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Measurements at n_TOF of the neutron capture cross section of minor actinides relevant to the nuclear waste transmutation

Abstract

Accurate and reliable neutron-capture cross-section data for actinides are necessary for the proper design, safety regulation, and precise performance assessment of transmutation devices such as Fast Critical Reactors or Accelerator Driven Systems. In particular, the neutron-capture cross sections of 237Np, 240Pu, and 243Am play a key role in the design and optimization of a strategy for the Nuclear Waste Transmutation. The listed cross sections have been measured in 2004 at n_TOF with a high accuracy due to a combination of features unique in the world: high instantaneous neutron fluence and excellent energy resolution of the n_TOF facility, innovative Data Acquisition System based on flash ADCs, and the use of a high-performance BaF2 Total Absorption Calorimeter as a detection device.

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Measurements at n_TOF of the neutron capture cross section of minor actinides relevant to the nuclear waste transmutation

Author: Cano-Ott, D.; Abbondanno, U.; Aerts, G.; Capote del Villar, Ramón; Lozano Leyva, Manuel Luis; Quesada Molina, José Manuel; Wisshak, K.
Publisher: American Institute of Physics
Year: 2005
DOI: 10.1063/1.1945275
Source: https://idus.us.es/bitstreams/d0153175-2f80-4c43-9ecd-684fa6cf8ae8/download
Measu emen s a n_TOF o he Neu on
Cap u e C oss Sec ion o Mino
Ac inides Rele an o he Nuclea Was e
T ansmu a ion
Ci e as: AIP Con e ence P oceedings 769, 1442 (2005); h ps://doi.o g/10.1063/1.1945275
Published Online: 13 June 2005
D. Cano-O , U. Abbondanno, G. Ae s, H. Ál a ez, F. Àl a ez-Vela de, S. And iamonje, J. And zejewski, P.
Assimakopoulos, L. Audouin, G. Badu ek, P. Baumann, F. Beč ář, J. Benlliu e, E. Be houmieux, F. Cal iño,
R. Capo e, A. Ca illo de Albo noz, P. Cennini, V. Chepel, E. Chia e i, N. Colonna, G. Co es, D. Co ina, A.
Cou u e, J. Cox, S. Da id, R. Dol ini, C. Domingo-Pa do, W. D idi, I. Du an, M. Embid-Segu a, L. Fe an ,
A. Fe a i, L. Fi zpa ick, R. Fe ei a-Ma ques, H. F ais-Koelbl, K. Fujii, W. Fu man, I. Goncal es, R. Gallino,
E. Gonzalez-Rome o, A. Go e do ski, F. G amegna, E. G iesmaye , C. Gue e o, F. Gunsing, B. Haas, R.
Haigh , M. Heil, A. He e a-Ma inez, M. Igashi a, S. Isae , E. Je icha, Y. Kadi, F. Käppele , D. Ka amanis, D.
Ka adimos, M. Ke eno, V. Ke le o , P. Koehle , V. Kono alo , E. Kossionides, M. K ička, C. Lamboudis,
H. Leeb, A. Lindo e, I. Lopes, M. Lozano, S. Lukic, J. Ma ganiec, L. Ma ques, S. Ma one, P. Mas inu, A.
Mengoni, P. M. Milazzo, C. Mo eau, M. Mosconi, F. Ne es, H. Obe humme , S. O’B ien, M. Oshima, J.
Pancin, C. Papach is odoulou, C. Papadopoulos, T. Papae angelou, C. Pa adela, N. Pa onis, A. Pa lik,
P. Pa lopoulos, G. Pe dikakis, L. Pe o , R. Plag, A. Plompen, A. Plukis, A. Poch, C. P e el, J. Quesada,
T. Rausche , R. Rei a h, M. Rose i, C. Rubbia, G. Rudol , P. Rullhusen, J. Salgado, L. Sa chiapone, C.
S ephan, G. Taglien e, J. L. Tain, L. Tassan-Go , L. Ta o a, R. Te lizzi, G. Vannini, P. Vaz, A. Ven u a, D.
Villama in, M. C. Vincen e, V. Vlachoudis, R. Vlas ou, F. Voss, H. Wendle , M. Wiesche , K. Wisshak, and
The n_TOF Collabo a ion
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© 2005 Ame ican Ins i u e o Physics.
Measu emen s a n_TOF o he Neu on Cap u e C oss
Sec ion o Mino Ac inides Rele an o he Nuclea Was e
T ansmu a ion
D. Cano-O 20 1
, U. Abbondanno14,G.Ae s
7,H.Ál a ez
24, F. Àl a ez-Vela de20, S. And iamonje7,
J. And zejewski33, P. Assimakopoulos9, L. Audouin 5G. Badu ek1,P.Baumann
6,F.Beˇc ᡠ31, J. Benlliu e24,
E. Be houmieux7, F. Cal iño25, R. Capo e23, A. Ca illo de Albo noz30, P. Cennini4, V. Chepel17,E.Chia e i
4,
N. Colonna13,G.Co es
25,D.Co ina
24, A. Cou u e29,J.Cox
29,S.Da id
5,R.Dol ini
15, C. Domingo-Pa do21,
W. D idi7,I.Du an
24, M. Embid-Segu a20,L.Fe an
5, A. Fe a i4, L. Fi zpa ick4,R.Fe ei a-Ma ques
17,
H. F ais-Koelbl3,K.Fujii
13,W.Fu man
18, I. Goncal es30, R. Gallino36, E. Gonzalez-Rome o20, A. Go e do ski19,
F. G amegna12,E.G iesmaye
3, C. Gue e o20, F. Gunsing7, B. Haas32, R. Haigh 27,M.Heil
8, A. He e a-Ma inez4,
M. Igashi a37,S.Isae
5,E.Je icha
1,Y.Kadi
4, F. Käppele 8, D. Ka amanis9, D. Ka adimos9, M. Ke eno,6,
V. Ke le o 19, P. Koehle 28, V. Kono alo 18, E. Kossionides39,M.K iˇcka31, C. Lamboudis10, H. Leeb1,
A. Lindo e17, I. Lopes17,M.Lozano
23, S. Lukic6, J. Ma ganiec33, L. Ma ques30, S. Ma one13,P.Mas inu
12,
A. Mengoni4, P.M. Milazzo14, C. Mo eau14, M. Mosconi8,F.Ne es
17,H.Obe humme
1, S. O’B ien29,
M. Oshima38,J.Pancin
7, C. Papach is odoulou9, C. Papadopoulos40, T. Papae angelou4, C. Pa adela24, N. Pa onis9,
A. Pa lik2, P. Pa lopoulos34, G. Pe dikakis40,L.Pe o
7,R.Plag
8,A.Plompen
16, A. Plukis7,A.Poch
25,C.P e el
25,
J. Quesada23,T.Rausche
26, R. Rei a h27,M.Rose i
11, C. Rubbia15, G. Rudol 6,P.Rullhusen
16, J. Salgado30,
L. Sa chiapone4, C. S ephan5, G. Taglien e13,J.L.Tain
21, L. Tassan-Go 5,L.Ta o a
30, R. Te lizzi13, G. Vannini35,
P. Vaz30,A.Ven u a
11, D. Villama in20,M.C.Vincen e
20, V. Vlachoudis4,R.Vlas ou
40 F. Voss8, H. Wendle 4,
M. Wiesche 29,K.Wisshak
8
The n_TOF Collabo a ion
1A omins i u de Ös e eichischen Uni e si ä en,Technische Uni e si ä Wien, Aus ia

2Ins i u ü
Iso open o schung und Ke nphysik, Uni e si ä Wien, Aus ia

3Fachhochschule Wiene Neus ad , Wiene
Neus ad , Aus ia

4CERN, Gene a, Swi ze land

5Cen e Na ional de la Reche che Scien i ique/IN2P3 -
IPN, O say, F ance

6Cen e Na ional de la Reche che Scien i ique/IN2P3 - IReS, S asbou g, F ance

7CEA/Saclay - DSM, Gi -su -Y e e, F ance

8Fo schungszen um Ka ls uhe GmbH (FZK), Ins i u ü
Ke nphysik, Ge many

9Uni e si y o Ioannina, G eece

10A is o le Uni e si y o Thessaloniki, G eece

11ENEA, Bologna, I aly

12Labo a o i Nazionali di Legna o, I aly

13Is i u o Nazionale di Fisica Nuclea e,
Ba i, I aly

14Is i u o Nazionale di Fisica Nuclea e, T ies e, I aly

15Uni e si à degli S udi Pa ia, Pa ia, I aly

16CEC-JRC-IRMM, Geel, Belgium

17LIP - Coimb a & Depa amen o de Fisica da Uni e sidade de
Coimb a, Po ugal

18Join Ins i u e o Nuclea Resea ch, F ank Labo a o y o Neu on Physics, Dubna,
Russia

19Ins i u e o Physics and Powe Enginee ing, Kaluga egion, Obninsk, Russia

20Cen o de
In es igaciones Ene ge icas Medioambien ales y Technològicas, Mad id, Spain

21Consejo Supe io de
In es igaciones Cien i icas - Uni e si y o Valencia, Spain

22Uni e sidad Poli ecnica de Mad id, Spain

23Uni e sidad de Se illa, Spain

24Uni e sidade de San iago de Compos ela, Spain

25Uni e si a
Poli ecnica de Ca alunya, Ba celona, Spain

26Depa men o Physics and As onomy - Uni e si y o Basel,
Basel, Swi ze land

27Los Alamos Na ional Labo a o y, New Mexico, USA

28Oak Ridge Na ional
Labo a o y, Physics Di ision, Oak Ridge, USA

29Uni e si y o No e Dame, No e Dame, USA

30Ins i u o
Tecnológico e Nuclea , Lisbon, Po ugal

31Cha les Uni e si y, P ague, Czech Republic

32Cen e Na ional
de la Reche che Scien i ique/IN2P3 - CENBG, Bo deaux, F ance

33Uni e si y o Lodz, Lodz, Poland

34Pôle
Uni e si ai e Léona d de Vinci, Pa is La Dé ense, F ance

35Dipa imen o di Fisica, Uni e si à di Bologna,
and Sezione INFN di Bologna, I aly

36Dipa imen o di Fisica Gene ale, Uni e si à di To ino and Sezione
INFN di To ino, I-10125 To ino, I aly

37Tokyo Ins i u e o Technology, Tokyo, Japan

38Japan A omic
Ene gy Resea ch Ins i u e, Tokai-mu a, Japan

39NCSR, A hens, G eece

40Na ional Technical Uni e si y o
A hens, G eece
Abs ac . Accu a e and eliable neu on-cap u e c oss-sec ion da a o ac inides a e necessa y o he p ope design, sa e y
egula ion, and p ecise pe o mance assessmen o ansmu a ion de ices such as Fas C i ical Reac o s o Accele a o D i en
Sys ems. In pa icula , he neu on-cap u e c oss sec ions o 237Np, 240Pu, and 243Am play a key ole in he design and
op imiza ion o a s a egy o he Nuclea Was e T ansmu a ion. The lis ed c oss sec ions ha e been measu ed in 2004 a
n_TOF wi h a high accu acy due o a combina ion o ea u es unique in he wo ld: high ins an aneous neu on luence and
excellen ene gy esolu ion o he n_TOF acili y, inno a i e Da a Acquisi ion Sys em based on lash ADCs, and he use o a
high-pe o mance BaF2To al Abso p ion Calo ime e as a de ec ion de ice.
1442
CP769, In e na ional Con e ence on Nuclea Da a o Science and Technology,
edi ed by R. C. Haigh , M. B. Chadwick, T. Kawano, and P. Talou
© 2005 Ame ican Ins i u e o Physics 0-7354-0254-X/05/$22.50
INTRODUCTION
Nuclea was e is one he main issues o he public pe -
cep ion o nuclea -ene gy p oduc ion and o he sus ain-
abili y o his ene gy sou ce. Nuclea was e ansmu a-
ion has been p oposed as a way o educe subs an ially
(by a ac o o 1/100 o mo e) he adio oxici y in en o y
o he long-li edcomponen o he nuclea was e, mainly
he ans-u anium ac inides.
Ac inide ansmu a ion is p oposed o ake place by
ission in nuclea sys ems like c i ical eac o s o sub-
c i ical Accele a o D i en Sys ems (ADS). In mos o
he scena ios, he use o as -neu on ene gy spec a and
speci ic uel composi ions, highly en iched in high-mass
ans-u anium ac inides, is p oposed.
2000 40000 8000 100006000
0
50
100
150
200
250
Pulse shape econs uc ions o he BaF2 signals
Digi ised BaF2 signals
ime (ns)
signal ampli ude ( lash ADC coun s)
FIGURE 1. Digi ised BaF2signals and he co esponding
econs uc ion a e he pulse-shape analysis.
The de ailed enginee ing designs, sa e y e alua ions,
and he de ailed pe o mance assessmen o dedica ed
ansmu a ion ADS and c i ical eac o s (i.e., wi h uels
highly en iched in ansu anic iso opes) equi e mo e
p ecise and comple e basic nuclea da a [1].
O c ucial impo ance is he composi ion o he uels
p oposed o ansmu a ion de ices, wi h a la ge concen-
a ion o mino ac inides and high-mass plu onium iso-
opes. These iso opes wi h smalle ele ance o he op-
e a ion o p esen eac o s will play an impo an ole in
he neu onics o he ansmu e s and o i s ansmu a-
ion pe o mance.
1co espondingau ho :daniel.cano@ciema .es
EXPERIMENT
Iso opically en iched a ge s o mino ac inides a e a ail-
able only in small amoun s, ypically o he o de o 1-
100 mg. E en o hese small amoun s, he ac i i y o he
samples ep esen s majo di icul ies ela ed bo h o he
expe imen al echniques and he adiop o ec ion aspec s.
FIGURE 2. View o he To al Abso p ion Calo ime e as
i is implemen ed in he code GEANT4 [8] used o he MC
simula ions.
The a ge s o 237Np (43.3 mg, 1.29 MBq), 240Pu
(51.2 mg, 458 MBq), and 243Am (10 mg, 75 MBq) mea-
su ed a n_TOF ha e been all assembled in hesame way:
he adioac i e ma e ial is sandwiched by wo hin Al
laye s ( o al mass < 75 mg) and canned inside a 0.35-
mm- hick Ti canning wi h ISO 2919 ce i ica ion ( e-
ques ed by he sa e y egula ions a CERN). Thei iso-
opic pu i y has been de e mined by
γ
- ay spec ome y
and is >98% in all cases.
In cap u e measu emen s a n_TOF [2] wi h a 4-cm-
diame e neu on beam spo , he ins an aneous luence
amoun s o 105neu ons/cm2/pulse o neu on ene gies
be ween 0.1 eV and 20 GeV. This is one o he key
ea u es o measu ing he (n,
γ
) c oss sec ion o low-
mass and highly adioac i e iso opes wi h a good signal-
o-noise a io. Du ing he measu emen s, he epe i ion
a e o he PS was on a e age 3-4 p o on pulses o a
PS supe cycle o 16.4 s. In addi ion, he n_TOF acili y
p o ides an excellen ene gy esolu ion o 10

3 o 10

4
a a 185-m ligh pa h be ween he Pb spalla ion a ge
and he coun ing s a ion.
The cap u e c oss-sec ion measu emen s a n_TOF
ha e been done ela i e o he s anda d cap u e c oss
1443
sec ion 197Au(n,
γ
). Fo his eason, se e al independen
moni o s we e used pe manen ly o a p ope no maliza-
ion be ween he 197Au(n,
γ
) and main measu emen s.
(eV)
n
E
2
10 3
10
-5
10
-4
10
-3
10
coun s (no malised o he lux moni o a e)
RAW DATA om he 237Np(n,γ) measu emen a n_TOF
2.) Backg ound due o he Ti canning + 1.)
1.) Room + a ge ame backg ound
3.) 43.3 mg o 237Np + 2.)
3000 bins/decade
FIGURE 3. Raw da a om he 237Np (n,
γ
) measu emen
in he esol ed esonance egion be ween 10 eV and 1 keV.
Below, he backg ound due o he Ti canning and he emp y
TAC (wi hou any sample in he beam).
(eV)
n
E
2
10 3
10
-5
10
-4
10
-3
10
coun s (no malised o he lux moni o a e)
RAW DATA om he 240Pu(n,γ) measu emen a n_TOF
2. ) Backg ound due o he Ti canning + 1.)
1.) Room + a ge ame backg ound
3.) 51.2 mg o 240Pu + 2.)
3000 bins/decade
FIGURE 4. Raw da a om he 240Pu (n,
γ
) measu emen in
he esol ed esonance egion be ween10 eV and1 keV. Below,
he backg ound due o he Ti canning and he emp y TAC
(wi hou any sample in he beam).
The Da a Acquisi ion sys em (DAQ) [3] used in
he measu emen s consis s o 54 channels o high-
pe o mance lash ADCs [4]. Each channel has 8 Mby es
o memo y and was ope a ed a a sampling a e o 500 M
samples/s, hus allowing eco ding o he ull de ec o
his o y o neu on ene gy anges be ween 0.3 eV and
20 GeV. A e ze o supp ession and da a o ma ing, he
aw da a a e sen o CERN’s massi e s o age acili y
CASTOR [5] ia se e al Gigabi links. In pa allel, es-
pecially designed pulse-shape analysis ou ines un on a
PC a m and ex ac om he digi ized de ec o signals
he necessa y in o ma ion o he da a analysis.
The n_TOF DAQ o e s unique ea u es such as an ex-
emely low dead ime (< 10 ns), good signal analysis,
and pileup disc imina ion among o he s, esul ing in an
excellen mechanism o con ollingall kinds o sys em-
a ic unce ain ies associa ed wi h he de ec o ’s beha -
io . The quali y o he econs uc ion o digi ised BaF2
signals ( wo scin illa ion componen s
τ
sho =0.7 ns and
τ
long=620 ns) is shown in Fig. 1.
The neu on cap u e de ec ion sys em consis s o a
segmen ed To al Abso p ion Calo ime e made o 40
BaF2c ys als wi h 10B loaded ca bon ib e capsules and
placed a a 185-m ligh pa h om he spalla ion sou ce.
The TAC has a nea ly 100% de ec ion e iciency o elec-
omagne ic cascades (i.e., cap u e e en s) and good en-
e gy esolu ion (14% a 662 keV and 6% a 6.1 MeV).
The adioac i e a ge s a e placed a he geome ic cen e
o he TAC and su ounded by a C12H2004(6Li)2neu on
abso be placed inside he inne hole o he TAC. The
neu on abso be and he 10B loaded ca bon ib e cap-
sules educe he sensi i i yo he de ec o o he sca e ed
neu ons, do no educe he cap u e de ec ion e iciency
(e en hough hey lowe he o al abso p ion e iciency),
and also help in a enua ing he low-ene gy componen
(10-100 keV) o he sample adioac i i y. Fo he mea-
su emen o 243Am, a cylind ical Pb shielding o 1 mm
hickness a ound he a ge and ou side he beam was
necessa y o supp essing he s ong
γ
-ac i i y wi h en-
e gies abou 100-200 keV.
Figu e 2 shows a iew o he expe imen al se up as i
is implemen ed in he code GEANT4 [8] used o he de-
ailed MC simula ions o he TAC. The pe o mance o
he TAC has been in es iga ed bo h expe imen ally (wi h
s anda d calib a ion sou ces and he e e ence 197Au(n,
γ
)
c oss sec ion) and by Mon e Ca lo simula ions [6, 7].
Fu he mo e, all sou ces o backg ound ha e been mea-
su ed and a e being simula ed o pe o ming he back-
g ound co ec ions necessa y o an accu a e cap u e
c oss-sec ion analysis.
RESULTS
The cap u e da a o 237Np, 240Pu we e aken du ing Au-
gus and Sep embe 2004, and he 243Am measu emen
is expec ed o inish in Oc obe 2004. Fo his eason,
he da a analysis is a a e y ea ly s age. Howe e , a
simple analysis o he aw da a wi h ull s a is ics indi-
ca es p omising esul s. In he esol ed esonance egion,
a la ge numbe o esonances a e obse ed wi h good
s a is ics in bo h he aw da a o 237Np and 240Pu shown
in Fig. 3 and 4, espec i ely. Fu he mo e, he le el o he
backg ound he e is ai ly low, hus allowing us o con-
clude al eady ha he ex ac ion o accu a e esonance
pa ame e s is possible. As is shown in Fig. 5 and 6, he
c oss-sec ion analysis in he un esol ed esonance egion
will equi e a mo e de ailed s udy and sub ac ion o he
backg ound, domina ed mainly by he e ec o he Ti
1444

canning o he samples. Howe e , clea cap u e signals
a e isible in he TAC ene gy-deposi ion spec a. The
backg ound due o he emp y Ti canning and o he mino
sou ces has been measu ed wi h high s a is ics and will
be sub ac ed om he main measu emen , hus leading
o an accu a e alue o he cap u e c oss sec ion up o
100 keV.
(eV)
n
1 10 2
10 3
10 4
10 5
10
E
coun s (no malised o he lux moni o a e)
-4
10
-3
10
-2
10
RAW DATA om he 237Np(n,γ) measu emen a n_TOF
200 bins/decade
2.) Backg ound due o he Ti canning + 1.)
1.) Room + a ge ame backg ound
3.) 43.3 mg o 237Np + 2.)
FIGURE 5. Raw da a om he 237Np (n,
γ
) measu emen
in he ene gy ange be ween 0.7 eV and 300 keV. Below, he
backg ound due o he Ti canning and he emp y TAC (wi hou
any sample in he beam).
(eV)
n
E
1 10 2
10 3
10 4
10 5
10
-4
10
-3
10
-2
10
-1
10
RAW DATA om he 240Pu(n,γ) measu emen a n_TOF
coun s (no malised o he lux moni o a e)
2. ) Backg ound due o he Ti canning + 1.)
1.) Room + a ge ame backg ound
3.) 51.2 mg o 240Pu + 2.)
200 bins/decade
FIGURE 6. Raw da a om he 240Pu (n,
γ
) measu emen in
he ene gy ange be ween 0.7 eV and 300 keV. Below, he
backg ound due o he Ti canning and he emp y TAC (wi hou
any sample in he beam).
CONCLUSIONS
The neu on cap u e c oss-sec ion measu emen s o
237Np, 240Pu, and 243Am ha e been pe o med a he
n_TOF acili y a CERN. A high-pe o mance To al Ab-
so p ion Calo ime e made o 40 BaF2c ys als was used
o his pu pose. The aw da a o 237Np and 240Pu a e
ex emely p omising in he esol ed esonance egion,
whe e a la ge numbe o esonances has been obse ed
wi h good s a is ics o bo h iso opes. Fu he mo e, he
cap u e e en s can be clea ly dis inguished om he
backg ound a neu on ene gies up o 100 keV, hus al-
lowing he conclusion ha i will be possible o ex ac
he cap u e c oss sec ion up o 100 keV a e a ca e ul
backg ound sub ac ion.
Las , 237Np and 240Pu a e he i s wo cap u e c oss-
sec ion measu emen s on highly adioac i e and low-
mass ac inides wi h he To al Abso p ion Calo ime e
a n_TOF . They a e a clea expe imen al alida ion
o he good pe o mance o he n_TOF acili y, da a
acquisi ion sys em, and TAC and allow design o e en
mo e ambi ious expe imen s o he nea u u e.
ACKNOWLEDGMENTS
This wo k is pa o he Eu opean Commission 5 h
F amewo k P og amme p ojec NTOF-ND-ADS unde
con ac FIKW-CT-2000-00107.
REFERENCES
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Nuclea Fuel Cycles, ISBN 92-64-18482-1 ENEA/OECD Repo ,
2002
2. U. Abbondanoe al., "n_TOF Pe o mance Repo ,” CERN/INTC-
O-011, INTC-2002-037
3. R. Plag e al., submi ed o Nucl. Ins um. Me hods A (2004).
4. h p://www.acqi is.com
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7. D. Cano-O e al., "Mon e Ca lo Simula ion o he 4
π
To al
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250-303.
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