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  • 8/10/2019 Enriched bomb uranium isotope ratios from Oak Ridge Oralloy

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    Diatrilnati01l:

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    DISCLAIMER

    This report was prepared as an account of work sponsored by anagency of the United States Government. Neither the United StatesGovernment nor any agency Thereof, nor any of their employees,makes any warranty, express or implied, or assumes any legalliability or responsibility for the accuracy, completeness, orusefulness of any information, apparatus, product, or processdisclosed, or represents that its use would not infringe privatelyowned rights. Reference herein to any specific commercial product,process, or service by trade name, trademark, manufacturer, orotherwise does not necessarily constitute or imply its endorsement,recommendation, or favoring by the United States Government or anyagency thereof. The views and opinions of authors expressed hereindo not necessarily state or reflect those of the United StatesGovernment or any agency thereof.

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    DISCLAIMER

    Portions of this document may be illegible inelectronic image products. Images are producedfrom the best available original document.

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    2

    TABLE

    OF

    CONTENTS

    INTRODUCTION

    ...................

    5

    EXPERIMENTALLY

    DETERMINED

    DOSE KATE

    3

    CALCULATED

    DOSE

    RATE

    4

    ABSORBED

    DOSE

    IN

    PLASTICS

    6

    GAI4A

    DOSE RATE

    ..................

    7

    CONCLUSIONS

    ....................

    9

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    IrRODUCTION

    Oralloy

    (enriched

    uranium)

    is

    a

    potential

    source

    of

    radiation

    damage

    because

    of

    its

    alpha

    and

    gamma

    radioactivity.

    The

    radiation

    effects

    will

    be

    relatively

    small

    because

    of

    the

    low

    specific

    activity.

    However,

    the

    long

    design

    lifetimes

    (many

    years)

    of

    some

    materials

    could

    lead

    to

    appreciable

    damage.

    To

    estimate

    this damage,

    the

    dose rate

    from

    the

    surface

    of

    oralloy

    must

    be

    determined.

    This

    has

    been

    done experimentally

    and

    theoretically.

    The isotopic

    composition

    of oralloy

    used

    at

    Rocky Flats,

    as

    determined by

    mass spectrometry,

    is

    the

    ollowing.

    U-24

    1.01

    U-23S

    93.13

    U-236

    0.32t

    U-238

    S.SSt

    EXPERIMENTALLY

    DETERMINED

    DOSE

    RATE

    Radioactive counting

    techniques

    were

    used

    to

    measure

    the

    dose

    rate

    from orallov.

    A

    counting

    source

    was fabricated

    by machining

    an

    oralloy

    disc

    (diameter

    1/4

    inch

    and thickness

    1/16 inch)

    which

    fit

    exactly

    into

    the

    machined

    depression

    of

    an

    almainu

    disc

    (di--eter-

    1

    inch

    and thickness

    1/8 inch).

    The

    top

    of

    the

    oralloy was flush with the aluminum surface

    so

    that

    only

    the

    top

    surface

    Carea

    0.316

    cm

    z

    would

    be

    counted.

    Since

    the

    range

    of the

    alpha particles

    in

    oralloy

    is about

    6

    microns,

    this

    is an

    infinite

    source.

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    4

    Results

    obtained

    from

    a

    machined

    or

    polished

    surface

    were

    essentially

    the

    same.

    The

    total

    alpha disintegration

    rate,

    measured

    with

    a

    proportional

    counter,

    was

    151,680

    +/-225

    counts

    per

    minute.

    The average alpha

    energy

    was

    determined

    using

    a

    silicon

    surface

    barrier

    detector

    coupled

    to

    a

    pulse

    height

    analyzer.

    Integration

    under

    the

    resulting

    spectrum

    gave

    an

    average energy

    of

    2.69

    MeV,

    which

    is

    56t

    of the

    maximum

    energy.

    s

    Multiplying

    the

    count rate

    by

    the

    average

    energy

    gives

    an

    alpha

    dose rate of 2.15 x 101

    eV

    per

    second

    per

    cm

    z

    CALCULATED

    DOSE

    RATE

    The

    following

    properties

    of

    the

    uranium

    isotopes

    were

    used.

    half life

    alpha energy

    ramie

    in

    alr

    z

    U-34

    2.47xi0

    years

    4.76

    MeV

    4.00

    ag/cm=

    U-235

    7.1

    xlO

    e

    years

    4.40

    MeV

    3.50

    mg/cm

    U-238

    4.51x10

    years

    4.18 14eV

    3.25

    mg/cm

    U-236 2.34x107

    years

    4.49

    eV

    The dose

    contributions

    from

    uranium-2 8

    and

    -236

    were

    considered

    and

    found

    to

    be

    negligible.

    The dose rate wa

    calculated

    by

    multiplying

    the

    alpha particle

    flux

    by

    the

    average

    energy

    of

    the

    emergent particles. The

    particle

    flux

    (n)

    calculated

    according

    to:

    *

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    5

    n

    sp

    k

    x

    R/4

    where

    sp

    A

    specific

    activity

    (disintegrati

    per

    second

    per

    R

    range

    The

    rahge

    was calculated

    according

    to:

    R

    z/0.01

    Z/z

    R

    a

    [0.90/

    0.0275

    Z/

    (0.06-

    0.0086

    Z) log

    where

    R

    z

    range,

    mg/cm

    2

    R

    a

    range

    in

    air

    Z

    atomic number

    of

    element

    z tomic

    number

    of

    particle

    E

    particle

    energy

    in

    MeV

    M mass

    number of

    particle

    The flux

    and

    range

    (dividing

    R

    z

    by

    18.81,

    the

    density

    of

    oralloy,

    gives

    the

    range in cm)

    of

    alpha

    particles

    from

    uranium-254 and

    -235

    are:

    n

    R

    z

    R

    U-254 7.48x10

    /sec/cm

    2

    15.I

    mg/cm

    2

    6.96x10

    .4

    cm

    U-255

    2.28x102

    /sec/cm

    2

    11.4

    mg/cm

    2

    6.08x10

    .4

    ca

    The

    average

    energy

    was

    taken to

    be

    2/3

    of the

    maximum

    energy.

    This

    value was derived

    using

    an

    approximation

    of

    the

    Bethe-Block

    equation.

    (s

    1/2

    E

    11

    where

    E

    energy

    of

    the

    particle

    E

    o

    initial

    particle

    energy

    r distance

    particle

    travels

    R

    particle

    range

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    6

    The

    average

    energy

    is defined

    as

    f

    Edr

    divided

    by

    f

    dr.

    o

    The

    dose

    rates

    fromU-Z34and

    U-Z3

    in

    oralloy were

    thereby

    determined

    to

    be:

    U-254

    2.57x1012

    eV/sec/cm

    2

    U-255

    6.68x108

    eV/sec/cm

    The

    dose rate from

    oralloy

    is the

    weighted

    average

    rom these

    two

    isotopes.

    2.37x10

    (1.01t)

    /

    6.68x10

    (95.15)

    2.45xI0s

    V/sec/cm

    This

    value

    is

    a little

    larger

    than

    the

    measured

    dose

    (2.15

    x

    10

    I

    eV/sec/cm

    )

    because

    of

    the

    difference

    in the

    average

    alpha

    energies.

    The measured

    energy

    was

    6

    of

    the

    maxim,,=

    energy

    and

    the theoretical

    energy

    (using

    an

    approximate

    calculation)

    was

    66.6t

    of

    the

    maximum

    energy.

    ABSORBED DOSE

    IN

    PLASTICS

    To

    assess

    the

    radiation

    damage upon

    prolonged exposure

    from

    oralloy,

    a calculation

    has been

    made

    using

    polyethylene as

    a

    representative

    plastic.

    The

    first

    step

    was to calculate

    the

    range

    of

    the

    alpha

    particles

    in

    polyethylene,(CH2)x.

    The

    assumption was

    made

    that

    the

    plastic

    is in

    contact

    with

    the

    oralloy

    so

    that

    the

    average

    particle

    energy

    is

    still

    2.69

    MeV.

    Ranges

    in

    hydrogen

    and

    carbon

    were

    calculated

    using equations

    similar

    to

    the one

    used

    previously in

    this

    report,

    r

    The

    ranges

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    7

    are

    0.51 mg/ca

    and

    1.75

    ag/ca

    2

    for

    hydrogen

    and

    carbon,

    The

    range

    in

    polyethylene

    was calculated

    espectively.

    according

    to:

    -,1

    0. S7

    0.143

    gC,)

    x

    /

    *weight

    fraction of element

    in

    CCH2)

    x

    The

    range

    was 1.30

    ag/ca

    2

    or ..:x10

    .3

    ca.

    The

    absorbed dose

    can

    thereby

    be

    calculated

    I

    radl0

    eY/gl( :3 lSxlO

    secl

    .15x101

    eV/sec/ca

    6 Z

    4

    ose

    1. :30

    x

    10-

    3

    g/ca

    x

    -e

    8.:3

    x

    10

    s

    fads/year

    This is

    the

    approximate

    dose at

    which

    polyethylene

    and

    uny

    other

    plastics

    start

    to

    decompose.

    The

    damaging

    dose

    is

    greatly variable

    and

    depends

    on

    the

    plastic

    as

    well

    as

    the

    property

    of

    interest.

    Nevertheless,

    it

    appears

    that

    many

    organic

    materials w111

    undergo

    significant

    decomposition

    in

    a

    few

    years

    of

    contact with

    oralloy.

    However, these

    effects will

    only occur to a

    depth

    of

    approxi-

    aately

    1-2x10

    .3

    ca.

    GA}@4A

    DOSE

    RATE

    Instrumentation

    was

    not available

    to

    measure

    the

    gam

    dose

    rate

    from

    oralloy,

    but

    a

    rough

    approximation

    was

    calculated for

    coapari-

    son with

    the

    alpha

    dose

    rate.

    Decay schemes

    for

    uranium-2:34

    and

    -2:35

    show the

    following:

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    U-234

    specific

    activity

    4.30xI0

    dis/sec/cm

    s

    72

    of

    decays

    to

    ground

    28

    of

    decays

    0.053

    MeV gamma ray

    U-235

    specific activity

    i. 0x10

    dis/sec/cm

    2

    75.8

    o

    decays

    a

    spectrum

    of

    gamma

    rays

    with

    an

    average energy

    of 0.18 MeV

    The

    absorption

    coeficients

    (

    and

    half

    thickness for these

    gamma

    rays in

    oralloy

    are:

    ulP

    Ccm21e)

    Cc

    )

    0.053

    MeV

    9.86

    185

    0.18 MeV

    1.79

    33.6

    Half thickness

    (ca)

    3.74

    x

    I0

    2.06

    x

    10

    .2

    For the

    dose

    rate

    approximation,

    assume

    that

    one-half

    (g

    ometry

    factor)

    of 811

    the

    gamma

    energy

    is

    released

    from

    a

    half thickness

    o

    oralloy.

    U-234 4.30x10

    dis

    13.74x10

    ec

    ca

    Dose 1.19

    x

    I0

    eV/sec/cm

    2

    (0.28)(0.50)(5.3x10

    s

    /

    dis

    U-235

    1.SO

    x

    10

    [2.06

    x

    10

    sec

    Dose

    2.19xl0

    s

    eV/sec/cn

    2

    c= w/

    (0.788) (0.

    so)

    1.8xlO

    s

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    -9-

    The total dose

    rate from

    oralloy

    is

    the

    weighted

    average.

    11

    t

    U-234

    1.01t

    (1.19

    x

    10

    1.20

    x

    10

    37.0t of

    energy

    9

    9

    U-235 95.13t (2.19

    x

    10

    2.04

    x

    10

    63.0t

    of

    energy

    Total dose

    rate 5.24

    x

    10

    eY/sec/cm

    a

    Not

    only

    is

    the

    gamma

    dose

    rate

    almost an order

    of

    magnitude

    less

    than

    the

    alpha

    dose

    rate,

    but

    the

    gamma

    penetration

    (half

    thickness)

    in

    plastics

    is

    about

    a

    thousand

    times

    that

    of

    alpha

    penetration,

    so

    that

    the

    absorbed

    dose

    from

    gamma

    radiation is

    negligible

    compared to

    that

    from

    alpha

    radiation.

    CONCLUSIONS

    The

    alpha

    dose

    rate

    from

    the

    surface

    of

    oralloy

    was

    determined

    10

    10

    to

    be 2.15

    x 10

    eV/sec/cm

    2

    (or

    2.45

    x 10

    eV/sec/cm

    2

    clculated

    value). Almost all

    of

    the

    dose

    emanates

    from

    uranlua-234, whose

    isotopic

    concentration

    is

    1.01t. The

    absorbed

    dose

    in

    poly-

    ethylene

    was

    calculated

    to

    be

    8.5

    x

    10

    fads/year

    indicating

    that

    most

    plastics

    would

    radiolytically

    decompose

    appreciably

    in

    a

    few

    years.

    However,

    the

    decomposition

    would

    only

    occur

    to

    a

    depth

    of

    1-2 x

    10

    s

    cm,

    the

    alpha

    partlcle

    range.

    The

    gma

    dose

    rate

    was

    also

    estimated

    and

    found to

    be

    negligible

    compared

    to

    the

    alpha dose

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    10

    REFERENCES

    I.

    The

    counting

    was done

    by

    Richard Murri

    of

    the

    Rocky

    Flats

    Environmental

    Science

    Group

    G.

    Friedlander,

    J.

    W.

    Kennedy,

    and

    J.

    M.

    Miller,

    Nuclear

    and

    Radiochemistry,

    John

    Wiley

    and

    Sons,

    New

    York,

    1964,

    page

    96.

    5. G.

    D.

    Finney

    and R.

    D.

    Evans,

    Physical Review, 48,

    505

    (1935).

    G.

    Friedlander,

    J. W.

    Kennedy,

    and

    J.

    M.

    Miller,

    Nuclear

    and

    Radiochemistry,

    John

    Wiley

    and

    Sons,

    New

    York, 1964,

    page

    95.

    S.

    M.

    McD.

    Baker,

    R.

    Hughes,

    J. A.

    Spooner,

    ACO/UK-2325,

    October 1964.

    J.

    H.

    Hubbell,

    Photon Cross

    Sections,

    Attenuation

    Coefficients,

    and

    Energy

    Absorption

    Coefficients

    from

    10 keV to 100

    GeV,

    NSRDS-NBS

    29, August

    1969.