m.baba, m.hagiwara, t.itoga, t.aoki cyclotron & radioisotope center, tohoku university , ...

Measurement of neutron emission spectra and activation in Li,

Be,C,Al,Fe,Ta(d,n) reactions by in the 20-40 MeV region

M.Baba, M.Hagiwara, T.Itoga, T.AokiCyclotron & Radioisotope Center, Tohoku University , Japan

M.SugimotoJapan Atomic Energy Research Institute, Tokai Establishment, Japan

T.Muroga,National Institute for Fusion Research, Toki, Japan

＊＊＊＊ CONTENTS ＊＊＊＊＊＊＊1. Introduction2. Apparatus & Experimental Methods

　　　 3. Results; Neutron spectra & Activation

4. Summary

1. INTRODUCTION

In IFMIF ・ Neutron spectrum extends beyond 50 MeV (High energy

tail)

・ Neutrons show very strong angular dependence ・ Beam intensity is as high as 250 mA

Design & maintenance of IFMIF require the data on 　　・ Energy-angular distribution of (d,n) neutrons; Li, accelerator structural elements 　　・ Production/ accumulation of radioactive nuclides 　　 3H , 7Be, 22Na, 24Na etc

Experimental data were very few and discrepant

INTRODUCTION(2)

７ Li （ d,n) TTY; M. A. Lone et al. Nucl. Instrum. and Methods 143 (1977) 331-344

＊ Large discrepancies, Energy range is limited

In this study

1. Neutron spectrum from thick, thin targets of - Li, Be, C, Al, Fe, Ta 　 - @ 25, 40 MeV - 0-110-deg. ・ Comparison with exp., calculations ・ Systematics vs mass 2. Radio-nuclide production - Li, Be, C, Al, Fe, (Ta) - 7Be, 22Na, 24Na, etc 　　

2. Experimental ApparatusCyclotron & Radioisotope Center, Tohoku University (CYRIC)Performance of

K=110 AVF cyclotron•Protons 10-90

MeV•Deuterons 10-65

MeV•3He 20-170

MeV•4He 20-130

MeV・ Heavy Ions ・ Beam Chopper 　　　etc.

Layout of CYRIC

Automated-irradiation apparatusOnline-mass separator

Semiconductor Irradiation apparatus

Beam swinger

Flight path

Beam chopper

CYRIC TOF Line

Beam-swinger system

Beam-swinger ＆ Well collimated TOF channel

Setup detectors at two locations

Vertical view of neutron course12

5cm

Target

1m

Beam Dump

1m 2.83m

30cm wide20cm high

Polyethylene

iron

5th Target Room TOF Room

Flight Path: 11mFlight Path:3.452m

Concrete

1m

30cm

Scattering Chamber

Beam Swinger

30cm

Bending Magnet

TOF MeasurementTOF Measurement

MCS

Copper Mesh(-500V)

3 parameter list mode・ 2-gain・ 2-flight path

Radio-nuclides production

After TOF measurement, γ-ray measurement with Ge detector　

4-1. SETUP

0 1000 2000100

101

102

103

104

105

106

-ray energy (keV)

Cou

nts

7Be 477.6 keV

4-2. γ-ray spectrum

Ge detectorHV+4000V

Amp

MCA

Sample

γray

19 cm0 1000 2000

100

101

102

103

104

105

106

-ray energy (keV)

Coun

ts

7Be 477.6 keV

deuteron neutron spectrum meas.

TOF data processing

n- discrimination [channel]

Pul

se h

eigh

t [c

hann

el]

n- discrimination [channel]

Pul

se h

eigh

t [c

hann

el]

high-gain raw data low-gain raw data

n-eventn-event -event

-event

Derivation of neutron spectrum

1. n-γdiscrimination2. Bias setting ；～ 0.6 MeV for high-gain, ～ 3.5 MeV for low-

gain3. TOF to energy spectrum

m0 : Rest mass of a neutron

I : Channel number of the eventsL : Flight pathc : Light velocity.

4. Absolute scale ；　 detector efficiency ， solid-angle, current　　　　　　　　　 (SCINFUL-R code).5. Corrections for attenuation in target (air:LA150 ） just stopping length to avoid excessive correction

)(

)(1

1

1)(

2

20

20

2

iTc

L

c

xvcmcmmciE

n

nn

Radionuclide production (1)

n

i

tini

TT eQee

CR

mc

1

)( }{)1(

totalQRN

tI

NA

: decay constant (s-1), C : total counts of gamma-ray peak area, : peak efficiency,Tc : cooling time (s),

: branching ratio of gamma rays,Tm: counting time (s),

Qi : beam current (Coulomb) for irradiation time

interval Dt (s) [using Multi Channel Scaler : MCS]N : number of produced atoms in the target (atom),A : dps/(A·h)I : beam current (A)T : irradiation total time (h)

1) Reaction rate

2) Number of products

3) Activity

0 500 1000 1500100

101

102

103

104

105

Cou

lom

b/1

min

[*1

0-10 ]

channel/1 min

Beam fluctuation with MCS

Energy determination & attenuation correction

ItN

RNQ

d

4) Cross-section

Rdionuclide production (2)

1. Energy of each stack sample-TRIM code

0 5 10 15 20 250

10

20

30

40 dE/dx (deuteron in Li) Energy distribution (deuteron in Li)

Depth (mm)

Ene

rgy

(MeV

)

0 1 210-1

100

Depth (cm)

Att

enat

ion

fact

or

by Shen's emprical formula

1. Attenuation of sample- Shen’s empirical formula

3. Results & Discussion

1. Neutron spectrum; 0~110-deg. ・ Li, Be Ed= 25 MeV thick, thin (Li) Ed= 40 MeV thick, thin (Li) ・ C, Al, Fe, Cu, Ta, W Ed= 40 MeV thick

2. Radionuclide production Target: Li, C, Al, Fe, Ta, W Nuclides; 7Be, 22Na, 24Na,

0 10 20 30 40105

106

107

108

109

1010

1011

Present Ed=25MeV 0deg

M.A.Lone et al. Ed=23MeV 0deg

Neu

tron

Yie

ld [

MeV

-1・

sr-1・

C-1

]

Neutron Energy [MeV]

Comparison with Lone’s data natLi(d,xn) 0-deg for 25 MeV

0 10 20 30 40 50104

105

106

107

108

109

1010

1011

Neutron energy [MeV]

Neu

tron

yie

lds

[MeV

-1sr

-1C

-1]

natLi(d,xn) spectra

0-deg 5-deg 10-deg 15-deg 20-deg 25-deg 30-deg 40-deg 60-deg 90-deg

natLi(d,xn) Ed = 25 MeVThick lithium

0 10 20 30 40 50106

107

108

109

1010

1011


Neu

tron

flu

x [#・

MeV

-1・

sr-1・

C-1

]

0-deg 10-deg 15-deg 20-deg 30-deg 45-deg 60-deg 90-deg 110-deg

0 10 20 30 40 50105

106

107

108

109

1010


Neu

tron

flu

x [#

・M

eV-1・

sr-1・

C-1

]

0-deg 10-deg 15-deg 20-deg 30-deg 45-deg 60-deg 90-deg 110-deg

thick natLi(d,xn) for Ed= 40 MeV [7Li(d,n) Qvalue=+15.0 MeV]

thin natLi(d,xn) for Ed= 40 MeV [7Li(d,n) Qvalue=+15.0 MeV]

natLi(d,xn) Ed = 40 MeV Thick and thin lithium

0 10 20 30 40 50104

105

106

107

108

109

1010

1011


Neu

tro

n y

ield

s [M

eV-1sr

-1C

-1]

natLi(d,xn) spectra


natLi(d,xn) [7Li(d,n) Q 値 =+15.0

MeV]

0 10 20 30 40 50104

105

106

107

108

109

1010

1011


Neu

tro

n y

ield

s [M

eV-1sr

-1C

-1]


natBe(d,xn) [9Be(d,n) Q 値 =4.36 MeV]

Li; comparison with exp. & calculation

0 10 20 30 40 50106

107

108

109

1010

1011


Neu

tron

flux

[#・

MeV

-1・

sr-1・

C-1

]

Present (0-deg) F.M. Mann et al McDeli McDeliciuos MCNPX

0 10 20 30 40 50106

107

108

109

1010

1011


Neu

tron

flu

x [#

・M

eV-1・

sr-1・

C-1

]

Present (20-deg) F.M. Mann et al McDeli McDeliciuos MCNPX

Neutron yields

0 10 20 30 40109

1010

1011

1012

Deuteron Energy [MeV]

Neu

tron

Yie

ld [

#・sr

-1・

C-1

]

Forward ( = 0 deg)

Present Aoki et al. Daruga et al. Weaver et al. Goland et al. Amols et al. Nelson et al. Lone et al. Salmarsh et al. Johnson et al. Sugimoto et al. MCDeLicious cal. MCDeLi cal. MCNPX cal.

1010

1011

Neu

tron

Yie

ld [

#・C

-1]

Present Aoki et al. Lone et al. Johnson et al. Sugimoto et al. Mann et al. MCDeLicious cal. MCDeLi cal. MCNPX cal.

Total ( = 4)

4π-integrated

0 ゜ - differential

0 10 20 30 40105

106

107

108

109

1010


Neutron Energy (MeV)

Neu

tron

Flu

x (#

・M

eV-1・

C-1・

sr-1

)

Li(d,n) 25 MeV neutron spectra

0 10 20 30 400

0.2

0.4

0.6

0.8

1[109] EXP 0-deg Ext-Serber model Serber model


Neu

tron

Flu

x (#

・M

eV-1・

C-1・

sr-1

)

7Li(d,n)8Be exitation level

7Li(d,n)8Be G.R.

Li(d,n) 25 MeV at 0 deg

D 25 MeV thin spectra: Serber / Advanced Serber model *

* H.Utsunomiya (MSU); Phys. Rev., C32 (1985) 32

0 10 20 30 40 500

1

2

3[109] EXP 0-deg Ext-Serber model Serber model


Neu

tron F

lux

(#・M

eV-1・

C-1・

sr-1)

Li(d,n) 40 MeV at 0-degree

7Li(d,n)8Be G.R.

7Li(d,n)8Be exitation level

D 40 MeV thin spectra: Serber / Advanced Serber model

natC(d,xn) ， 27Al(d,n) spectra

0 10 20 30 40 50105

106

107

108

109

1010

Neu

tron

yie

lds

[#・

MeV

-1・

sr-1・

C-1

]



0 10 20 30 40 50105

106

107

108

109

1010

Neu

tron

yie

lds

[#・

MeV

-1・

sr-1・

C-1

]



ＣＡ

ｌ

Fe, Ta(d,n)

0 10 20 30 40 50102

103

104

105

106

107

108

109

1010

0 10 20 30 40 50102

103

104

105

106

107

108

109

1010

natTa(d,n)

Neu

tron F

lux [#/

(MeV

·sr·

C)]


natFe(d,n)

00 deg. 05 deg. 15 deg. 30 deg. 60 deg. 90 deg. 110 deg.

Fe, Ta(d,n): comparison

0 10 20 30 40104

105

106

107

108

109

1010

0 10 20 30 40102

103

104

105

106

107

108

109

1010

Meulders et al., Ed =33 MeV

Neu

tron

Flu

x [#

/(M

eV·s

r·C

)]


Meulders et al., Ed =50 MeV

present Ed = 40 MeV

Ta(d,n) at 0 degree

15 deg.


Line : Shin et al., Ed=33MeV, Cu(d,n)Symbol : present, Ed=40 MeV, Fe(d,n)

0 deg.

J. P. Meulders, et al., Phys. Med. Biol., 20, (1975) 235-243K. Shin, et al., Phys. Rev. C, 29, (1984) 1307-1316

0.5 1 5 10 5010-1

100

101

102

103

104

105

106

107

108

109

1010

1011

15 deg

Ta Fe C Al Li

Neu

tro

n F

lux

[#

/(MeV

·sr·C

)]


0 deg.

Cross-section systematics vs mass

(d,n) @Ed=40MeVLi(d,n) :

largest yieldsC(d,n) :

yield is larger than heavy element

M. Hagiwara, et al., J. Nucl. Materials, 329-333, (2004) 218-222

M. Hagiwara, et al., J. Fusion Sci. Tech., in print

Spectrum mass-dependence

・ Spectrum becomes softer with mass

1 2 3 4 5

109

1010

Fe

C

Al

Ta

Neu

tro

n F

lux

[#

/(M

eV·s

r·C)]


Li

M. Hagiwara, et al., J. Nucl. Materials, 329-333, (2004) 218-222

M. Hagiwara, et al., J. Fusion Sci. Tech., in print

Comparison with MCNPX; Fe, Ta

104

105

106

107

108

109

Fe, 60 deg.

104

105

106

107

108

109

Fe, 110 deg.

0 10 20 30 40 50104

105

106

107

108

109

MCNPX present exp.

Ta, 0 deg.

Neu

tron

Flu

x [#

/(M

eV·s

r·C

)]

0 10 20 30 40 50

Ta, 110 deg.

Neutron energy [MeV]0 10 20 30 40 50

104

105

106

107

108

109

Ta, 110 deg.

Fe, 0 deg.

Radionuclide production

0 10 20 30 40 500

20

40

60

80

100

Deuteron Energy (MeV)

Cros

s Sec

tion

(mb)

PresentIRACM XS fileB.Ja.Guzhovskij et al.O.N.Vysotskij et al.

0 10 20 30 40104

105

106

107


dps

μ・

A-1

・ho

ur-1

Presentdata with present XSU.Von Möllendorff et al.S.Mukhammedov et al.P.P.Dmitriev et al.IRACM calculation

natLi(d,x)7Be activation cross-section ， natLi(d,x)7Be activity (TTY)

lithium (IFMIF target) Ed= 40, 38.6, 29.7, 28.2, 19.7, 17.7, 10, 7.05 MeVnatLi(d,x)7Be activation cross-section natLi(d,x)7Be activity (TTY)

natC(d,x)7Be

27Al(d,x)7Be 　

・ PHITScode・ other exps.

20 30 40 500

2

4

6

8

10

Deuteron Energy (MeV)C

ross

Sec

tion

(m

b)

PresentPHITS calc.

20 30 40 500

0.1

0.2

0.3

0.4

0.5

0.6


Cro

ss S

ecti

on (

mb)

PresentU.Martens et al.PHITS calc.

・ PHITS code (JQMD and GEM)

27Al(d,x)24Na

27Al(d,x)22Na

0 10 20 30 40 500

20

40

60

80

Deuteron Energy (MeV)C

ross

Sec

tion

(m

b)

PresentIAEA recomendS.Takacs et al.U.Martens et al.PHITS calc.

20 30 400

10

20


Cro

ss S

ecti

on (

mb)

PresentIAEA recomendS.Takacs et al.U.Martens et al.PHITS calc.

・ PHITS code・ Other Exps.・ Recommendation

・ PHITS code・ Other Exps.・ Recommendation

27Al(d,x)24Na activity (TTY)

27Al(d,x)22Na activity (TTY)

・ compare with IAEA data

Estimation

・ compare with IAEA

10 20 30 40104

105

106

107

108

109

1010


dpa・

A-1・

hour

-1

Al(d,x) 24Na Present estimationAl(d,x) 24Na Estimation with IAEA dataC(d,x)7Be Present estimationAl(d,x) 24Na Present TTYC(d,x)7Be Present TTY

20 30 40101

102

103

104


dpa・

A-1・

hour

-1Al(d,x) 22Na Present estimationAl(d,x) 22Na Estimation with IAEA dataAl(d,x) 7Be Present estimationAl(d,x) 22Na Present TTYAl(d,x) 7Be Present TTY

27Al(d,x)7Be activity (TTY)

natC(d,x)7Be activity (TTY)

Fe Activation cross-section (I)

natFe(d,x)51CrnatFe(d,x)52Mn

*TALYS is a nuclear reaction program using update code parameter created at NRG Petten.

0 10 20 30 40 5010-3

10-2

10-1

100

101

102

present 51Cr A. Hermanne et al. J. W. Clark et al. TALYS

Cro

ss s

ecto

n [m

b]

0 10 20 30 40 5010-3

10-2

10-1

100

101

102

present 52Mn A. Hermanne et al. Zhao Wenrong et al. TALYS

Deuteron energy [MeV]

Fe Activation cross-section (II) 　

natFe(d,x)56Co

natFe(d,x)57ConatFe(d,x)58Co

0 10 20 30 40 50100

101

102

present 56Co J. W. Clark et al. Zhao Wenrong et al. P. Jung IAEA recommend TALYS

Cro

ss s

ecti

on [

mb]

0 10 20 30 40 50

present 57Co A. Hermanne et al. J. W. Clark et al. S. Takacs et al. TALYS

Deuteron energy [MeV]

0 10 20 30 40100

101

102 present 58Co J. W. Clark et al. Zhao Wenrong et al. TALYS

Summary & Future

1.Measurements of neutron spectrum for (d,nx) reactions 1) Li ， Be, C ， Al ， Fe ， Cu ， Ta 　 - Ed=40, 25 MeV, - 0 ～ 110 deg

- Energy spectrum shape was clarified, high energy tail 2) Systematics vs target mass

2. Production yields of radio-nuclides via (d,x) reaction 1) Li ， C ， Al ， Fe ， Cu ， Ta

Provided data base for IFMIF optimization & post irradiation analysis

Future program: Deuteron induced reactions & neutron induced reactions

* CDCC (Continuum-discritized coupled-channel) model; BRC * Extended Serber model ?

CYRIC new neutron course (@TR3 extension)

Ep = 50 MeV, E = 2 MeV mono-E n flux 106 n/cm2sA

beam dump7Li(p,n)

74 cm

3~100 Ap beam

• Software error rate• n-induced activation, reaction few-body reactions, etc.

0 20 40 60 800

1

2


Neu

tron

yei

ld [

sr-1

MeV

-1C

-1] [× 109]

En=75 [MeV] En=65 [MeV] En=55 [MeV]

Reference [1] IFMIF CDA TEAM, IFMIF Conceptual Design Activity Final Report edited by Marcello Martone, Report 96.11,

Enea, Dipartimento Energia, Frascati (1996) [2] M.A.Lone et al., Nucl. Instrum. Methods, 143 (1977) 331 [3] M. Baba, T. Aoki, M. Hagiwara et al., J. Nucl. Materials 307-311 (2002) 1715-1718. [4] T. Aoki, M. Hagiwara, M. Baba et al., J. Nucl. Sci. and Tech. to be published [5] A.Terakawa et al., Nucl. Instrum. Methods A 491 (2002) 419. [6] M. Baba, H. Wakabayashi, M. Ishikawa, T. Ito and N. Hirakawa, J. Nucl. Sci. Technol., 27(No.7), 601 (1990) [7] T. Aoki , M. Baba, S. Yonai, N. Kawata, M. Hagiwara, T. Miura, T. Nakamura, Nucl. Sci. Eng., in print [8] J. F. Ziegler, J. P, Biersack, U. Littmark, Pergamon Press, New York (1984). [9] S.Meigo Nucl. Instrum. Methods in Physics Research A 401 (1997) 365 [10] M. B. Chadwick, P. G. Young et al., Nucl. Sci. Eng. 131, 293, 1999 [11] W.Nelson, H.Hirayama, D.W.O.Rogers, “The EGS4 Code System” SLAC-265, Stanford University, Stanford

(1985) [12] W. Q. Shen, B. Wang, J. Feng, W. L. Zhan, Y. T. Zhu and E. P. Feng, Nucl. Phys. A, 491, 130 (1989) [13] J. P. Meulders et al. Phys. Med. Biol., 20, p.235, 1975 [14] Z. Radivojevic, A. Honkanen, J. Aysto, V. Lyapin, V. Rubchenya, W. H. Trzaska, D. Vakhtin and G. Walter, Nucl.

Instr. and Meth. B., 183, p.212, 2001 [15] S.P.Simakov, U.Fisher, U.von Mllendorf, I.Schmuck, A.Yu.Konobeev, Yu. A. Korvin, P.Pereslavtsev; J. Nucl.

Materials, 307-311 1710-1714 (2002) [16] S. Takacs, F. Szelecsenyi, F. Tarkanyi, M. Sonck, A. Hermanne, Yu. Shubin, A. Dityuk, M.G. Mustafa, Z.

Youxiang, Nucl. Instr. and Meth. B., 174 (2001) 235-258 [17] U. Martens and G. W. Schweimer, Zeitschrift für Physics 233 (1970) 170 [18] IAEA, Charged-particle cross section database for medical radioisotope production http://www-nds.iaea.org/medical/ [19] H. Iwase, K. Niita, T. Nakamura, J. Nucl. Sci. Tech. 39, No.11, 1142 (2002)

Differential TTY of natC: 12C(p,n), 13C(p,n)　

　　　　　　　

0 10 20 30 40 50102

103

104

105

106

107

108

109

1010

1011

1012

1013

1014


Neu

tro

n y

ield

s [M

eV-1sr

-1C

-1]

Points :PresentSolid line:LA150

0-deg*1000 15-deg*100 30-deg*10 45-deg 60-deg*0.1 90-deg*0.01

1.E+02

1.E+03

1.E+04

1.E+05

1.E+06

1.E+07

1.E+08

1.E+09

1.E+10

1.E+11

0 10 20 30 40 50 60 70

Energy [MeV]

Neut

ron

Yie

ls [

neut

ron/

MeV

/sr/

μC]

LA150_0 deg.× 100LA150_30 deg.× 10LA150_60 deg.× 1 LA150_90 deg.× 0.1LA150_110 deg.× 0.010 deg.× 10030 deg.× 1060 deg.90 deg.× 0.1110 deg.× 0.01

Ep=50 MeV

Ep=70 MeV

・ Scarcity of experimental data for whole spectrum

　　　　　　“ Measurement of full energy range ”・ Target: 30-mm-diam x full stop thickness 　 0-110 deg.,・ Efficiency; SCINFUL-R Correction; Attenuation in target, air・ Comparison with LA-150

3. Differential TTY (Thick target neutron yield) 　

'/exp

/

00

0

002

02

dtdtdtdEEN

dEd

dtdtdEEdN

dEd

EYd

t

t

nonel

T

t

TTY: W(p,n)

0 10 20 30 40 50102

103

104

105

106

107

108

109

1010

1011

1012

1013

1014


Neu

tron

yie

lds

[MeV

-1sr

-1C

-1]

natW(p,xn) spectraPoints :PresentSolid line:LA150

0-deg*1000 15-deg*100 30-deg*10 45-deg 60-deg*0.1 90-deg*0.01

1.E+04

1.E+05

1.E+06

1.E+07

1.E+08

1.E+09

1.E+10

1.E+11

1.E+12

1.E+13

0 10 20 30 40 50 60 70

Energy [MeV]

Neut

ron

Yiel

s [n

eutr

on/M

eV/s

r/μ

C]

0 × 100度30 × 10度60 × 1度90 × 0.1度110 × 0.01度LA150_0 × 100度LA150_30 × 10度LA150_60 × 1 度LA150_90 × 0.1度LA150_110 × 0.01度

Ep=50 MeV Ep=70 MeV

0.1

1

10

100

0 10 20 30 40 50 60 70 80 90


Cro

ss s

ecti

on [

mb]

14N(n,2n)13NPHITSINC/ GEMEXFOR dataENDF/ B- VI

0.1

1

10

100

0 10 20 30 40 50 60 70 80 90


Cross s

ectio

n [

mb]

16O(n,2n)15OPHITSINC/ GEMEXFOR dataENDF/ B- VI

Neutron-induced activation X-section

1. はじめに (4)

目　的1. IFMIF 加速器構成材核種の（ d,n) 中性子スペクトルの測定　　・ Li, C, Al, (Fe, Cu) ・ Ed=25- 40 MeV, 0 – 90 ゜・厚いターゲット，薄いターゲット　　・スペクトルの全範囲の測定

2. IFMIF 加速器構成材核種と重陽子反応による放射性核種生成　　・ Li, C, Al, (Fe, Cu)　・厚いターゲット，薄いターゲット・スタックターゲット法による励起関数の導出　　・ 7Be, (3H), , 24Na, 24Na 　　

3. 実験

１．東北大学サイクロトロン　　・第五ターゲット室，　　・ビームチョッパー　　・ビームスウィンガー＋飛行管室；　　　　　高いエネルギー分解能，　 S/N 比，広いスペクト

ル範囲

2. スタックターゲットの利用　　・厚いターゲットと薄いターゲットの対する同時測定　　・中性子スペクトル，放射化の同時測定

INTRODUCTION(2) 　

n+28Si (LA150)

m.baba, m.hagiwara, t.itoga, t.aoki cyclotron & radioisotope center, tohoku university , ...

Documents

ifmif neutron spectrum

mev thick

n neutrons li

energy spectrum m0

mev high energy tail

mev region

energy range

radionuclide production