Nuclear Data Study for
Nuclear Transmutation
Research Laboratory for Nuclear Reactors,
Tokyo Institute of Technology
Masayuki IGASHIRAContents
1. Introduction
2. Present Status of the Accuracy ofNuclear Databases for MAs and LLFPs
3. Cross Section Measurements for MAs and LLFPs
4. A Japanese Nuclear Data Project
5. Summary
MAs: Minor Actinides (Np-237, Am-241, Am-242m, Am-243,Cm-244, Cm-245, Cm-246, etc)
LLFPs: Long-Lived Fission Products (Se-79, Zr-93, Tc-99,Pd-107, Sn-126, I-129, Cs-135, etc.)21. Introduction# The current national policy in Japan for the managementand disposal of MAs and LLFPs is a sequence ofvitrification,interim storage, and thendepositing
underground together with other nuclear wastes.
# If MAs and LLFPs are extracted and transmuted into stable
nuclides, the environmental loading in the geologicalrepository becomes very small.
# The ethical problem that MAs and LLFPs are undesirable
property for our far descendants will be solved.
3

1. Introduction# The nuclear transmutation of MAs and LLFPs isa very attractive subject.
--> Neutron capture and/or fission reactions are the mostpromising transmutation reactions.
--> Databases on neutron capture and/or fission reaction
cross sections for MAs, LLFPs, and related nuclides
are indispensable for developing the transmutation
technology.
# The accuracy of nuclear databases for those nuclides isquite poor at the present time.
--> The improvement of the database accuracy isan urgent task.
4

2. Present Status of the Accuracy of Nuclear
Databases for MAs and LLFPs
Nuclear Databases in the WorldJENDL-4.0: Japanese Evaluated Nuclear Data Library
ENDF/B-VII.1: Evaluated Nuclear Data File
JEFF-3.1.1: Joint Evaluated Fission and Fusion Library52. Present Status of the Accuracy of Nuclear
Databases for MAs and LLFPs

Evaluated Error of JENDL-4.0: 4.8%

6

2. Present Status of the Accuracy of Nuclear
Databases for MAs and LLFPs

Evaluated Error of JENDL-4.0: 5.7%7

2. Present Status of the Accuracy of Nuclear
Databases for MAs and LLFPs

Evaluated Error of JENDL-4.0: 5.7%
Measurement at GELINA: ND2013
8

2. Present Status of the Accuracy of NuclearDatabases for MAs and LLFPs

Evaluated Error: 7.0%

243Am92. Present Status of the Accuracy of Nuclear
Databases for MAs and LLFPs

Capture cross sections of 99Tc10

2. Present Status of the Accuracy of Nuclear
Databases for MAs and LLFPs
Capture cross sections of 107Pd

11

2. Present Status of the Accuracy of Nuclear
Databases for MAs and LLFPs
Capture cross sections of 79Se

12

2. Present Status of the Accuracy of Nuclear
Databases for MAs and LLFPs# Accuracy at the present moment:
5% - 100%# Accuracy needed for the development ofNuclear Transmutation Technology:
3% - 5%13

3. Cross Section Measurements
for MAs and LLFPs# Problems in Measurements for MAs and LLFPs- Isotopic and Chemical Impurities in Samples*(Preparation of High-Purity Sample is essential.)--> Impurity identification is necessary.
--> Measurements are required for Impurities.
- Radioactivity of Sample--> Small amount of sample--> Intense and Pulsed Neutron Source*Samples of MAs and LLFPs are chemically extracted fromspent fuel. No isotopic separation is usually performed.
14

3. Cross Section Measurementsfor MAs and LLFPs- Intense and Pulsed neutron sources:# Electron Linear Accelerators: Photo-Neutron Sources
ORELA, GELINA, KURRI-LINAC, etc. (40 - 200 MeV)
0.01 - 0.001 neutron/electron# Proton Linear Accelerators (+ Synchrotron): Spallation
Neutron Sources
LANCE, n_TOF, J-PARC/MLF, etc. (0.8 - 20 GeV)
20 - 300 neutrons/proton153. Cross Section Measurements
for MAs and LLFPs

Spallation Neutron Sources- LANSCE: 0.8 GeV protons + W target (80 KW)
LANSCE: Los Alamos Neutron Science CenterLujan Center- n_TOF at CERN: 20 GeV + Pb target (9 KW)- MLF at J-PARC: 3 GeV protons + Hg target (>200 KW)
J-PARC: Japan Proton Accelerator Research Complex
MLF: Material and Life Sciences Experimental Facilities
163. Cross Section Measurements
for MAs and LLFPs- LANSCE (Lujan)
Capture, Fission and Inelastic Cross Sections,DDX- n_TOF
Capture and Fission Cross Sections- ANNRI* at J-PARC/MLF
Capture Cross Sections of MAs, LLFPs, etc.
# Th, U, Pu and unsealed RI are not usable in MLF* ANNRI: Accurate Neutron-Nucleus Reaction Measurement Instrument173. Cross Section Measurements
for MAs and LLFPs

High Intensity
200 kW
80 kW
9 kW

K. Kino et al., NIM-A, 626, 58 -66 (2011).

18

3. Cross Section Measurements
for MAs and LLFPs
LANSCE(Los Alamos Neutron Science Center),“http://michael.e.gruchalla.org/WebpageImages/Lansce1.jpg”

Lujan Neutron
Scattering Center19

3. Cross Section Measurements
for MAs and LLFPs

LANSCE Activity Report 2010,
http://lansce.lanl.gov/news/activityreport/
LANSCE%20Activity%20Report%20201
0.pdf

20

3. Cross Section Measurements
for MAs and LLFPs
DANCE
Detector for Advanced
Capture Experiments

http://lansce.lanl.gov/lujan/instruments/DANCE/pdfs/DANCE.pdf
21

3. Cross Section Measurements
for MAs and LLFPs
EAR-2 underconstruction

EAR-1“http://pceet075.cern.ch/ “CERN n_TOF Facility: Performance Report”

22

3. Cross Section Measurements
for MAs and LLFPs
TAC: Total
Absorption
Calorimeter
40 BaF223

3. Cross Section Measurements
for MAs and LLFPs
Parameters
Dimensions:20x20 cm2
Isobutane gas:
7 mbarHigh Voltage:
500-600 V
Gap between electrodes: 3mmElectrode thickness:
1.5 µm (Mylar+Al)
Deposit thickness:
100-300 µg/cm2
Backing thickness:
0.1 µm (Al)1.5 µm (Mylar)
Fission event identification:
T1 in coincidence with T2
1 anode: Mylar foil Al-plated
2 cathodes with 2mm strips
Delay between strips:
3 ns
 Position sensitive 5 channels/detector
Construction by:
IN2P3 (IPN Orsay)

Parallel Plate Avalanche Counters PPACs

24

3. Cross Section Measurements
for MAs and LLFPs
Materials and Life Science
Experimental Facility

Nuclear and Particle Physics
Experimental Facility

Nuclear
Transmutation

Neutrinos to SK
50 GeV Synchrotron(0.75 MW)Linac(350m)

3 GeV Synchrotron(25 Hz, 1MW)

J-PARC25

3. Cross Section Measurements
for MAs and LLFPs
Building dimension :Width : 70m
Length : 146m

Height : 30m
Exp. Hall Height : 22m

Target remote handling room

Cooling systems(Basement)

23 neutron beam lines will be Installedin experimental halls under present design.

MLF

26

3. Cross Section Measurements
for MAs and LLFPs

ANNRI (July, 2009)27

3. Cross Section Measurements
for MAs and LLFPs

ANNRI

28

3. Cross Section Measurements
for MAs and LLFPs

Large Ge detector array

Lead shield– Two cluster Ge detectors: 7 crystals for each
– Eight coaxial Ge detectors– BGO anti-Compton detectors
Shielding– Borated rubber sheet– 6LiH– Lead shields



Data acquisition system– Digital data processing– Pulse height andTOF are recorded
sequentially– Time resolution= 10 nsec

4π Ge Spectrometer

Ge29

3. Cross Section Measurements
for MAs and LLFPs







Use for:– Complementary use to Ge array– Measurement in the high energy
rangeDetectors– 90°detector: 13” diam. × 8” long
– 125°detector: 8” diam. × 8” longShielding– Borated polyethylene, Pb, 6LiH, Cd
Data acquisition– Multi-stop time digitizer– TOF, pulse height, pulse width arerecorded sequentiallyNaI(Tl) Spectrometer30

4. A Japanese Nuclear Data Project# Title of Project
Systematic Study on Neutron Capture Reaction Cross
Sections for the Technological Development of Nuclear
Transmutation of Long-Lived Nuclear Wastes# Objective of Project
To contribute to the improvement of nuclear databaseaccuracy, by making the precise measurements ofcapture cross sections of Long-Lived Nuclear Wastes(LLNW), analyzing the measured results theoretically,
elucidating the capture reaction mechanism of LLNW,
and supplying reliable calculated capture cross sections
for all LLNW and in the whole neutron energy region.
# Term of Project
From June, 2010 to March, 201531

4. A Japanese Nuclear Data Project
Project Representative

Measurement @Kyoto U

Measurement
using Ge Array

Measurement @J-PARC/MLF/ANNRI

Improvement ofNeutron Beam

Measurement @Tokyo Tech

TheoreticalAnalysis

Measurement
using NaI(Tl)

Structure of Project32

4. A Japanese Nuclear Data ProjectMA

Radioactive samples ofMAs and LLFPs wereprepared.
All samples are sealedin Al or Ti containers.

RadioactiveSamples

Half Life

Decay
ModeActivity(Bq)

Net Weight(mg)Np-237

2.1 ×106 y

α

26M
5.2M
1M

1000
200
38Am-241

4.3 ×102 y

α

0.95G

7.5Am-243

7.4 ×103 y

α

0.95G

128

Cm-244

1.8 ×10 yα

1.8G×60.6×6

Cm-246

4.4 ×103 yα

1.8G×4

1.1×4

Half Life

Decay
ModeActivity(Bq)

Net Weight(mg)Zr-93

1.5 ×106 yβ−

47M

472

Tc-99

2.1 ×105 yβ−

50M

78

Pd-107

6.5 ×106 yβ−

380k

20I-129

1.6 ×103 yβ−

3M404

LLFP

Samples of important stable
isotopes were also prepared.

33

Experiments of 244,246Cm- Samples and Measurement Conditions Outside
9mmΦ 1.5mmt
Inside5mmΦ 0.5mmt
Table 1 The isotopic composition of the244Cm sample or the 246Cm sample.
244Cm sample

244Cm
245Cm
246Cm
247Cm
248Cm

TIMS (mole%)
90.1±1.7
2.71±0.34
7.22±0.34
N.D.
N.D.

246Cm sample

TIMS (mole%)
27.5±0.5
1.06±0.28
59.4±1.3
2.9±0.4
9.10±0.24

Samples:
Cm-244 (T1/2=18.1y: MA)
Net weight = 0.6 mg
Activity = 1.8 GBq
Measurement Periods: 64 hours
Cm-246 (T1/2=4753y: MA)
Net weight = 2.1 mg
Activity = 12.1 MBq (244Cm: 1.7GBq)
Measurement Periods: 94 hours
Both of the samples
Chemical form = CmO2
Container = Al capsule
For the background estimation, a dummycase (Al 278mg) and a blank sample wasmeasured for 48 and 44 hours.
34Capture Cross Sections of 244Cm

A. Kimura et al., J. Nucl. Sci. Technol., 49, 708-724 (2012)
Only one set of cross section data for 244Cm (n,γ) was reported in 1971[1].
The results of theresonance peaks
under 20-eV are also
the first experimental
results in the world.

First DATA

[1]M. S. Moore et.al. , Physical Review C, 3, 1656 (1971).

35

Capture Cross Sections of 246Cm

A. Kimura et al., J. Nucl. Sci. Technol., 49, 708-724 (2012)
Only one set of cross-section data of 246Cm (n,γ) was reported in 1971[1].
The results of theresonance peaks
under 50-eV are thefirst experimental
results in the world.

First DATA

[1]M. S. Moore et.al. , Physical Review C, 3, 1656 (1971).

36Capture Cross Sections of 237Np

K. Hirose et al., J. Nucl. Sci. Technol., 50, 188-200 (2013)37

Capture Cross Sections of 241Am
H. Harada et al., ND2013

8000

Cross Section (b)eng (eV) vs sigma/GE, LAS vs Sig, LAS *1.03

6000

4000

2000

00.1

1Neutron Energy (eV)665 [b] at 25.3 meV (DANCE) was normalized as 684.87 [b]38Capture Cross Sections of 107Pd
S. Nakamura et al., ND2013

3.9-eV Res. --> 105Pd
5.2-eV Res. --> 109Ag

39

5. Summary# It was explained that databases on neutron capture and/orfission reaction cross sections for MAs, LLFPs, andrelated nuclides were indispensable for developing thenuclear transmutation technology.
# The present status of the accuracy of nuclear databasesfor MAs and LLFPs was briefly reviewed.
# A general view of cross section measurements for MAs
and LLFPs using SNSs was taken.
# A Japanese nuclear data project was explained.

40Thank you for your attention
Collaborators

Hokkaido Univ.: Y. Kiyanagi (moved to Nagoya Univ.), K. Kino
Japan Atomic Energy Agency: H. Harada, S. Nakamura, A. Kimura, N. Iwamoto
Tokyo Institute of Technology: T. Katabuchi
Kyoto University: J. Hori, H. Yashima
This Work was supported by JSPS KAKENHI Grant Number 22226016.
41