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Nuclear data at n_TOF for fundamental

science and industrial applications

Enrique M. González Romero


CIEMAT, on behalf of the n_TOF Collaboration

New Opportunities in the Physics Landscape at CERN

CERN, Geneva
12-05-2009

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 1
n_TOF: Neutrons at CERN.
A world leading facility for accurate measurements of

Nuclear data at n_TOF for fundamental science and


industrial applications

- Nuclear data needs for industrial applications and n_TOF opportunities


The example of Nuclear Wastes management

- Synergy with fundamental nuclear physics

- The short term program of n_TOF

- The next frontier (upgrading the n_TOF facility)

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 2
There is a wide range of Nuclear Data
applications from:
- Medical treatment and diagnostics to
- search for oil or space exploration,
however the largest social impact is at:
- the electricity production by fission
- the reduction of nuclear wastes.

In a nuclear reactor, the dominant


processes are:
- n- induced fission (energy+wastes)
- neutron capture (activation+breeding)
- elastic and inelastic neutron scattering
- radioactive decay
- (n,xn), (n, charged particle), …

It is intrinsic to nuclear fission the large energy release per reaction and the production of
short lived nuclear wastes (fission fragments)
However, the amount and nature of production of isotopes per activation (Pu and other
actinides + structural materials) depends on the technological design.
New reactor concepts under evaluation might allow to reduce (1/100) the existing stock and
production of the long lived high level waste (Transmutation).

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 3
- n- induced fission (energy + wastes)
Main reactions in a - neutron capture (activation + breeding)
nuclear reactor or - elastic and inelastic neutron scattering
transmutation device - radioactive decay
- (n,xn), (n, charged particle), …

(n, X+charged part.)

ay)
c
de
e (+
ptur
ca β + x n) y)
n ,
(n eca
d
(+
β -

fission Standard reactor


1500 isotopes
ADS with spallation
3000 isotopes

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 4
σ (E ) 238
U Capture
Rate = ∫ n σ ( E )ϕ ( E ) dE 235
U Fission

- n- induced fission
- neutron capture

- elastic and inelastic neutron scattering


1meV 1eV 1keV 1MeV
Thermalization, Moderation

Resonances (absorption, elastic, inelastic,…)

ϕ (E ) Pressurized ϕ (E )
Water cooled
Reactor

Lead (Pb/Bi)
cooled
Fast ADS

1keV 1MeV
1meV 1eV 1keV 1MeV
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 5
One example: Nuclear waste minimization and P&T
Partitioning & Transmutation HLW + ILW: Radiotoxicity
(providing new solutions to social
request for nuclear wastes manag.)
Heterogeneity of Spent nuclear fuel
1E+

1/100
Components -> Separate and recycle 1/1000
materials dangerous for environment
or valuable to produce energy.
P&T will:
• Reduce by 1/1000 the HLW mass
• Reduce by 1/100 the HLW radiotoxicity
1 100 10000 yr 106
• Reduce by 1/100 the Heat Load to
repository 1,E+04
Heat Load to repository
B2 B1 A3
• Reduce by 1/1000 the time
Heat after unloading (W/TWhe)
A2 A1
1,E+03

• Reduce by 1/100 the proliferation in 1,E+02


repository
1,E+01
• Increase by 5-30 the capacity of hard-rock
repositories 1,E+00

• Increase by 30% to 3000% the energy from 1,E-01

the fuel

1E+
1,E-02
1 10 100 1000 10000
Cooling time (a)

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 6
Present in nuclear wastes Thermal and Fast Fission
Medium Half-Life (<100 años) Fast Fissión
Short Half-Life (< 30 dias) Low Fission Cross Section TRU Transmutat
High A actinides
Fast Spec
Fast Spectrum Transmutation Scheme
Av. Flux Intensity (n/cm2/s)
3,00E+15
Cm242 Cm243 Cm244 Cm245 C
Second 1 Time Unit α / SF α / EC/ SF α / SF α / SF
Hour 3600 31570560 100 / 6.2E-6 99.7/0.29/ 5.3E- 9 100 / 1.35E-4 100 / 6.1E-7
Day 86400 0,446 29,068 18,080 8490,695
Year 3E+07 18,130 2,798 6,257 2,922
64,7% 8,0% 65,2% 11,4%

Am241 Am242 Am242m Am243 Am244


α / SF β− / EC IT / α / SF α / SF β− / EC
100 / 3.77E-10 82.7 / 17.3 99.5/0.46/1E- 3 100 / 3.7E-9 100 / 4E-2
432,225 0,002 140,846 7361,922 0,001
3,652 17,792 1,844 4,892
44% : 44% 13,1% 8,4% 87,0%

Pu238 Pu239 Pu240 Pu241 Pu242 Pu243


α / SF α / SF α / SF β− / α α / SF β−
100 / 1.9E-7 100 / 3.1E-10 100 / 5.7E-6 100 / 2.45E-3 100 / 5.5E-4 100
87,644 24083,608 6556,805 14,334 372891,707 0,001
4,220 3,477 9,033 2,688 11,354 6,775
37,5% 19,4% 54,8% 14,2% 61,1% 30,6%
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 7
Fuel
Fabrication

Reactors: (∆ <0.5%)
Performance: Reaction rates,
Nuclear
Power Plant Power distribution, Flux, Energy
Spectrum
Safety: Criticality, Feedbacks,
Interim
Reactivity coeffs, Damage, Shielding
Storage
SPENT FUEL Waste: Isotopic evolution, activation

Storage, Reprocessing and


Reprocessing
Fabrication plants: (∆ <5%-10%)
Plant
High Level Wastes Isotopic composition !!!
Radioactivity, Neutron emissions,
High Level Decay Heat,
Liquid Wastes
Advanced
Aqueous
Fabrication
of new fuels Proliferation interest
Minor (MA) and Targets
Partitioning
Actinides

Fission (FP)
Storage, Reprocessing and
Fabrication plants: (∆ <5%-10%)
HLW Products

Isotopic composition !!!


High
Radioactivity, Neutron emissions,
Level
Wastes
Decay Heat,
Proliferation interest
Pyrochemical Partitioning ADS Transmuter
Deep Geological
Repository for Radiotoxicity and Dose to Public and
High Level Wastes
Environment
Effective capacity
E. Gonzalez:Open
CycleNuclear dataStandard
at n_TOF Advanced
Reprocessing
Reprocessing
for fundamental science and industrial applications (CERN, 12-05-2009) 8
(Partitioning and Transmutation)
New isotopic composition of transmutation and future reactor fuels
New coolants and fuel matrices
New requirements for structural materials
New neutron spectra
High energy neutrons from the Spallation Source

New isotopic composition of transmutation and future reactor fuels

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 9
Sensitivity analysis – ADS for Transmutation

keff

a) Upper limit of the group


E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 10
NEA/WPEC-26.
One possible optimization for
target accuracy for innovative
systems using recent
covariance data evaluations
(BOLNA).
M. Salvatores and R.
Jacqmin (Eds),
NEA/WPEC-26.
ISBN 978-92-64-99053-1

Similar tables for each


present or proposed future
reactor
Still serious dependence on
the reactor and fuel models
and on the transmutation
model (homogeneous) can
slightly modify the target
accuracy and details on the
priority order
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 11
Important isotopes for Transmutation Fuel Cycles: The multi-
recycling point of view

Report of the
Numerical results
from the Evaluation of
the nuclear data
sensitivities, Priority
list and table of
required accuracies
for nuclear data. E.
Gonzalez-Romero
(Ed), NUDATRA
Deliverable D5.11
from IP-Eurotrans

T= Transmutation efficiency
DH= Decay Heat load
N = Neutron emission
R = Radiotoxicity

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 12
Identifying and setting priorities of Nuclear data for
applications: An international endeavor
• Applications set the problems to be analyzed and the required accuracies for the
simulation.
• Detailed uncertainty and covariance propagation to evaluate the accuracy.
• Sensitivity analysis identify the relevance of each data for each
isotope/reaction/energy on the most significant parameters
• Linear Optimization with expert assessment of “cost” (experimental difficulties) to set
priorities
Efforts coordinated by dedicated expert groups of NEA/OECD, IAEA, and
dedicated EU framework programs

EU leadership on nuclear data measurements:


• Measurements at USA, Japan, Russia and EU.
• Clear and repeated demand from the Nuclear Waste community, Sustainability of
Nuclear Energy (Resources, Safety, Waste) by EU Framework Program calls:
- FP5: nTOF_ND_ADS (start of nTOF facility at CERN)
- FP6: NUDATRA (inside EUROTRANS),
- FP6: EFNUDAT (Transnat. Access) + CANDIDE (Roadmap for ND)
- FP7: ANDES proposal to WP2009
One EU call on Nuclear Data for each FP (FP5-FP7),
nTOF measurements in all of them

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 13
n_TOF beam characteristics
• Wide energy range 2nd collimator φ =1.8 cm (capture mode)
• High instantaneous n- flux
• High resolution
• Low ambient background
• Low repetition frequency
• Favorable duty cycle for
radioactive samples.

Capture (0.1eV-1MeV)

Fission (0.1 eV-20MeV)


Spallation (1keV-200MeV)

One of the best worldwide facilities for radioactive samples:


slightly smaller peak n-flux than LANCE but lower repetition rate and longer fly path
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 14
n_TOF: Advanced DAQ and detectors
+ Precision simulations (Geant4, MCNPX, Fluka): Utilization and Validation

Low n-sensitivity capture detectors Total Absor. Segmented Calorimeter

First FADC DAQ for T.o.F facilities Fission det. reconstructing F.F. trajectories
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 15
n_TOF experiments
Capture 2000-2004
151
Sm
204,206,207,208
Pb, 209 Bi
measurements
Sensitivity analysis
232
Th
24,25,26
Mg NSE 146, 13–50 (2004))
90,91,92,94,96
Zr, 93 Zr NEA/WPEC-26 (2008)
139
La
NUDATRA Deliverable D5.11 of IP-Eurotrans (2009)
186,187,188
Os
233,234
U Other types of reactor & cycles (Th-U, PWR)
237
Np,240 Pu,243 Am

Fission
233,234,235,236,238
U
232
Th
209
Bi
237
Np All data first published then stored
241,243
Am, 245 Cm in the EXFOR database
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 16
The n_TOF Collaboration
n_TOF measurements are designed to obtain the maximum
information for fundamental nuclear physics
• Nuclear structure models
- Improving the accuracy and statistical information from resolved resonances
(RR)
Extending the RR region
Level densities and criteria for the estimation of missed resonances
- Photon Strength functions from the TAC
- Direct vs. compound nuclei mechanism
- Measurements in closed-shell nuclei and light nuclei (Pb, Mg,…)
• Fission towards a better understanding of the process
- High resolution measurements over large energy ranges in the same setup
- FF kinetic energy and angular distributions determination
- Fissile (233 U, 235 U, 245 Cm) and Fissionable isotopes (234 U, 232 Th, …)
- Sub-threshold, direct and multiple chance fission
- Fine structures in the fission barriers (outer fission barrier and hyper-
deformation of the fission potential)
• Basic reactions
- n-n scattering by 2H(n,np)n
- (n, l.c.p.) reactions (l.c.p. = light charged particles like p, α , 3H, Li,…)
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 17
High resolution low backgr. of radioactive samples: 232 Th by C6D6
Resolved Resonance Region Unresolved Resonance Region

High peak n flux


intensity reduce the
radioactive
background
+ high resolution
-> larger RRR +
Small resonances

level spacing reduced neutron


width distribution ∞
mass (232 Th) =
N(Γt ) = N(0)∫Γ P(x)dx

2.8037 g
t

diameter = 1.5 cm
purity = 99.5%

F.Gunsing, Nuc. Data. Conf.-2007


G. Aerts et al. (n_TOF Collaboration), Phys. Rev. C 73, 054610 (2006)
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 18
High resolution low backgr. of radioactive samples: 237 Np TAC

n_TOF
capture
+
Geel
transmission
=
One of the
best measur.
made at
Europe.

C. Guerrero et al. (n_TOF Collaboration), Proc. Int. Conf. Nuc. Data for Sci. and Tech. 2007, Nice.
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 19
High resolution low backgr. of radioactive samples: 243 Am TAC

First direct 243 Am(n,γ ) measurement EVER

D. Cano-Ott et al. (n_TOF Collaboration), Proc. Int. Conf. Capture Gamma-Ray Spec.
2005, Santa Fe.

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 20
High resolution low capture cross section samples: C6D6 + TAC
204
Pb

Fitting of resonance parameter in progress!

first know n
Impurities
Mg resona nce
In, Sb at 20 keV

206
Pb

M.Heil (FZK), Nuclei in the Cosmos IX,


Geneva 2005

C.Domingo-Pardo et al. (n_TOF


Collaboration), Phys. Rev. C 74/75, 2006/7
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 21
Nuclear structure: TAC response 197 Au(n,γ ): Esum and mγ
Validation of Adjusted Photon Strength Functions models with 197 Au(n,γ ) TAC
data for deposited energy (with and without conditions in mγ ) but also for mγ
(Esum >1.5 MeV).
Similar studies for several isotopes.

mγ >0

mγ >2

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 22
High resolution and large energy range accurate fission data
U: High
235
Cm: poor previous
245

accuracy experimental results


differences

U:
233

n_TOF vs
ENDF BVII

U/235 U: both isotopes


238

are fission standards up


to 200 MeV.

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 23
High resolution and large energy range accurate fission data

Fine structures in the fission


barriers (outer fission barrier
and hyper-deformation of
the fission potential)

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 24
Capture and Fission accurate measurement in the same facility

Neutron induced capture Neutron induced fission


234
U(n,γ )
234
U(n,f)
ENDF/B-
VI
n_TOF
(PPACS)

W.Dridi, PhD-Thesis, 2006 C.Paradela, PhD-Thesis, 2005

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 25
n_TOF_ph2 experiments

Capture Sensitivity
analysis
Stable Isotopes:
Mo,Bi: Materials for fuel matrix (Mo) and coolant (Bi)
Fe, Ni, Zn, Se: Structural materials NEA/WPEC-26
234,236,238
U, 231,233 Pa: Th/U fuel cycle (2008)
239,240,242
Pu,241,243 Am, 245 Cm: transmutation of minor actinides
NUDATRA
Fission Deliverable D5.11
231
Pa,234,235,236,238 U : Safety and sustainability of nuclear energy of IP-Eurotrans
241
Pu,245 Cm,241,243 Am, 244,245 Cm : transmutation of minor actinides (2009)
234
U: study of vibrational resonances below the bareer
Other types of
reactor & cycles
Other (Th-U, PWR)
n-n scattering by 2H(n,np)n
(n, lcp) (lcp = light charged particles like p, α , 3H, Li,…)

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The next frontier: n_TOF @ EAR2 and SPL/PS2
• Increasing the flux by 100-1000 and maintaining acceptable resolution
• Reducing the mass by 100 from 1mg -> 10µg
• Reducing the acceptable half-life from 500y -> 10y
• Open the possibility of measuring presently challenging isotopes like
238,241
Pu, 242m Am, 243,244 Cm
• Critical isotopes for waste transmutation and basic nuclear physics
n_TOF @ PS-EAR2:
- Shorter path 1/10 -> 100 times larger flux
- Resolution reduced to 1/1000 still accept.
- Improving the ambient background
- Improving the beam induced background
n_TOF @ SPL/PS2:
- Further increase of peak flux intensity (x10)
- Lower background 20 -> 4 GeV protons
- Dedicated capture and fission areas
Additional opportunities combined with
HI_E_ISOLDE
E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 27
The (future) second n_TOF experimental area

New
experimental
area at 20 m

n_TOF target
Experimental
area at 185 m

Flight-path length : ~20 m


at 90° respect to p-beam direction
100 times more intense!

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 28
Summary and conclusions
• n_TOF @ CERN is a first class neutron Time Of Flight facility coupled to a
spallation neutron source: 185 m flight path, very high peak flux, wide energy
range, favorable duty cycle and excellent energy resolution.
• It is specially well suited for radioactive materials, samples of rare materials or
low cross section.
• Excellent facility for measuring neutron capture and fission cross sections and
the most needed cross sections identified for nuclear applications (nuclear
waste minimization). Sustained support from the EU framework programs.
• The measurements provide very relevant parameters to improve the
understanding and physics models of nuclides and reactions
• Combined with High performance detectors and DAQ allows to perform high
accuracy cross section measurements
• The n_TOF potentiality was proved by successful operation from 2000 to 2004
• The new campaign, with improved setup, will allow to fully exploit its possibilities
addressing the remaining high priority nuclear data needs
• Enhanced performance from EAR2 or SPL will allow to open a new frontier of
sample masses, short lived isotopes and accurate measurements

E. Gonzalez: Nuclear data at n_TOF for fundamental science and industrial applications (CERN, 12-05-2009) 29