2.3±0.2 7.6±0.3

Yb 2.22±0.07 2.43±0.05 2.36±0.21 1.31±0.13 Zn 70±10 106±7 106±10 210±8

105

Elemental data


168 169 170 171 172 173 174 175

As 8.5±0.3 6.5±0.3 8.7±0.4 9.8±0.3 12.9±0.3 9.5±0.3 9.0±0.4 3.3±0.2 Ba 330±50 320±40 290±50 300±30 350±40 Br 15±0.3 18±1 33±1 82±2 23±1 65±2 53±1 43±1

Ca% 10.03±1.5 8.83±1.5 7.10±1.5 8.87±1.5 31.82±2.0Ce 92±2 94±2 82±2 79±2 79±2 54±1 50±2 7.3±0.5 Co 22.6±0.5 21.8±0.5 15.2±0.5 15.7±0.3 14.6±0.3 20.7±0.5 12.6±0.4 1.29±0.08Cs 1.77±0.23 2.46±0.22 2.46±0.25 1.68±0.20 2.87±0.23 5.42±0.27 3.01±0.2 0.78±0.06Cr 145±5 143±3 172±5 174±5 173±3 122±3 110±3 38.1±1.1 Eu 1.83±0.11 1.80±0.9 1.60±0.1 1.89±0.09 1.75±0.09 1.19±0.07 1.10±0.08 0.17±0.02

Fe% 5.34±0.05 5.29±0.05 5.14±0.05 5.08±0.05 5.27±0.05 4.35±0.04 4.07±0.04 0.24±0.01Hf 12.9±0.3 12.8±0.3 9.3±0.3 8.6±0.3 8.2±0.2 3.7±0.2 3.67±0.22 0.35±0.05

K% 1.52±0.01 1.54±0.08 1.66±0.09 1.70±0.08 4.34±0.17 4.75±0.19 0.23±0.03La 40.0±0.4 42.2±0.4 40.0±0.3 37.3±0.3 39.0±0.4 24.3±0.2 21.6±0.2 5.12±0.05Lu 0.40±0.02 0.50±0.02 0.45±0.02 0.41±0.02 0.42±0.02 0.29±0.01 0.28±0.02 0.67±0.02Mo 6.2±1.2 4.0±1.3 7.1±1.2 10.3±1.3 8.0±0.8 5.2±0.8 3.0±0.7 11.6±0.5

Na% 0.87±0.03 1.0±0.03 0.76±0.01 0.98±0.01 0.64±0.01 0.60±0.01 0.60±0.01 0.25±0.01Nd 22±3 30±5 25±5 26±6 24±4 19±3 18±3 Rb 53±10 63±9 66±10 52±8 76±8 95±9 90±10 Sb 0.87±0.05 0.55±0.04 0.96±0.05 0.99±0.06 0.61±0.04 0.54±0.04 0.54±0.05 0.47±0.02Sc 15.1±0.2 14.9±0.1 15.1±0.1 14.9±0.2 15.4±0.2 18.1±0.2 16.7±0.2 1.06±0.01Se 3.5±1.5 2.7±0.3 Sm 8.62±0.09 8.94±0.09 8.42±0.17 7.97±0.16 8.37±0.17 5.85±0.12 5.61±0.06 1.13±0.06Ta 1.35±0.12 1.67±0.12 1.60±0.13 1.12±0.11 1.42±0.11 0.72±0.09 Tb 1.3±0.2 1.08±0.14 1.01±0.17 1.09±0.14 1.24±0.14 0.90±0.15 1.58±0.03Th 10.9±0.2 10.9±0.2 9.2±0.3 8.8±0.3 9.2±0.2 7.9±0.2 7.1±0.2 0.62±0.05U 2.95±0.21 2.95±0.21 4.60±0.23 3.97±0.20 4.65±0.19 2.82±0.20 2.94±0.15 6.45±0.06

Yb 3.52±0.07 3.38±0.07 3.15±0.09 3.13±0.09 3.0±0.1 2.09±0.08 2.13±0.06 0.51±0.03Zn 120±8 110±8 156±10 168±8 189±8 210±10 126±10 56±6

106

Elemental data


176 177 178 179 180 181 182 183 Ag 4.2±0.4 As 3.4±0.2 6.4±0.3 4.2±0.3 10.7±0.3 10.0±0.5 13.6±0.5 6.2±0.4 7.6±0.2 Ba 320±25 180±30 180±30 198±40 Br 53±1 97±2 260±2 58±2 52±2 20±2 39±2 28±2

Ca% 36.5±2.0 25.41±2.0 19.65±2.0 6.67±1.5 6.87±1.5 32.44±2.0 6.41±1.5 5.62±1.5 Ce 8.45±0.51 36.2±0.7 11.1±0.6 54.5±1.1 53.5±1.6 25.0±0.8 63.4±0.6 66.6±1.3 Co 1.77±0.11 8.6±0.2 2.6±0.2 18.4±0.4 18.0±0.5 4.8±0.3 12.1±0.4 12.5±0.4 Cs 0.2±0.02 1.49±0.04 0.2±0.03 5.37±0.27 4.6±0.3 4.12±0.25 4.40±0.22Cr 40±2 170±3 53±2 120±2 120±4 350±5 118±4 123±3 Eu 0.70±0.04 1.31±0.08 1.20±0.08 0.83±0.08 1.42±0.07 1.39±0.08

Fe% 0.32±0.01 2.07±0.02 0.48±0.01 4.46±0.05 4.46±0.05 1.26±0.04 4.36±0.04 4.58±0.05Hf 0.78±0.07 2.97±0.12 1.0±0.07 4.4±0.2 4.5±0.2 1.57±0.19 5.64±0.23 7.14±0.21

K% 0.39±0.07 1.34±0.09 0.73±0.11 3.15±0.22 2.61±0.23 2.50±0.23 2.02±0.08La 5.23±0.10 19.1±0.2 6.2±0.1 23.9±0.2 25.0±0.3 20.1±0.4 29.0±0.3 30.9±0.3 Lu 0.81±0.04 0.21±0.01 0.65±0.04 0.31±0.01 0.33±0.01 0.38±0.02 0.35±0.01 0.42±0.02Mo 11.2±0.7 14.2±0.7 15.6±0.8 6.0±1.0 4.8±0.9 44±2 4.6±1.0 6.1±0.9

Na% 0.44±0.01 0.52±0.01 1.01±0.01 0.82±0.01 0.85±0.01 0.26±0.01 1.13±0.01 0.53±0.02Nd 14±3 33±2 19±5 21±4 16±2 21±5 21±3 Rb 35±5 60±8 74±10 77±8 84±7 Sb 0.94±0.03 0.82±0.03 0.60±0.04 0.44±0.04 0.67±0.05 1.2±0.1 0.44±0.04 0.51±0.04Sc 1.30±0.03 6.64±0.07 1.57±0.02 19.2±0.1 19.0±0.2 6.91±0.07 17.8±0.1 16.6±0.2 Se 3.0±0.4 4.8±0.3 2.5±0.4 25±2 Sm 1.15±0.06 3.95±0.12 1.43±0.07 6.14±0.12 5.92±0.12 4.55±0.23 6.75±0.14 7.28±0.07Ta 0.57±0.06 1.05±0.08 1.07±0.1 Tb 0.48±0.07 0.21±0.04 0.77±0.15 0.95±0.12 0.80±0.13Th 0.73±0.05 3.92±0.12 1.00±0.05 7.03±0.21 6.7±0.2 2.49±0.20 8.4±0.2 8.9±0.2 U 5.9±0.18 8.4±0.1 7.6±0.2 2.9±0.2 2.03±0.24 26.5±0.5 3.2±0.2 4.3±0.2

Yb 0.57±0.04 1.53±0.05 0.50±0.06 2.40±0.07 2.33±0.07 2.76±0.11 2.55±0.08 2.85±0.10Zn 89±8 155±5 125±5 92±8 108±9 280±12 88±8 118±7

107

Elemental data


184 185 186 187 188 189 190 191

As 3.9±0.3 6.1±0.3 4.9±0.2 6.03±0.24 3.8±0.3 8.1±0.2 6.0±0.4 6.5±0.3 Ba 230±30 340±50 Br 30±1 56±1 40±1 16±1 55±1 40±1 30±1 48±1

Ca% 3.63±1.5 6.56±1.5 5.93±1.5 8.91±1.5 3.99±1.5 7.75±1.5 4.25±1.5 2.94±0.5 Ce 47.9±1.0 53.4±1.1 58.7±1.2 61.1±1.2 59.0±1.8 49.7±1.0 54.8±1.1 54.2±0.6 Co 16.1±0.5 16.1±0.5 13.0±0.4 11.3±0.3 17.9±0.4 17.5±0.4 12.8±0.5 11.9±0.4 Cs 5.0±0.3 3.02±0.24 3.80±0.23 3.13±0.22 5.24±0.26 4.66±0.28 4.84±0.34 3.83±0.27Cr 98±3 130±3 114±2 148±3 120±2 112±2 120±5 112±2 Eu 0.93±0.1 1.20±0.08 1.26±0.08 1.13±0.07 1.27±0.08 1.45±0.09 1.47±0.10 1.22±0.09

Fe% 3.69±0.04 4.68±0.05 4.38±0.04 4.12±0.04 4.20±0.05 4.25±0.04 4.13±0.25 4.02±0.04Hf 3.48±0.21 4.66±0.23 4.48±0.18 6.16±0.18 4.12±0.21 3.45±0.17 4.13±0.25 5.1±0.2

K% 2.36±0.10 2.51±0.11 2.27±0.09 1.74±0.09 2.88±0.12 2.61±0.13 2.26±0.16 2.83±0.17La 23.4±0.3 23.9±0.3 27.3±0.3 29.0±0.3 28.0±0.4 23.0±0.3 25.4±0.3 24.3±0.2 Lu 0.26±0.11 0.29±0.01 0.34±0.08 0.35±0.02 0.29±0.02 0.29±0.01 0.32±0.02 0.33±0.02Mo 3.8±0.9 6.1±1.2 6.7±0.8 6.5±0.8 4.7±1.0 4.4±0.2 6.1±0.9 7.4±0.8

Na% 1.23±0.04 1.08±0.02 1.03±0.02 0.55±0.01 1.39±0.04 0.74±0.07 0.59±0.04 0.73±0.01Nd 14±3 24±2 22±2 20±3 18±3 19±2 24±3 21±2 Rb 86±8 50±8 75±7 66±6 86±8 76±8 72±8 80±8 Sb 0.33±0.04 0.63±0.04 0.42±0.04 0.6±0.04 0.37±0.04 0.41±0.04 0.43±0.04Sc 14.7±0.2 16.9±0.2 16.6±0.1 13.3±0.2 17.4±0.2 17.9±0.2 16.8±0.2 16.2±0.2 Se Sm 5.13±0.15 5.79±0.12 6.23±0.12 6.42±0.13 5.86±0.06 5.67±0.11 6.25±0.12 5.90±0.12Ta 0.61±0.09 0.88±0.1 0.92±0.08 0.95±0.09 0.87±0.10 0.69±0.10Tb 0.75±0.15 0.69±0.12 1.02±0.15 0.74±0.13 0.73±0.14Th 6.8±0.2 7.9±0.2 7.9±0.2 7.0±0.2 8.1±0.2 6.46±0.19 7.6±0.2 7.32±0.22U 2.29±0.23 3.42±0.21 2.75±0.14 4.24±0.17 4.13±0.21 3.0±0.2 3.0±0.2 3.1±0.3

Yb 2.17±0.08 1.97±0.06 2.29±0.07 2.43±0.05 2.22±0.09 2.19±0.09 2.23±0.09 2.27±0.09Zn 70±7 142±10 100±8 184±7 130±10 91±10 99±10

108

Elemental data


192 193 194 195 196

As 4.2±0.3 7.7±0.6 6.8±0.5 5.7±0.3 6.4±0.4 Ba 360±30 310±30 Br 41±1 90±1 72±1 21±1

Ca% 4.46±1.0 4.04±1.0 7.34±1.5 Ce 55.4±1.7 49.8±1.5 51.4±1.5 88.8±2.7 109±2 Co 16.5±0.3 11.5±0.4 14.7±0.4 19.5±0.4 28.1±0.6 Cs 4.98±0.25 4.09±0.25 3.97±0.36 3.08±0.25 3.16±0.28Cr 120±3 109±2 122±4 134±3 160±5 Eu 1.22±0.07 1.12±0.08 1.14±0.1 1.65±0.10 2.1±0.1

Fe% 4.01±0.04 4.20±0.04 3.85±0.08 5.01±0.05 6.03±0.06Hf 4.10±0.15 4.94±0.20 3.71±0.26 14.7±0.3 13.2±0.3

K% 2.98±0.12 2.01±0.34 3.58±0.21 1.45±0.16 1.15±0.14La 26.5±0.3 22.1±0.2 24.0±0.2 39.4±0.4 46.2±0.5 Lu 0.30±0.01 0.31±0.01 0.27±0.02 0.46±0.02 0.55±0.02Mo 5.8±0.9 3.9±0.6 5.3±1.1 2.8±0.9 2.7±0.8

Na% 0.59±0.01 0.73±0.01 0.75±0.01 0.46±0.01Nd 19±3 18±2 20±2 32±6 36±6 Rb 110±10 70±8 100±10 58±8 60±8 Sb 0.41±0.04 0.41±0.05 0.49±0.05 0.69±0.04 0.65±0.05Sc 16.5±0.2 15.2±0.2 15.8±0.2 14.6±0.2 17.1±0.2 Se Sm 5.70±0.06 5.30±0.11 5.65±0.11 8.36±0.17 10.01±0.2Ta 1.06±0.10 0.65±0.09 1.39±0.11 1.82±0.13Tb 0.71±0.12 0.89±0.15 1.31±0.17 1.34±0.16Th 7.5±0.2 7.5±0.2 7.1±0.3 10.8±0.2 11.9±0.2 U 3.51±0.18 3.32±0.23 3.1±0.3 2.54±0.20 2.54±0.2

Yb 2.26±0.05 2.36±0.05 2.10±0.11 3.45±0.07 4.12±0.08Zn 98±8 85±4 147±9 111±7 133±9

109

Elemental data


197 198 199 200 201 202 203 204

As 7.0±0.1 7.1±0.3 6.1±0.3 11.4±0.2 5.0±0.4 4.9±0.3 11.5±0.5 12.6±0.6 Ba 510±46 Br 14±0.2 32±1 18±0.5 18±0.5 6±0.5 60±1 20±1

Ca% 3.70±0.5 15.1±1.0 6.09±0.61 12.28±1.0 6.69±0.67 11.31±1.0 12.52±1.0Ce 115±2 75±2 58±2 83±2 50±1 49±2 85±2 101±2 Co 27.0±0.5 13.9±0.6 18.2±0.6 17.4±0.5 18.2±0.5 17.0±0.7 17.5±0.5 16.5±0.8 Cs 3.48±0.30 3.10±0.4 4.2±0.3 2.59±0.36 3.5±0.4 5.21±0.47 2.3±0.3 2.67±0.21Cr 179±4 170±7 103±3 164±5 107±4 102±4 166±5 183±7 Eu 2.23±0.10 1.50±0.12 1.24±0.1 1.55±0.11 0.97±0.10 1.11±0.13 1.59±0.13 1.92±0.21

Fe% 6.59±0.07 4.45±0.10 4.20±0.04 5.25±0.05 3.88±0.08 4.09±0.08 5.74±0.06 5.61±0.11Hf 14.0±0.4 7.7±0.4 4.9±0.3 9.3±0.4 3.7±0.3 3.2±0.4 8.9±0.4 8.7±0.5

K% 1.26±0.05 2.08±0.06 3.66±0.20 1.54±0.15 1.81±0.14 2.37±0.17 1.82±0.16 1.58±0.25La 48.4±0.5 34.5±0.5 26.4±0.3 39.8±0.4 19.9±0.4 20.9±0.4 38.0±0.4 42.7±0.5 Lu 0.64±0.08 0.44±0.02 0.27±0.03 0.44±0.02 0.32±0.03 0.28±0.03 0.49±0.02 0.51±0.03Mo 5±1 9±1 4±1 11±2 6±1 9±2 6±1

Na% 0.52±0.01 0.62±0.01 1.34±0.01 0.51±0.01 0.36±0.01 1.12±0.01 0.91±0.01Nd 33±4 28±5 23±4 19±3 Rb 82±10 92±9 60±10 60±11 74±13 Sb 0.82±0.31 1.1±0.1 0.82±0.06 1.00±0.05 1.3±0.3 5.4±0.5 1.2±0.06 1.2±0.1 Sc 19.2±0.2 13.6±0.1 16.5±0.1 14.8±0.2 16.5±0.2 16.8±0.2 15.5±0.2 16.2±0.2 Se Sm 10.2±0.1 7.2±0.1 5.6±0.1 8.1±0.1 4.8±0.1 4.8±0.1 8.3±0.1 8.9±0.10 Ta 2.0±0.2 1.24±0.2 1.56±0.16 1.51±0.18 Tb 1.4±0.2 Th 13.8±0.4 8.3±0.3 8.1±0.2 8.9±0.4 5.8±0.3 5.8±0.4 9.4±0.4 8.9±0.5 U 3.2±0.2 5.5±0.3 3.04±0.33 6.2±0.4 1.6±0.4 1.9±0.2 5.0±0.5 4.6±0.3

Yb 4.05±0.08 3.1±0.2 2.13±0.10 3.40±0.10 1.98±0.16 2.02±0.42 3.2±0.2 4.0±0.2 Zn 100±16 210±30 71±10 177±20 86±13 54±9 199±24 284±34

110

Elemental data

QUMRAN SAMPLES concentrations in ppm 205 206 207 208 209 210 211 212

As 10.7±0.5 10.6±0.5 9.5±0.5 7.6±0.5 8.2±0.4 6.7±0.4 12.4±0.5 5.1±0.5 Ba 750±90 470±90 Br 18±1 8±0.4 115±5 20±1 30±2 20±1 80±2 28±2 Ce 93±2 86±2 84±2 66±3 90±2 65±2 70±2 58±2 Co 18.4±0.7 18.0±0.7 19.3±0.6 19.2±0.8 25.1±0.8 10.6±0.5 14.5±0.6 19.4±0.8 Cs 2.6±0.3 2.7±0.4 7.2±0.5 3.8±0.5 5.14±0.46 4.2±0.4 6.0±0.5 Cr 181±5 152±5 150±6 135±5 157±6 116±5 108±3 108±5 Eu 1.89±0.15 1.95±0.16 1.78±0.14 135±5 1.45±0.15 1.32±0.13 1.28±0.12 1.37±0.14

Fe% 5.68±0.11 5.78±0.12 5.15±0.10 4.82±0.10 6.06±0.12 4.30±0.09 3.98±0.08 4.62±0.09Hf 11.0±0.4 9.2±0.5 9.6±0.5 6.3±0.5 13.0±0.5 5.5±0.4 6.2±0.3 4.8±0.4

K% 1.61±0.23 2.12±0.21 2.66±0.27 4.33±0.35 2.80±0.31 2.92±0.29 3.38±0.27 3.13±0.3 La 40.0±0.4 37.9±0.4 38.0±0.4 31.1±0.6 38.1±0.8 26.6±0.5 28.0±0.6 26.9±0.5 Lu 0.50±0.05 0.62±0.03 0.48±0.03 0.53±0.03 0.50±0.04 0.43±0.03 0.37±0.02 0.36±0.03Mo 8±1 7±1 8±1 6±2 5±1 6±1 9±2

Na% 0.49±0.02 1.19±0.01 0.44±0.01 0.78±0.01 0.67±0.01 1.00±0.01 0.61±0.01Nd 29±6 25±4 Rb 50±12 126±19 87±11 133±15 Sb 0.85±0.06 1.06±0.07 1.68±0.08 0.82±0.07 0.95±0.06 0.72±0.06 0.50±0.06 Sc 16.2±0.2 14.8±0.2 14.9±0.2 18.9±0.2 17.6±0.2 17.3±0.2 14.9±0.2 17.0±0.2 Se Sm 8.5±0.1 8.3±0.1 8.3±0.1 6.6±0.1 8.4±0.1 6.7±0.2 7.0±0.1 5.9±0.2 Ta 1.84±0.18 1.81±0.2 1.76±0.19 1.48±0.19 0.87±0.14 Tb 1.46±0.26 1.33±0.27 1.45±0.23 1.45±0.25 Th 9.4±0.4 9.2±0.4 9.0±0.4 8.5±0.5 10.1±0.4 7.8±0.4 8.9±0.4 8.8±0.4 U 3.8±0.3 6.6±0.5 5.5±0.3 4.6±0.7 3.3±0.3 4.6±0.6 2.8±0.3 3.0±0.5

Yb 3.39±0.17 3.92±0.12 3.16±0.22 2.81±0.17 3.29±0.20 2.69±0.21 3.07±0.15 2.28±0.21Zn 188±20 139±17 217±22 206±25 194±19 89±15 52±9 46±10

111

Elemental data


As 6.8±0.3 9.7±1.0 6.1±0.5 11.9±0.4 9.3±0.4 10.7±0.4 8.9±0.5 13.1±0.4 Ba 470±90 427±70 1145±104Br 17±1 36±1 6±1 40±1 32±1 45±2 20±1 36±2 Ce 66±2 84±2 70±2 90±2 86±1 87±2 78±2 87±2 Co 12.3±0.5 18.0±0.5 16.4±0.7 17.7±0.5 17.0±0.5 17.4±0.5 17.1±0.5 18.6±0.6 Cs 4.7±0.4 2.4±0.3 5.6±0.6 1.4±0.3 2.8±0.3 2.04±0.31 4.9±0.3 2.8±0.3 Cr 135±4 169±3 155±6 168±5 166±3 165±3 137±3 170±5 Eu 1.49±0.12 1.83±0.11 1.69±0.15 1.74±0.12 3.81±0.23 2.02±0.10 1.76±0.11 1.71±0.12

Fe% 4.42±0.01 5.30±0.05 5.02±0.10 5.54±0.06 5.06±0.05 5.88±0.06 5.58±0.06 5.01±0.04Hf 6.0±0.3 9.3±0.3 5.8±0.4 9.4±0.4 8.8±0.3 9.1±0.3 7.3±0.3 7.88±0.32

K% 2.80±0.22 2.03±0.20 1.83±0.26 1.77±0.21 1.45±0.16 2.57±0.23 2.62±0.21 1.93±0.24La 27.1±0.5 36.9±0.4 29.7±0.6 37.4±0.8 36.8±0.4 36.8±0.4 33.1±0.3 36.7±0.4 Lu 0.43±0.03 0.52±0.03 0.40±0.03 0.43±0.03 0.53±0.03 0.48±0.02 0.45±0.02 0.45±0.02Mo 11±2 12±2 12±2 10±2 7±2 10±2

Na% 0.61±0.01 0.79±0.01 0.32±0.01 0.92±0.01 0.72±0.01 1.20±0.01 0.61±0.01 0.62±0.01Nd 31±6 24±7 30±5 20±5 Rb 70±9 85±12 52±7 52±7 82±8 63±8 Sb 0.75±0.04 2.12±0.08 1.0±0.06 1.07±0.05 0.90±0.06 4.28±0.09 1.05±0.06Sc 17.8±0.2 15.2±0.2 19.1±0.2 15.1±0.2 14.5±0.2 16.2±0.2 18.2±0.2 14.9±0.2 Se Sm 6.6±0.1 7.8±0.1 6.4±0.1 7.9±0.1 7.9±0.1 7.8±0.1 7.6±0.1 7.5±0.2 Ta 0.97±0.13 1.25±0.14 0.93±0.20 1.23±0.16 1.33±0.12 1.29±0.12 1.03±0.12 1.36±0.14Tb 1.05±0.16 1.18±0.15 1.0±0.2 1.02±0.18Th 8.7±0.3 8.6±0.3 8.4±0.4 8.9±0.3 8.7±0.2 9.5±0.3 9.2±0.3 9.0±0.3 U 4.4±0.3 5.1±0.3 3.2±0.4 4.3±0.3 5.1±0.3 4.5±0.4 2.8±0.3 4.9±0.3

Yb 2.68±0.19 3.38±0.2 2.87±0.23 2.95±0.21 3.39±0.17 3.11±0.12 3.0±0.3 3.40±0.14Zn 109±16 169±19 90±17 202±20 150±18 223±16 95±14 158±17

112

Elemental data


As 8.3±0.5 10.3±0.3 8.2±1.0 4.9±0.3 8.8±0.2 6.5±0.1 Ba 1550±50 313±60 Br 1100±5 380±5 15±1 3±0.3 Ce 63±2 72±1 43±2 49±1 79±1 73±1 Co 17.1±0.9 12.2±0.2 11.5±0.5 11.3±0.3 13.6±0.3 17.7±0.4 Cs 3.6±0.6 1.5±0.2 1.63±0.33 2.3±0.3 6.3±0.3 Cr 103±6 164±3 146±5 103±3 178±4 138±3 Eu 1.44±0.17 1.49±0.06 1.09±0.10 0.94±0.1 1.66±0.08 1.49±0.06

Fe% 3.66±0.11 4.39±0.04 2.41±0.05 2.31±0.05 5.07±0.05 5.30±0.05Hf 6.2±0.5 7.5±0.2 4.6±0.3 7.9±0.2 9.0±0.3 4.7±0.2

K% 2.64±0.40 2.07±0.14 1.14±0.06 0.83±0.03 1.81±0.01 4.33±0.04La 26.7±0.5 34.3±0.3 22.6±0.3 23.5±0.2 36.8±0.4 32.1±0.3 Lu 0.36±0.04 0.45±0.02 0.29±0.03 0.41±0.02 0.42±0.02Mo 9±1 23±3 10±2 9±1

Na% 0.76±0.01 0.91±0.01 1.28±0.01 0.65±0.01 0.87±0.01 0.07±0.01Nd 30±3 24±4 30±3 Rb 49±6 36±7 45±8 119±7 Sb 1.44±0.09 0.95±0.02 1.04±0.20 0.53±0.10 0.91±0.04 0.52±0.02Sc 13.9±0.1 13.1±0.1 7.62±0.08 7.87±0.08 14.4±0.07 21.8±0.07Se Sm 6.9±0.1 7.2±0.1 4.6±0.1 4.7±0.1 7.7±0.1 7.1±0.1 Ta 1.36±0.08 1.14±0.16 0.63±0.09 1.37±0.11 0.75±0.08Tb 1.15±0.13 0.64±0.17 0.37±0.10 0.75±0.14 0.72±0.12Th 7.4±0.4 7.8±0.2 4.6±0.3 5.7±0.2 8.3±0.3 9.6±0.2 U 3.8±0.5 4.9±0.2 10.2±0.4 6.6±0.2 4.3±0.2 2.8±0.1

Yb 2.97±0.27 2.95±0.09 2.46±0.15 3.04±0.09 2.80±0.06Zn 107±16 147±12 209±13 82±8 164±16 46±9

113

Elemental data


As 5.7±0.1 1.0±0.05 5.9±0.2 6.0±0.2 4.0±0.4 6.3±0.2 5.1±0.2 6.5±0.2 Ba 374±70 1024±270 313±80 Br 2±0.02 15±1 85±2 13±1 30±1 15±1 20±1 55±1 Ce 65±1 3.9±0.4 54±2 62±2 29±3 67±1 33±1 54±1 Co 18.3±0.4 1.31±0.09 11.0±0.5 15.9±0.5 7.86±0.80 15.1±0.5 4.26±0.26 17.8±0.4 Cs 5.2±0.2 0.2±0.03 2.02±0.26 2.4±0.3 2.51±0.28 0.88±0.21Cr 116±2 19.3±1.0 103±4 114±3 68±7 128±4 57±2 124±2 Eu 1.31±0.05 0.09±0.01 1.15±0.09 1.34±0.09 1.27±0.10 0.56±0.06 1.24±0.06

Fe% 4.41±0.04 0.25±0.01 3.83±0.08 3.71±0.07 1.19±0.08 3.56±0.07 1.35±0.03 4.36±0.04Hf 4.22±0.21 0.71±0.07 4.22±0.30 9.3±0.4 7.5±0.4 2.8±0.2 4.1±0.2

K% 3.67±0.04 0.15±0.01 2.01±0.08 2.32±0.07 0.91±0.01 1.22±0.07 0.44±0.01 1.52±0.01La 27.6±0.1 2.29±0.05 24.3±0.3 26.8±0.3 11.1±0.4 31.1±0.03 15.0±0.2 22.9±0.2 Lu 0.40±0.02 0.37±0.02 0.43±0.02 0.40±0.02 0.16±0.02 0.38±0.02Mo 3±0.5 7±1 9±1 17±1

Na% 0.06±0.01 0.13±0.01 1.17±0.012 0.67±0.01 1.28±0.01 0.45±0.01 0.30±0.01 2.63±0.02Nd 24±4 Rb 88±7 55±10 53±10 58±10 Sb 0.46±0.02 0.14±0.01 0.57±0.03 3.5±0.1 0.78±0.03 0.42±0.03 0.56±0.04Sc 18.1±0.07 0.79±0.02 15.4±0.2 12.5±0.2 3.3±0.1 11.5±0.1 3.39±0.03 17.9±0.1 Se 13.3±0.7 Sm 6.1±0.1 0.46±0.01 5.5±0.1 5.8±0.1 2.4±0.05 6.6±0.1 3.0±0.01 5.7±0.1 Ta 0.66±0.07 0.88±0.11 0.92±0.13 0.43±0.08 0.72±0.08Tb 0.73±0.10 0.68±0.20 0.35±0.09 0.56±0.13Th 7.9±0.2 0.52±0.06 6.6±0.3 6.8±0.1 3.7±0.5 7.2±0.3 3.8±0.2 6.2±0.2 U 2.4±0.1 0.9±0.08 3.8±0.3 3.9±0.2 3.5±0.7 5.3±0.2 2.4±0.2 2.6±0.2

Yb 2.53±0.03 0.21±0.04 2.32±0.14 2.95±0.12 2.27±0.14 1.06±0.07 2.07±0.10Zn 40±6 24±2 58±8 74±12 455±27 136±12 46±5 86±10

114

Elemental data


As 9.7±0.3 6.1±0.2 5.8±0.4 8.6±0.3 7.6±0.3 4±1 5.0±0.4 Ba Br 34±2 14±1 45±1 16±1 30±1 27±1 13±1 7±1 Ce 57±2 65±1 48±1 58±2 53±2 56±1 79±1 57±2 Co 18.0±0.2 19.5±0.6 10.4±0.4 10.7±0.3 12.5±0.4 19.1±0.4 18.4±0.4 17.2±0.5 Cs 3.1±0.3 6.3±0.4 1.9±0.2 3.8±0.3 6.2±0.3 5.3±0.3 4.2±0.3 6.8±0.3 Cr 131±4 126±4 97±4 141±4 153±3 184±4 167±3 193±4 Eu 1.28±0.09 1.28±0.09 1.06±0.1 1.19±0.08 1.17±0.08 1.42±0.07 1.59±0.08 1.13±0.08

Fe% 4.46±0.05 4.65±0.05 3.11±0.06 4.13±0.04 4.05±0.04 4.64±0.05 4.62±0.05 4.58±0.05Hf 4.3±0.3 4.98±0.30 5.3±0.3 4.17±0.25 6.4±0.3 4.2±0.3 5.4±0.2 4.7±0.3

K% 2.09±0.11 4.12±0.12 2.47±0.30 1.65±0.28 2.89±0.35 2.64±0.30 3.51±0.39La 23.8±0.2 28.9±0.3 21.1±0.4 25.6±0.5 24.1±0.5 25.2±0.5 35.4±0.4 26.3±0.5 Lu 0.36±0.02 0.40±0.02 0.24±0.02 0.38±0.02 0.34±0.02 0.39±0.02 0.38±0.02 0.39±0.02Mo 4±1 7±1 6±1 7±1 5±1 6±1 7±1

Na% 1.85±0.01 0.42±0.01 0.89±0.01 0.69±0.01 0.46±0.01 1.14±0.01 0.49±0.01 0.53±0.01Nd Rb 55±9 128±11 67±8 98±8 74±7 90±7 95±9 Sb 0.53±0.04 0.57±0.03 0.91±0.06 0.49±0.04 0.61±0.04 0.53±0.04 Sc 18.9±0.2 17.8±0.2 11.0±0.1 16.1±0.2 15.6±0.2 19.6±0.2 16.7±0.2 17.1±0.2 Se Sm 6.0±0.1 6.2±0.1 4.6±0.1 5.7±0.1 5.4±0.1 6.1±0.1 7.2±0.1 5.6±0.1 Ta 0.52±0.10 0.94±0.11 0.75±0.10 0.7±0.1 0.68±0.08 1.15±0.10 Tb 0.88±0.13 Th 6.6±0.1 8.3±0.3 5.7±0.2 7.1±0.2 7.3±0.2 6.9±0.2 9.5±0.2 7.8±0.2 U 2.5±0.2 4.3±0.2 4.2±0.3 3.7±0.4 4.8±0.2 2.4±0.2 2.1±0.3 2.7±0.2

Yb 2.4±0.12 2.6±0.08 2.4±0.2 2.6±0.2 2.5±0.2 2.8±0.1 2.5±0.1 2.3±0.1 Zn 33±5 80±11 57±11 103±14 88±13 49±8 60±9 30±5

115

Elemental data


As 6.6±0.5 7.9±1.4 6.4±0.5 6.9±0.6 7.4±0.4 8.8±0.6 7.5±0.6 9.6±0.2 Ba Br 10±1 17±1 16±1 12±1 15±1 53±2 64±1 Ce 63±2 64±1 62±2 70±2 62±1 54±1 62±2 80±2 Co 19.3±0.4 19.4±0.4 19.6±0.6 18.8±0.4 19.9±0.4 20.5±0.6 14.7±0.4 16.7±0.5 Cs 6.6±0.3 4.6±0.3 6.0±0.4 6.9±0.3 6.7±0.3 3.7±0.4 3.1±0.3 2.3±0.3 Cr 211±4 168±4 256±5 210±4 224±5 283±6 339±5 425±8 Eu 1.43±0.09 1.38±0.08 1.18±0.09 1.47±0.01 1.22±0.09 1.18±0.09 1.44±0.09 1.47±0.10

Fe% 4.64±0.05 4.50±0.01 4.43±0.04 4.71±0.05 4.45±0.05 4.54±0.05 4.31±0.04 4.88±0.05Hf 5.4±0.3 4.7±0.2 4.6±0.3 5.0±0.3 4.6±0.3 4.8±0.3 6.9±0.3 9.3±0.4

K% 4.68±0.47 3.94±0.43 3.77±0.49 4.07±0.45 La 30.3±0.3 27.6±0.6 28.4±0.6 31.8±0.6 27.3±0.6 22.3±0.5 28.7±0.6 36.6±0.7 Lu 0.39±0.02 0.40±0.03 0.40±0.03 0.38±0.03 0.34±0.02 0.33±0.03 0.41±0.02 0.44±0.04Mo 10±2 8±1 8±2 6±2 5±1 2±0.4 9±2 10±2

Na% 0.72±0.01 0.79±0.01 0.63±0.01 0.68±0.02 0.81±0.01 1.17±0.01 1.05±0.01 1.53±0.02Nd 21±1 Rb 130±10 108±9 134±11 133±11 98±10 70±12 Sb 0.53±0.05 0.83±0.06 0.75±0.06 0.72±0.05 1.2±0.3 0.71±0.06 0.96±0.10Sc 18.2±0.2 17.5±0.3 17.3±0.2 18.4±0.2 17.0±0.2 18.4±0.2 13.6±0.1 13.6±0.2 Se Sm 6.4±0.1 6.1±0.1 6.0±0.1 6.6±0.1 6.2±0.1 5.8±0.1 6.3±0.1 7.4±0.1 Ta 0.98±0.11 0.84±0.10 1.09±0.11 0.99±0.12 0.93±0.11 0.77±0.11 1.42±0.16Tb 0.75±0.13 0.70±0.16 Th 8.5±0.3 8.3±0.3 8.8±0.3 9.2±0.3 7.9±0.2 6.9±0.3 7.4±0.2 8.0±0.3 U 3.6±0.3 3.5±0.1 4.2±0.3 3.4±0.3 3.3±0.5 2.5±0.5 4.5±0.4 4.8±0.8

Yb 2.46±0.15 2.55±0.15 2.55±0.08 2.67±0.16 2.41±0.14 2.42±0.19 2.77±0.17 3.26±0.23Zn 66±12 79±15 70±10 89±13 63±11 86±17 132±13 137±14

116

Elemental data


As 6.8±0.6 12.3±0.9 6.8±0.7 6.9±0.6 12±1 11±1 12±1 Ba 520±70 580±60 Br 40±2 82±2 88±2 56±2 17±1 18±1 29±1 29±2 Ce 70±1 65±2 59±1 83±2 66±1 96±2 87±2 86±2 Co 14.5±0.4 15.2±0.6 20.5±0.4 16.5±0.5 20.8±0.4 16.4±0.5 16.3±0.5 18.3±0.6 Cs 3.2±0.3 5.3±0.5 2.7±0.3 2.3±0.3 6.6±0.3 1.6±0.3 3.4±0.3 2.2±0.3 Cr 140±4 139±6 109±3 181±4 115±2 188±4 155±5 169±5 Eu 1.48±0.12 1.41±0.15 1.17±0.07 1.78±0.10 1.44±0.07 1.71±0.1 1.89±0.11 1.83±0.11

Fe% 4.47±0.09 4.16±0.08 4.37±0.05 4.89±0.05 4.69±0.05 5.72±0.06 5.49±0.05 5.65±0.06Hf 7.4±0.2 4.4±0.4 4.7±0.2 9.8±0.3 4.8±0.2 10.9±0.4 8.4±0.3 9.6±0.4

K% 4.39±0.57 3.42±0.51 La 32.7±0.7 27.0±0.5 28.6±0.6 38.5±0.4 29.3±0.3 41.6±0.8 38.2±0.8 38.0±0.8 Lu 0.43±0.02 0.42±0.03 0.33±0.02 0.48±0.02 0.42±0.02 0.51±0.04 0.43±0.03 0.48±0.02Mo 11±2 10±2 11±2 10±2 10±2 9±2

Na% 1.12±0.01 1.01±0.01 2.52±0.05 0.78±0.01 0.73±0.01 1.62±0.03 0.95±0.02 1.28±0.03Nd Rb 88±16 72±9 57±8 130±10 67±12 80±10 50±11 Sb 0.8±0.1 0.9±0.1 0.7±0.2 1.0±0.08 1.1±0.1 0.9±0.1 Sc 13.8±0.1 17.0±0.2 17.0±0.2 14.5±0.1 18.3±0.1 16.2±0.2 16.5±0.2 15.7±0.2 Se Sm 7.0±0.1 6.55±0.13 5.74±0.11 8.23±0.08 6.1±0.1 8.6±0.2 8.3±0.1 8.1±0.1 Ta 1.11±0.14 1.22±0.11 1.38±0.12 0.93±0.09 1.76±0.16 1.24±0.15 1.47±0.16Tb 0.74±0.13 0.82±0.13 1.15±0.17Th 8.8±0.4 8.1±0.4 8.2±0.3 9.6±0.3 8.4±0.3 10.0±0.3 9.5±0.3 9.9±0.3 U 5.0±0.6 3.3±0.4 5.4±0.3 3.7±0.2 3.8±0.5 5.3±0.6 3.6±0.5

Yb 2.93±0.15 2.47±0.17 2.44±0.15 3.6±0.1 2.39±0.12 2.96±0.21 3.33±0.10 3.32±0.2 Zn 127±14 109±15 84±14 134±13 86±8 153±15 117±14 154±15

117

Elemental data


As 12±1 7±1 7±1 Ba 560±100 420±80 Br 33±2 10±1 14±1 13±1 18±2 15±1 17±1 24±2 Ce 84±2 84±2 72±2 65±1 64±1 85±2 86±3 64±2 Co 18.2±0.7 18.7±0.6 14.6±0.4 18.3±0.6 13.6±0.4 16.3±0.7 14.5±0.7 13.0±0.4 Cs 3.8±0.4 3.9±0.4 5.4±0.4 5.2±0.4 5.0±0.3 4.2±0.4 3.0±0.4 4.2±0.3 Cr 165±5 200±4 124±4 115±5 124±4 167±5 220±7 140±3 Eu 1.86±0.15 2.08±0.12 1.59±0.11 1.54±0.11 1.47±0.09 1.72±0.14 1.83±0.17 1.43±0.09

Fe% 5.28±0.11 5.68±0.06 4.69±0.05 4.50±0.04 4.52±0.05 5.74±0.12 5.19±0.11 4.54±0.05Hf 8.8±0.4 7.75±0.31 5.7±0.3 5.3±0.3 7.4±0.3 8.3±0.4 7.0±0.5 5.1±0.3

K% 1.67±0.03 2.48±0.02La 37.8±0.8 41.4±0.8 29.5±0.6 29.9±0.6 26.2±0.5 35.7±1.1 37.7±0.4 25.9±0.3 Lu 0.57±0.03 0.58±0.03 0.48±0.02 0.43±0.03 0.40±0.02 0.48±0.02 0.49±0.02 0.42±0.03Mo 13±2 8±2 7±1 11±2 15±2 16±2 6±1

Na% 1.19±0.02 0.60±0.02 0.48±0.01 1.06±0.02 0.45±0.02 0.54±0.03 0.53±0.01 1.24±0.01Nd Rb 93±16 80±11 112±12 92±10 112±12 92±13 64±8 Sb 1.4±0.2 1.1±0.4 0.6±0.1 0.7±0.1 1.0±0.3 1.4±0.2 1.1±0.1 0.57±0.02Sc 16.1±0.2 17.9±0.2 18.7±0.2 17.3±0.2 17.9±0.2 17.9±0.2 14.9±0.2 17.7±0.2 Se Sm 8.2±0.1 9.0±0.1 7.6±0.2 7.0±0.1 6.9±0.1 8.1±0.1 7.8±0.1 5.9±0.1 Ta 1.49±0.16 0.94±0.13 0.95±0.13 0.8±0.1 0.91±0.1 Tb 1.21±0.21 1.05±0.22 Th 10.3±0.4 10.3±0.3 9.2±0.3 8.4±0.3 9.1±0.3 9.2±0.4 9.3±0.5 8.1±0.2 U 5.8±0.8 5.6±0.2 4.5±0.3 3.7±0.6 4.0±0.3 5.8±0.9 6.0±0.6 4.0±0.16

Yb 3.33±0.27 3.53±0.14 2.76±0.08 3.0±0.2 2.88±0.14 2.94±0.26 3.0±0.3 2.29±0.18Zn 153±18 152±15 70±10 37±6 72±12 107±15 230±20 128±13

118

Elemental data


As 5.3±0.1 1.8±0.3 7.6±0.2 6.8±0.2 5.8±0.2 8.3±0.2 3.2±0.2 9.9±0.4 Ba Br 20±2 14±1 23±1 32±2 11±1 10±1 28±1 100±2 Ce 47±1 53±2 53±2 56±1 64±1 88±2 76±2 54±2 Co 16.5±0.5 19.0±1.0 12.8±0.5 19.4±0.6 14.0±0.4 15.6±0.6 13.6±0.5 20.1±0.6 Cs 4.0±0.3 3.6±0.6 3.5±0.5 4.59±0.37 4.0±0.3 2.3±0.4 2.2±0.4 3.9±0.5 Cr 126±4 250±8 147±4 160±5 156±3 248±5 240±5 245±7 Eu 1.01±0.08 1.05±0.12 1.10±0.1 1.48±0.1 1.92±0.13 1.71±0.12 1.32±0.13

Fe% 3.70±0.04 4.43±0.09 3.74±0.07 4.58±0.05 4.75±0.05 5.24±0.11 4.42±0.09 4.20±0.1 Hf 3.56±0.25 5.52±0.55 3.8±0.3 5.6±0.3 7.0±0.3 9.6±0.4 7.8±0.4 4.02±0.4

K% 1.84±0.02 1.56±0.06 1.98±0.04 2.06±0.04 1.98±0.04 1.71±0.03 1.50±0.05 2.90±0.06La 21.2±0.2 22.0±0.4 23.3±0.2 21.9±0.2 25.2±0.3 38.7±0.4 32.9±0.3 22.9±0.5 Lu 0.31±0.03 0.35±0.03 0.30±0.03 0.44±0.02 0.40±0.03 0.26±0.06Mo 13±2 6±1 12±1 7±1 11±1

Na% 0.42±0.01 2.15±0.01 1.08±0.01 0.80±0.01 0.98±0.01 0.61±0.01 0.77±0.01 2.39±0.01Nd Rb 63±9 67±8 79±14 89±13 Sb 0.43±0.04 0.8±0.1 0.5±0.1 0.4±0.09 1.0±0.05 0.9±0.1 0.74±0.12Sc 15.9±0.2 18.0±0.2 14.4±0.1 19.0±0.2 16.3±0.2 15.4±0.2 13.4±0.1 17.6±0.2 Se Sm 4.7±0.1 5.2±0.1 5.0±0.1 5.3±0.1 6.2±0.1 8.2±0.1 7.1±0.1 5.7±0.1 Ta 0.81±0.11 1.12±0.18 Tb 0.88±0.18 Th 5.9±0.2 6.7±0.5 6.3±0.3 7.2±0.3 8.0±0.2 9.0±0.4 7.9±0.3 7.0±0.4 U 2.6±0.2 3.9±0.6 1.33±0.7 3.2±0.2 6.3±0.3 4.7±0.2 3.7±0.8

Yb 2.06±0.21 2.27±0.45 1.51±0.23 2.25±0.18 2.51±0.18 3.39±0.17 2.91±0.17 2.17±0.35Zn 68±10 70±15 73±16 57±9 160±18 96±17 86±1

119

Elemental data

QUMRAN SAMPLES Concentrations in ppm 285 286 287 288 289 290 291 292

As 11,8±0,2 5,9±0,2 6,1±0,2 5,1±0,2 3,8±0,2 6,7±0,3 3,1±0,2 5,7±0,3 Ba 316±40 400±50 330±50 482±52 Br 3,3±0,1 24±1 18±1 20±1 9±0,2 50±1 17±1 34±1

Ca% 27,6±0,6 9,57±1,3 10,56±1,42 7,76±0,39 4,96±0,29 14,63±0,6 4,42±0,27 11,47±0,57Ce 12,5±0,6 64,4±1,3 42,4±1,7 50,2±1,5 50,5±1,5 56,1±1,2 43,0±0,9 61,8±1,2 Co 1,92±0,10 14,0±0,14 11,1±0,3 14,7±0,3 13,5±0,3 12,6±0,3 8,2±0,2 15,2±0,3 Cs 2,63±0,16 3,45±0,24 3,69±0,22 5,06±0,20 1,71±0,19 3,33±0,17 3,18±0,25 Cr 290±3 168±2 86±3 142±3 92±2 160±3 78±1 166±3 Eu 0,47±0,03 1,44±0,04 0,96±0,07 1,33±0,07 1,38±0,06 1,37±0,07 1,10±0,06 1,56±0,08

Fe% 0,34±0,01 4,90±0,05 3,45±0,04 4,20±0,04 3,64±0,04 4,55±0,05 2,99±0,03 4,58±0,05 Hf 0,60±0,05 7,36±0,10 3,19±0,19 5,66±0,23 7,16±0,21 7,41±0,22 4,49±0,13 7,22±0,22

K% 1,66±0,10 1,72±0,10 2,53±0,02 2,23±0,11 1,54±0,14 1,81±0,01 1,93±0,17 La 12,8±0,2 33,3±0,3 21,5±0,2 26,9±0,3 25,1±0,3 28,4±0,3 20,9±0,2 33,3±0,3 Lu 0,31±0,02 0,45±0,02 0,28±0,01 0,32±0,02 0,38±0,02 0,44±0,02 0,30±0,02 0,45±0,02 Mo 20±2 5±0,2 2±0,8 1,4±0,7

Na% 0,096±0,01 0,63±0,01 0,83±0,01 0,76±0,01 0,41±0,01 0,85±0,01 0,61±0,01 0,66±0,01 Nd 27±5 24±5 29±6 20±4 Rb 57±4 58±8 73±7 85±6 46±7 54±5 70±8 Sb 1,01±0,03 0,77±0,04 0,39±0,04 0,57±0,03 0,27±0,03 0,82±0,06 0,30±0,03 0,80±0,05 Sc 3,24±0,03 15,3±0,2 13,7±0,1 15,3±0,2 16,0±0,2 13,2±0,1 12,5±0,2 15,7±0,2 Se 32,8±1 3,6±0,6 Sm 2,68±0,11 5,81±0,17 3,87±0,12 4,94±0,10 4,96±0,15 5,09±0,15 4,06±0,12 5,84±0,18 Ta 1,55±0,08 1,05±0,12 1,08±0,09 1,3±0,12 0,70±0,07 1,42±0,11 Tb 0,34±0,05 0,94±0,08 0,82±0,11 0,73±0,12 0,88±0,11 0,47±0,08 0,96±0,13 Th 1,02±0,06 8,11±0,08 6,11±0,18 7,18±0,22 6,94±0,14 7,45±0,22 5,51±0,11 8,02±0,24 U 22,7±0,23 4,2±0,21 3,04±0,18 2,99±0,15 3,32±0,13 3,82±0,20 1,74±0,10 4,26±0,21

Yb 2,11±0,06 3,33±1 2,00±0,12 2,69±0,08 2,62±0,1 2,93±0,06 2,14±0,11 3,06±0,12 Zn 304±9 214±9 140±10 204±8 113±6 207±8 77±6 180±9

120

Elemental data


As 6,3±0,4 7,1±0,4 3,8±0,2 4,7±0,2 6,8±0,3 5,9±0,3 5,7±0,2 3,9±0,2 Ba 1000±50 650±65 722±50 Br 41±1 68±2 4±0,3 11±1 3±0,3 4±0,2 0,7±0,1 18±1

Ca% 8,86±0,53 17,30±2,7 7,95±0,40 5,87±0,35 8,36±0,50 8,18±0,33 8,21±0,49 12,57±0,4Ce 49,3±1,5 53,9±1,6 49,7±1,5 53,9±1,6 48,8±1,5 52,1±1,6 100±2 73,7±2,2 Co 15,9±0,5 9,7±0,3 12,4±0,3 12,2±0,2 16,9±0,3 14,2±0,3 9,94±0,2 27,6±0,6 Cs 5,50±0,27 1,72±0,16 4,97±0,25 5,10±0,20 7,46±0,30 6,92±0,28 10,5±0,1 3,81±0,23Cr 116±3 170±4 94±3 110±2 117±4 118±4 81±2 96±3 Eu 1,33±0,08 1,40±0,06 1,18±0,06 1,34±0,05 1,30±0,08 1,40±0,07 1,62±0,06 1,58±0,06

Fe% 4,18±0,05 3,10±0,03 3,90±0,04 4,27±0,04 4,49±0,05 4,85±0,05 3,68±0,04 3,43±0,03Hf 4,09±0,25 3,62±0,18 5,81±0,23 6,31±0,19 3,67±0,66 4,18±0,25 8,17±0,16 6,93±0,21

K% 3,74±0,22 1,95±0,16 1,84±0,09 2,19±0,09 4,22±0,17 4,28±0,17 1,44±0,10 1,16±0,13La 23,5±0,2 34,2±0,34 24,7±0,3 25,5±0,3 24,6±0,3 24,5±0,2 45,0±0,5 38,0±0,3 Lu 0,41±0,02 0,49±0,03 0,37±0,02 0,41±0,04 0,34±0,02 0,37±0,02 0,41±0,02 0,41±0,02Mo 4±1 2±0,9

Na% 0,73±0,01 0,61±0,01 0,27±0,01 0,30±0,01 0,34±0,01 0,28±0,02 0,99±0,09 1,14±0,01Nd 22±6 25±5 19±5 20±4 31±7 16±2 26±5 Rb 106±10 42±5 83±8 76±7 103±9 117±11 88±6 Sb 0,82±0,20 0,53±0,05 0,41±0,03 0,48±0,03 0,49±0,04 0,47±0,04 0,46±0,03 0,28±0,04Sc 17,7±0,2 11,4±5,1 15,9±0,2 17,9±0,2 18,7±0,2 19,5±0,2 11,1±0,1 13,6±0,1 Se Sm 4,73±0,14 5,66±0,17 4,73±0,14 5,30±0,16 4,94±0,20 4,92±0,15 7,09±0,14 6,27±0,13Ta 0,81±0,13 1,09±0,10 1,17±0,09 1,07±0,09 1,07±0,11 1,07±0,11 1,66±0,08 1,41±0,12Tb 0,98±0,10 0,88±0,11 0,76±0,10 0,93±0,1 0,83±0,12Th 7,72±0,23 7,97±0,16 7,24±0,22 7,52±0,15 7,73±0,23 8,06±0,24 21,5±0,2 9,69±0,19U 3,08±0,18 6,25±0,19 2,81±0,14 2,99±0,15 3,17±0,16 2,83±0,20 3,29±0,16 2,93±0,21

Yb 2,21±0,15 3,22±0,13 2,60±0,05 2,75±0,08 2,48±0,25 2,45±0,12 2,64±0,08 2,87±0,11Zn 182±9 187±7 115±6 110±7 112±9 121±7 80±5 158±6

121

Elemental data

QUMRAN SAMPLES Concentrations in ppm 301 302 303 304 305 306 306/b 307

As 5,4±0,2 7,7±0,4 10,4±0,3 5,6±0,3 18,8±0,4 4,0±0,2 3,7±0,2 13,4±0,4 Ba 240±40 330±40 229±40 820±60 Br 22±1 100±2 26±1 6±0,6 23±0,6 19±0,4 14±1

Ca% 8,11±0,41 29,58±0,3 8,74±0,52 8,07±0,4 6,34±0,95 31,11±0,6 30,56±0,6 9,81±0,39Ce 48,9±1,5 34,0±0,7 66,4±1,3 48,6±1,5 43,6±1,3 26,4±1,1 17,2±0,9 93,2±1,9 Co 12,1±0,2 11,0±0,2 16,1±0,3 14,6±0,3 20,1±0,4 8,70±0,26 4,05±0,16 13,3±0,3 Cs 1,60±0,14 1,51±0,11 3,14±0,22 5,60±0,22 3,42±0,24 0,95±0,15 0,75±0,11 3,45±0,21Cr 130±3 135±3 160±3 114±3 122±2 105±2 72±2 101±3 Eu 1,24±0,05 0,70±0,03 1,65±0,07 1,30±0,06 1,30±0,06 0,68±0,05 0,44±0,04 1,62±0,06

Fe% 3,64±0,04 2,04±0,02 5,45±0,05 4,54±0,05 4,51±0,05 2,13±0,04 2,07±0,02 4,24±0,04Hf 7,01±0,21 3,60±0,10 5,98±0,24 3,73±0,22 4,16±0,25 2,25±0,16 1,46±0,12 5,91±0,18

K% 1,41±0,01 1,31±0,12 2,26±0,18 4,36±0,22 2,77±0,19 0,52±0,01 2,65±0,26La 25,7±0,3 19,7±0,2 35,2±0,4 23,7±0,2 21,9±0,2 17,02±0,34 9,60±0,19 44,5±0,5 Lu 0,38±0,06 0,24±0,02 0,46±0,02 0,35±0,02 0,35±0,02 0,21±0,05 0,14±0,01 0,37±0,02Mo 3±0,7 2±0,9 5±0,7 7±1

Na% 0,60±0,01 0,65±0,01 0,74±0,01 0,21±0,01 0,82±0,01 0,26±0,01 0,19±0,01 0,68±0,01Nd 21±5 21±5 24±9 24±8 Rb 42±5 29±4 72±9 84±9 70±8 86±9 Sb 0,63±0,04 0,90±0,05 0,52±0,04 0,40±0,04 0,70±0,05 0,45±0,03 0,32±0,02 0,74±0,04Sc 11,2±0,11 6,61±0,07 18,3±0,2 19,2±0,2 17,6±0,2 8,74±0,09 6,25±0,06 12,2±0,2 Se 43±1 5,7±1,0 Sm 4,63±0,09 3,19±0,10 6,15±0,18 4,52±0,18 4,29±0,13 2,60±0,08 1,89±0,08 6,85±0,21Ta 1,25±0,09 0,64±0,06 1,58±0,13 0,94±0,09 0,98±0,11 1,63±0,11Tb 0,70±0,11 0,36±0,06 0,80±0,13 1,06±0,13 0,64±0,09 Th 5,97±0,18 3,82±0,11 8,50±0,26 7,58±0,23 6,32±0,25 2,62±0,16 1,48±0,12 20,3±0,2 U 3,88±0,16 7,85±0,24 3,89±0,23 2,87±0,11 2,47±0,22 6,55±0,13 10,2±0,1 4,37±0,13

Yb 2,48±0,07 1,86±0,09 3,22±0,16 2,33±0,12 2,50±0,15 1,53±0,09 1,01±0,07 2,84±0,11Zn 153±6 230±20 174±7 137±8 121±7 115±6 70±3 134±7

122

Elemental data


As 6,3±0,3 7,1±0,2 6,1±0,3 7,5±0,2 6,67±0,27 4,71±0,24 6,3±0,3 8,9±0,3 Ba 470±50 Br 9±0,5 13±1 58±1 24±1 14±1 24±1 22±1 10±1

Ca% 8,88±0,53 10,92±0,4 17,44±0,5 12,02±0,5 4,25±0,3 6,83±0,34 9,73±0,4 6,20±0,3 Ce 67,8±1,4 75,0±2,0 37,5±1,2 58,2±1,3 50,6±1,0 40,2±0,8 53,9±1,1 57,5±1,2 Co 15,3±0,3 17,0±0,3 10,3±0,3 16,1±0,1 18,8±0,4 8,9±0,2 11,1±0,2 16,8±0,3 Cs 2,70±0,22 2,24±0,22 5,04±0,25 4,52±0,23 7,22±0,29 3,83±0,19 4,57±0,23 5,28±0,21Cr 211±4 201±4 133±3 153±3 154±4 133±3 138±3 150±3 Eu 1,62±0,08 1,74±0,07 0,91±0,06 1,41±0,06 1,19±0,06 1,04±0,05 1,29±0,05 1,39±0,06

Fe% 4,87±0,05 5,21±0,05 3,46±0,03 4,52±0,05 4,87±0,05 3,53±0,04 3,99±0,04 4,55±0,05Hf 7,25±0,22 10,2±0,3 2,90±0,17 4,97±0,20 3,77±0,19 4,87±0,15 4,90±0,20 5,34±0,21

K% 1,79±0,09 1,77±0,11 3,20±0,13 0,20±0,11 3,49±0,14 2,17±0,13 1,90±0,11 3,05±0,15La 33,5±0,3 36,7±0,4 18,6±0,2 27,2±0,3 24,1±0,2 20,5±0,2 24,5±0,2 27,7±0,3 Lu 0,44±0,02 0,45±0,02 0,26±0,01 0,37±0,02 0,32±0,02 0,32±0,02 0,38±0,02 0,40±0,04Mo 3±1 3±1 4±1 4±1 2±0,8

Na% 0,61±0,01 0,61±0,06 0,42±0,01 0,60±0,06 0,47±0,05 0,58±0,01 0,46±0,01 0,65±0,01Nd 32±8 14±4 30±5 21±4 20±4 18±4 26±5 Rb 59±2 44±7 95±9 89±10 89±6 69±6 84±7 106±7 Sb 0,75±0,05 0,62±0,04 0,49±0,04 0,42±0,04 0,31±0,03 0,45±0,04 0,57±0,03Sc 15,9±0,2 15,5±0,2 14,4±0,1 17,6±0,2 20,5±0,2 14,7±0,2 16,1±0,2 18,4±0,2 Se Sm 6,0±0,2 6,48±0,26 3,65±0,11 5,51±0,05 4,66±0,14 3,86±0,12 5,10±0,15 5,50±0,17Ta 1,61±0,13 2,06±0,14 0,56±0,09 1,07±0,11 0,96±0,10 1,01±0,08 0,99±0,08 1,11±0,09Tb 1,10±0,15 0,98±0,13 0,85±0,12 0,76±0,09 1,10±0,11 0,92±0,10Th 8,27±0,17 9,55±0,19 5,59±0,22 7,82±0,23 8,24±0,16 6,39±0,13 7,11±0,14 8,29±0,17U 4,29±0,21 4,41±0,18 2,18±0,22 3,41±0,20 2,85±0,17 3,14±0,22 3,15±0,16 3,23±0,16

Yb 2,67±0,32 3,37±0,07 1,86±0,22 2,71±0,12 2,37±0,07 2,07±0,10 2,57±0,15 2,94±0,09Zn 193±8 170±7 100±8 129±9 168±10 125±3 105±7 190±8

123

Elemental data

QUMRAN SAMPLES Concentrations in ppm 316 317 318 319 320 321

As 11,8±0,5 6,9±0,3 6,7±0,3 5,7±0,4 5,4±0,3 8,9±0,5 Ba 411±60 Br 18±1 7±0,5 37±0,5 23±0,5 20±1 6±0,3

Ca% 4,40±1,3 3,83±0,4 6,68±0,3 8,84±0,3 4,68±0,29 Ce 73,4±2,2 44,8±1,4 45,4±1,4 45,5±1,0 49,0±1,0 60,7±1,8 Co 16,1±0,3 9,2±0,2 12,2±0,2 17,8±0,4 10,4±0,2 15,4±0,3 Cs 3,81±0,23 7,55±0,23 5,78±0,23 5,45±0,22 5,43±0,22 6,16±0,25Cr 228±3 170±5 140±3 131±3 156±3 179±4 Eu 1,76±0,07 0,99±0,05 1,15±0,05 2,22±0,22 1,30±0,10 1,48±0,06

Fe% 5,52±0,06 4,84±0,05 4,19±0,05 3,95±0,04 4,31±0,04 4,95±0,05Hf 6,13±0,25 3,16±0,19 6,96±0,21 5,39±0,16 5,63±0,17 6,43±0,18

K% 1,60±0,19 4,82±0,24 1,65±0,18 2,22±0,22 2,79±0,25 2,74±0,27La 41,4±0,4 21,0±0,5 23,0±0,2 23,5±0,5 23,7±0,2 28,7±0,3 Lu 0,53±0,02 0,29±0,01 0,35±0,02 0,37±0,02 0,40±0,02 0,42±0,02Mo 2±0,5

Na% 0,68±0,01 0,31±0,01 0,50±0,01 0,59±0,01 0,74±0,01 0,57±0,01Nd 32±8 16±5 25±5 17±5 19±7 Rb 64±7 125±8 85±5 104±7 92±6 109±8 Sb 0,79±0,06 0,42±0,04 0,52±0,04 0,40±0,04 0,39±0,03 0,50±0,05Sc 17,5±0,2 19,2±0,2 16,3±0,2 15,8±0,2 18,2±0,2 20,1±0,2 Se 5,1±1,0 Sm 7,27±0,15 4,16±0,12 4,55±0,14 4,85±0,04 4,95±0,15 5,57±0,11Ta 2,13±0,13 1,10±0,09 1,24±0,09 1,10±0,10 1,00±0,08 1,53±0,11Tb 1,13±0,11 0,61±0,10 0,81±0,09 0,69±0,10 0,76±0,10 Th 9,58±0,19 7,65±0,15 7,53±0,15 7,09±0,14 7,74±0,15 9,23±0,18U 4,29±0,26 3,30±0,17 3,01±0,12 2,79±0,14 3,17±0,16 2,14±0,21

Yb 3,65±0,07 1,97±0,10 2,16±0,11 2,36±0,10 2,42±0,10 2,71±0,05Zn 188±8 137±8 102±6 78±5 106±6 114±9

124

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Acknowledgements

I would like to thank to Professor Gyula Csom and Professor Zoltán Szatmáry for

giving me the opportunity of performing archaeological studies at the Institute of Nuclear

Techniques. I am grateful for their unflagging attention and support.

I am indebted to my colleagues, Nóra Vajda, Dénes Bódizs, József Szabó, Györgyi

Csuday, Katalin Jovicza, who have contributed in various ways to the production of this

Thesis.

I am particularly grateful to Zsuzsa Molnár, for helping me with her expertise in the

fild of neutron activation analysis, and to László Balázs for the statistical analyses, which

were of vital importance.

Finally, my special thanks go to Jan Gunneweg, wrapped in a text from Qumran

Cave4: “…he will not answer before he hears and he will not speak before he understands.

With patience he will reply and humbly he will express himself. He will seek truth and

justice, and in seeking for the righteousness he will find its origins.” (4Q421)

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