Nuclear Data for Transmutation
NUDATRA(DM5 of IP-EUROTRANS)EU Project: FI6W-CT-2004-516520

Enrique M. González
CIEMAT

9th International Exchange Meeting on Actinide and Fission ProductPartitioning and Transmutation NEA/OCDE

Nimes (France), September

Simulation is still and will continue to be for few years, the basis of theevaluation and extrapolation of performance, viability, cost and safety ofthe proposed transmutation devices.
Improvements on the simulation tools, programs and evaluated nuclear datalibraries, are key elements to base our benefit/cost evaluations and toprepare a solid base for the definition of DEMO reactors that can provide
the required validation before industrial deployment of transmuters.
NUDATRA is the Domain addressing this issue within EUROTRANS
Includes: Improvement of simulation programs and underlying models,
Data measurement and evaluation, uncertainty propagation and sensitivity
analysis
Device: Lead cooled ADS
Scope: Transmutation device and fuel cycle
Selection of activities initially based on relevance according to basic principles
has been later confirmed by independent sensitivity analysis.
The viability in the FP6 time frame and the complementarities with others
programs (in particular FP5) was important for the selection of measurements.

Nuclear data for Transmutation from the fuel cycle point of view
The isotopic composition of the equilibrium fuel, and correspondingly of the losses finally
going to the storage, is defined by:• The isotopic composition of the LWR wastes feed into the transmutation reactor• the isotopes decay constants,• the neutron flux intensity (reactor power) and,• the effective cross sections of the activation reactions
Activation reaction Cross section(n,γ), (n,γ)* of actinides with(n,2n) +… half-live > 100d⊗

Neutron flux Spectrum
elastic, inelastic,(n,2n),…
fuel matrix, Struct. Materials,
coolant

Transmutation takes place in a reactor: Critical or Subcritical (ADS)
Critical Reactors or ADS devoted to transmutation present new features:
In all cases
New fuels: High content on minor actinide and high mass Pu isotopes.
Very high Burn-up per irradiation cycle.

Most Frequently
Fast neutron flux spectrum.
Subcritical configurations + Spallation sources
New Technologies:

Coolant: Molten Lead or Pb/Bi,
Fuel matrix: Inert matrix,..

FF
P5
TECLA Meeting, March 25-26, 2002,
Rome

FF
P5
nT
O

nTOF FP5

nT
O

nT
O

FF
P5

Contributions to capture of present and transmutation fuels

5Sensitivity analysis(from Impact of Nuclear Data Uncertainties on Transmutation of Actinides in AcceleratorDriven Assemblies, G. Aliberti et al., NSE 146, 13–50 (2004))

keff

βeff

Pb and Bi inelastic and (n,2n)also specially relevant for He,
H production, reactivity loss
during irradiation, and void
coefficient.

Sensitivity analysis(from Impact of Nuclear Data Uncertainties on Transmutation of Actinides in AcceleratorDriven Assemblies, G. Aliberti et al., NSE 146, 13–50 (2004))
Cm244 fission
Np239 Fission
at nTOF in FP5

Cm245 Fission
at nTOF in FP5
Pb inelastic
Pb n,2nAm241 Fission
at nTOF in FP5

Bi inelastic
Bi n,2nAm243
captureAm243 Fission
at nTOF in FP5

Cross-Section
Uncertainties andRequired Uncertainty
to Meet Integral
Parameter Target
Accuracy

NUDATRA project
Nuclear DAta for TRAnsmutation
DM5 of IP-EUROTRANS
General objective:

Improve nuclear data evaluated files and models which involves sensitivity
analysis and validation of simulation tools, low and intermediate energy nuclear
data measurements, nuclear data libraries evaluation at low and medium
energies, and high energy experiments and modelling.
Participants: 13 Research Centers + 9 Universities
CEA (France), CIEMAT (Spain), CNRS (France), CSIC (Spain), FZJ (Germany), FZK(Germany), GSI (Germany), INFN (Italy), INRNE (Bulgaria), NRG (Netherlands), PSI(Switzerland), SCK-CEN (Belgium), JRC-Geel (EC)
Universities: AGH (Poland),TUW (Austria), KTH (Sweden), ULG (Belgium), UNED
(Spain), USDC (Spain), USE (Spain), UU (Sweden), ZSR (Germany).

NUDATRA Organisation

IRMM/
Geel
(JRC)

CIEMAT

NRG
UNED (ENEN)

CEANUDATRA Specific objectives¾ Pb-Bi cross sections: inelastic, (n,xn), Po production (B.R.)¾ MA: Capture in 243Am + Fission on 244Cm¾ TALYS improvements for MA evaluation and test on new Pb data
¾ High energy measurements: Gas (He) and Light Charged Particles
production, Absolute Spallation product x-section¾ High energy models improvement (INCL & ABLA)¾ Sensitivity analysis of ETD fuel cycle¾ New versions of transmutation simulation systems

WP5.2 Low and intermediate energy nuclear data measurements:
Participants: FZK,CEA,CIEMAT,CNRS,CSIC, INFN, JRC-Geel, TUW,UU

Task T5.2.1 Pb and Bi cross section and branching ratios
High resolution excitation functions for the
inelastic scattering cross sections of Pb andBi
Critical to model correctly the ADS neutron spectra
206, 207, 208Pb and 209Bi, thr-20 MeV by (n,n’γ)

at Gelina
Gamma-ray production cross sections
are measured and total and levelinelastic cross sections will be deduced
209Bi

13/2+Æ9/2- M1+E2

209Bi (n,n’) 1608.53keV γ production

Total 209Bi inelastic cross-section

WP5.2

206, 207, 208Pb and 209Bi, thr-20 MeV by (n,n’γ) at Gelina

Data is already taken and analysis is progressing. First EXFOR files produced.

209Bi

206Pb

Total inelastic

207Pb

Total inelastic

Total inelastic

208Pb

Total inelastic

209Bi(n,2n) 565 keV

WP5.2 Low and intermediate energy nuclear data measurements:
5.2.1.4 Measurements of Pb and Bi (n,xn) cross sections
206Pb,209Bi (n,xnγ)

206Pb(n,n’γ)206Pb

208Pb(n,3nγ)206Pb

Effects on the neutron multiplication, the source
importance and neutron spectra of ADS cooled with
Pb/Bi or using Pb/Bi spallation target

803 keV

Progress: Measurements performed and analysis
ongoing for: 207Pb(n,2n)206Pb, 208Pb(n,2n)207Pb ,208Pb(n,3n)206Pb, 209Bi (n,2n) 208Bi
Online HPGe detectors at Gelina
Pb (n,2nγ)206Pb

Pb (n,2n)803 keV integral

207

803 keV

Cross section (mb)

Cross section (mb)our data
Vonach et al.
TALYS
EMPIREPb (n,2n)206Pb Total

Our work
Frehaut
TALYS
EMPIRE-II

208Pb (n,2n) 570 keV

4π dσ/dΩ (mb/st)

207
207

En (MeV)

En (MeV)WP5.2 Low and intermediate energy nuclear data measurements:
Participants: FZK,CEA,CIEMAT,CNRS,CSIC, INFN, JRC-Geel, TUW,UU

Task T5.2.1 Pb and Bi cross section and branching ratios
Bi capture branching ratio (209Bi(n,γ)210m,gBi)
Production of 210gBi is the mechanism leading to 210Po production.
210mBi decay α to 206Tl.
210Po is one of the main ADS target and coolant activation concerns

The time-of-flight technique will be used at Gelina
Two (3) HPGe detectors will be used to distinguishbetween capture events leading to the ground state andthe meta-stable state
Compensation for γ angular dependence
Setup prepared andoptimized,
Preliminary data
presented at
Physor 2006

800 eV
209Bi resonance

320 keV
γ-ray

210Bi

WP5.2 Low and intermediate energy nuclear data measurements:
5.2.1.3 Meas. of Pb (n, n’+X ) cross section at 100 MeV
Non existing differential data required for Pb based ADS highenergy neutron shielding calculations and spallation n multiplication
Pb (n,n’+X) at The Scandal facility at Uppsala
Setup optimization, preliminary analysis of 2003-2004 data.

Pb(n,xn) Uppsala ’03
Uppsala ‘04
Fe(n,xn) Uppsala ‘04

TSL - UPPSALA ’03 ‘04
DECOI & DEMON
En ~ 10 - 50 MeVTARGETΦ ~ 106-7 s-1
d ~ 8 cme ~ 2 cms ~ 10x10 cm2

neutron beam

CLODIA & SCANDAL
En ~ 40 - 100 MeV

Double Differential Cross Section
Fe, Pb (n,xn) @ 96 MeV – 15, 30, 50, 70°

WP5.2 Low and intermediate energy nuclear data measurements:
MA Capture and Fission cross sections
T5.2.2 MA capture cross sections 243Am (n,γ) at nTOF-Ph2 (at CERN)Transmutation of MA: 243Am is the path to 244,245,246,247Cm production
Time of flight + 4π TAC.
The methodology and setup tested in 2004 at the FP5 nTOF-ADS project.
Setup optimization, Preliminary analysis of 2004 data.
n_TOF_Ph2 proposal including 243Am (n,γ) submitted+supported by CERN Res. Board.
Test 243Am(n,γ) measurement performed in 2004
First measurement worldwide in the RRR:
Mass=10 mg and activity > 80 MBq!

237Np(n,γ)

WP5.2 Low and intermediate energy nuclear data measurements:
MA Capture and Fission cross sections
T5.2.3 244Cm neutron induced fission crosssection measurements
244Cm(n,f) from 243Am(3He,pf)

242

Cm(n,f)3,5
3
2,5Measurements of the transfer reactions
243Am(3He,pf) at Orsay + Evaluations andmodels for the formation of the composite
nucleusHe

Vorotnikov et al.
CENBG
ENDF
JEFF
JENDL

2
1,5
1
0,5
0

3

0

1

2

3

4

241
242Am

241Am

(3He,α)3

243Am(3He,p)+n(3He,t)

5

6

7

8

9

10

Am(n,f)

2,5
CENBG

2

(3He,d)
245Cm

ENDF

1,5
242Cm

243Cm

+n

244Cm

+n

Fission
Detectors

+n

JEFF

1

JENDL

0,5
Fission Fragment00

3He (30 MeV)

1

2

3

4

5

6

7

8

9

10

243Am-target(x= p,d,t,α)ΔE

Si Telescopes

E

Setup optimization, First data taken.
241Am(n,f) and 242Cm(n,f) deduced

WP5.3 Nuclear data library evaluation and low and intermediate
energy models
Participants: CEA,INRNE, NRG, TUW,USE

Measurements must be evaluated to become useful for simulations
Models can help to complete libraries many channels and isotopes without
experimental data, above the resolved resonance region.
T5.3.1 Improvement of low and intermediate nuclear reaction models
Improvement of Nuclear model code TALYS: generalized superfluid model for level
densities implemented and tested with U isotopes
Development of Methods to generate covariance data: 2 methods in good progressT5.3.2 Evaluation of minor actinide data
Optical model, pre-equilibrium, compound nucleus and fission model parameters will be finetuned
Priority to Americium isotopes in the fast neutron range first test to 241Am.
The resonance regions is also being analyzed
New isospin-dependent dispersive optical model potentials for actinides have beendeveloped and and sent to publication

T5.3.3 Re-evaluation of data libraries for Pb and Bi
Using the data from the WP5.2 to complement the existing and FP5 data (nTOF,…),
First test already made with the new WP5.2 and CEA/BRC data from 7 to 14 MeV

WP5.3 Nuclear data library evaluation and low and intermediate energy
models (NRG)
T5.3.3 Re-evaluation of data libraries for Pb and Bi
Using the data from the WP5.2 to complement the existing and FP5 data (nTOF,…),
First test already made with the new WP5.2 and CEA/BRC data from 7 to 14 MeV
206Pb(n,n’γ)206Pb

208Pb(n,3nγ)206Pb

803 keV207

Pb (n,2n)803 keV
integralWP5.4 High energy experiments and modelling
Participants: CEA, FZJ, GSI, ULG, USDC, ZSRThe energy range (200-1000 MeV) specific of the ADS
spallation target
Completing the experimental database of the HINDAS FP5
project (Very big progress on H.E. models but still some weak
points)T5.4.1 High energy experiments for Radioactivity,
chemical modification and damage assessment (USDC)
Total fission cross-section (200 MeV - 1 GeV) for
Pb and W
Total fission cross sections in reactions induced by
208Pb on 1H and 2H have been measured at 500 A
MeV at GSI. Analysis is on progress.
Production of long lived Intermediate massfragments as 7Be and 10Be from Bi, W, Ni targets:
100-1000 MeVHelium production in W or Ta and Fe or Ni, between
E=100-800 MeV (NESSI/PISA experiment at FZJ)GSI @ Darmstadt(Germany)

WP5.4 High energy experiments and modelling
He, LCP and Long-lived IMFs as 7Be/10Be production from selected targets
measured at Hannover (ZSR) and NESSI+PISA
Comparison INCL4/ABLA withrecent NESSI data
Helium production
ZSR Hannover

Helium production cross−section (mb)p + Fe1000

NESSI
MichelBertini−Dresner
INCL4−ABLA
INCL4−GEMINIINCL4−Clus−GEMININESSI newSPALADIN preliminary

100

10

0

500

1000
1500
2000
Incident energy (MeV)

2500

3000

1.2 GeV p+Ta4oNessi1
Entries
23
Mean
23.5
11.72
RMS

Au(p, He)X 2.5GeV 100

Comparisons PISA / NESSI… 10

2

Au(p,4He)X at 2.5 GeV, 100o
10

Nessi (105 ) 1.1mm Si+7cm CsI
Pisa 2005 3.5 mm Sio1

Note that energy range
for PISA will be extended
when CsI is taken
into account

10-1

-2

10

0

20

40

60

80

Nice agreem
ent on

100

absol
ute

scale
!

Au(p,7Li)X at 2.5 GeV, 35o

WP5.4 High energy experiments and modelingT5.4.2 High-energy nuclear model improvement: Extension of INCL4 and ABLA
INCL4: Implementation of a dynamical coalescence model for cluster production(seems to correctly reproduce the production of high energy light clusters except 4He/3He
ratio), Introduction of isospin- and energy-dependent average nucleon potentials,
Improvements of pion dynamics (n multiplicity at very high energies)
ABLA: Fission, Composite LCP, Intermediate Mass Fragments
1 A GeV 238U + p
ALL

LCP(d,t,3
He,...)IMF
FISSIONIMF

noproduction
calculated
here

EVAP.
RESIDUESZABLA improvement on IMF emission

T5.4.3 Quality assessment, validation and impact of the new models in ADS (ETD)
simulations
Implementation in High Energy transport codes (MCNPX)
Calculations of radiotoxicity, radioactivity due to residue production in the MEGAPIE. Calculationsof DPA, chemical composition modifications, and activities in ETD with the new codes .

WP5.1 Sensitivity Analysis and Validation of Nuclear Dataand Simulation Tools
Participants: FZK,CEA,CIEMAT,NRG,PSI,SCK,AGH,KTH,UNED

T5.1.1 and T5.1.2: Uncertainties propagation and Sensitivity analysis forthe fuel Cycle
A list of topics for sensitivity evaluation of the transmutation ADS fuel Cycles had
been proposed.
Wide review/compilation/comparison of uncertainties from the most recent activation
data files, evaluated nuclear data files and bibliography proposals has been
performed.
Proposals and tests of methodologies for the definition of covariance matrixes on
nuclear data when not available.

Review/Compilation, Processing and Analysis of Available Uncertainty Cross-Section Data
Complete list of materials with covariances of neutron cross section (FILE 33/40)
BROND-2.2

CENDL-2.1

ENDF/B-VI.8

ENDF/B-VIIb

IRDF90-2.0

IRDF2002

JEF-2.2

JEFF-3.1

JENDL-3.3

N. of MAT=3

N. of MAT=9N.of MAT=44

N.of MAT=35

N. of MAT=37

N. of MAT=48

N. of MAT= 15

N. of MAT= 34

N. of MAT=20

C
Au197
Pb

H2 – 3
O16
F19
Mn55
Fe 56
U238
Pu240
Am 241

Li7
C
F19
Na23
Si, Si28 – 29 – 30
Ti46 – 48
V
Cr50 – 52 – 53 – 54
Mn55
Fe 54 – 56 – 57 – 58
Co59
Ni58 – 60 – 61 – 62 – 64
Cu63 – 65
Y89
Nb93
In, In115
Re 185 – 187
Au197
Pb206 – 207 – 208
Bi209
Th232
U238
Pu240 – 242
Am 241

Li7
C
F19
Na23
Si28 – 29 – 30
Ti 48
VCr50 – 52 – 53 – 54
Mn55
Fe 54 – 56 – 57 – 58
Co59
Ni58 – 60 – 61 – 62 – 64
Cu63 – 65
Re 185 – 187
Au197
Pb 208Bi209
U238
Pu240 – 242
Am 241

Li6
B10
F19
Na23
Mg24
Al27
P31
S32
Sc45
Ti46-47-48
V
Cr 52
Mn55
Fe 54 – 56 – 58
Co59
Ni58 – 60
Cu63 – 65
Zn64
Y89
Zr90
Nb93
Rh103
Ag109
In115
I127
Au197
Th232
U235 - 238
Np237
Pu239

H1
Li6 – 7
Be 9
CCo59
Ni58-60–61-62-64
Y89
Au197
U235 – 238

H3
Be 9
C
F19
Si28
Ti46–47-48–49-50
V
Cr50–52–53–54
Mn55
Fe 54–56–57–58
Co59
Ni58–60–61–62–64
Cu63 – 65
Y89
Zr90
Nb93
Re 185 – 187
Au197

H1
B10 – 11
O16
Na23
Ti 48
V
Cr52
Mn55
Fe 56
Co59
Ni58 – 60
Zr90
U233 – 235 – 238
Pu239 – 240 – 241

Li6, B10, F19, Na23
Mg24, Al27, P31, S32
Sc45
Ti46-47-48 -49 Ti49(n,x)Sc48
V 51
Cr 52
Mn55
Fe 54 – 56 – 58
Co59
Ni58 – 60
Cu63 – 65
Y89
Zn64
As75
Y89
Zr90
Nb93
Rh103 Rh103(n,n')Rh103m
Ag109 Ag109(n,g)Ag110M
In115 In115(n,n')In115m
I127
La139
Pr 141
Tm 169
Ta181
W186
Au197
Hg199 Hg199(n,n’)Hg199M
Pb204 Pb204(n,n')Pb204m
Th232
U235 - 238
Np237
Pu239
Am 241LIBRARY

Nº of materials withcovariance data

Nº of xs with covariancedata (approx.)

BROND-2.2

3

35

CENDL-2.1

9

75

IRDF90-2.0

37

>100

IRDF2002

48>100

ENDF/B-VI.8

44

400

ENDF/B-VIIb

35

>200

JEF-2.2

15

130

JEFF-3.1

34

400

JENDL-3.3

20

180• Assessment of Uncertainties in the Calculation of Neutron Induced Reaction Crosssections at Energies Above 0.1 MeV• Proposals for Generation of Uncertainty Data
• Topics for Uncertainty Evaluation• Progress in Defining Uncertainty Methodologies: Implementation and Proof of
Principle for Practical Use

Sensitivity/
uncertainty
analysis+Monte Carlo
MethodHistogram of the 1000 values of the
242Cm concentration obtained byMonte Carlo Method. The red line isthe lognormal density function

WP5.1 Sensitivity Analysis and Validation of Nuclear Data andSimulation Tools
Improvement of Transmutation plants simulation programs
T5.1.3 Development and validation of simulation programs for transmutation plants:
MCB, EVOLCODE and KAPROS/KARBUS.

Updated versions of MCB, EVOLCODE.
EVOLCODE2:
Improved approximations on:
Energy dependence of Fission yields, Isomer production
Convolution method, Isotopes without transport x-sections
Different cross sections (T, library,…) at different cells
Increased number of isotopes for burnup (Spallat. prod.)
Improve coding, portability and bug fixes
Examples of benchmarks and applications
MCB:
New options: Normalization to proton intensity or total power
Improved fuel lattice handling, Spallation products included.
Bug fixes.

WP5.1 Sensitivity Analysis and Validation of Nuclear Data andSimulation Tools
Validation of Data, Models and programs
T5.1.4 Nuclear data and models validation for the spallation target (PSI):
Residual nuclei production in SINQ targets.
Measurements of absolute activities of residues (eg.: 194Hg, 207Bi) in spallation target models(Dubna, PSI).

Predefinition of spallation residues benchmarks based on Dubna data (IAEA).
T5.1.5 Minor actinide and Pb nuclear data validation in integral experiments (CIEMAT):
Fission cross section from MASURCA (Cadarache) experiments
240,241,242Pu, 237Np and 241,243Am

First analysis done from MASURCA 1A’ and 1B
Other Minor actinide and Pb nuclear data validation based on results from ISTC projects
Facilities: BFS, SAD, Yalina
Experiments completed and in preparation

Preparation/Definition of SAD and YALINA setups (but review might be needed after
clarification of ECATS)

Conclusions and Outlook
Progress In the first year of NUDATRA
WP5.1:Development and validation of sensitivity analysis methodologies and collection ofexisting covariance information. Development of new versions of transmutation simulation
codes (EVOLCODE2, MCB) + test of new/old codes KAPROS/ALEPH

WP5.2:

Measurements of:206, 207, 208Pb and 209Bi, thr-20 MeV by (n,n’γ) at Gelina
206Pb,209Bi (n,xnγ) two techniques at Gelina
Preparatory setups/analyses for 244Cm(n,f) from 243Am(3He,pf), 243Am (n,γ), Pb (n,xn’) at
100 MeV, 209Bi(n,γ)210m,gBi Branching Ratio.

WP5.3:

Improvements of TALYS (low intermediate energy reactions modelling code used forevaluation) to be able to handle actinides

WP5.4:

Measurements of He and Be production in high energy protons reactions at NESSI/PISA+ prep. spallation @ GSI. Improvements on high energy reaction models INCL and ABLAIn the coming years:
Complete evaluation of uncertainties for transmutation fuel cycles most relevant
parameters & identification of additional data
Completing the Pb and Bi data at low energies & Reliable Am and Cm data
Upgraded TALYS and model generated complete cross section and covariance libraries
Validated reliable high energy codes in MCNPXGSI @ Darmstadt (Germany)nTOF @ CERN (Switzerland)

Gelina @ Geel (UE-Belgium)

and its TAS γ-calorimeter

Cyclotron @ Uppsala(Sweden)Neutron capture (n,γ)
resonances in one actinide