Nuclear Measurements

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Nuclear Measurements Roland Schenkel Acting Director General Joint Research Centre, European Commission, Brussels http://www.jrc.cec.eu.

1 Nuclear Measurements Roland Schenkel Acting Director General Joint Research Centre, European Commission, Brussels IAEA SCIENTIFIC FORUM 2005 Nuclear Science: Physics Helping the World September 2005 Vienna, Austria Session: Developing advanced materials and technologies

2 JRC s Mission to provide customer-driven scientific and technical support for the conception, development, implementation and monitoring of EU policies the JRC functions as a centre of science and technology reference for the EU, independent of special interests, private and national

The structure of the JRC 7 Institutes in 5 Member States 2300 staff 300 M /y budget + 40 M income IE - Petten The Netherlands -Institute for Energy IRMM - Geel Belgium - Institute for Reference

3 The structure of the JRC 7 Institutes in 5 Member States 2300 staff 300 M /y budget + 40 M income IE - Petten The Netherlands -Institute for Energy IRMM - Geel Belgium - Institute for Reference Materials and Measurements ITU - Karlsruhe Germany - Institute for Transuranium Elements IPSC - IHCP - IES - Ispra Italy - Institute for the Protection and Security of the Citizen - Institute for Health and Consumer Protection - Institute for Environment and Sustainability IPTS - Seville Spain - Institute for Prospective Technological Studies

4 2. Challenges and opportunities in nuclear science and measurements 2.1 Basic Nuclear Physics 2.2 Basic Materials Science 2.3 Examples of nuclear measurements for different applications

GELINA: neutron time-of-flight facility very high energy resolution energy range 10 mev 20 MeV Facilities for nuclear data measurements Neutron source U Sample 150 MeV LINAC total-absorption capture

5 GELINA: neutron time-of-flight facility very high energy resolution energy range 10 mev 20 MeV Facilities for nuclear data measurements Neutron source U Sample 150 MeV LINAC total-absorption capture inelastic scattering neutron emission light charged-particles fission σ abs (n,γ) (n,n'), (n,n'g) (n,2n), (n,2ng) (n,a), (n,p) (n,f) Cooperations: CEA (Cadarache, Saclay), CNRS-IN2P3 (Orsay, Bordeaux, IReS Strasbourg), INFN (Trieste, Bari), CIEMAT, Oak Ridge Ntl. Lab., Universities Bucharest, Delft, Gent, Sofia, Torino, Uppsala, Valencia, Vienna

6 Th-U fuel cycle first direct measurement of neutron-induced fission of 233 Pa (T 1/2 =27 d), collab U. Örebro comparison of 233 Pa(n,f) reaction to surrogate reaction 232 Th( 3 He,pf) evaluated nuclear data files and a new calculation (red curve), collab. U. Bucharest Data are being included in IAEA-CRP F "Evaluated nuclear data for the Th-U fuel cycle" Phys. Rev. Lett. 88 (2002) ; Nucl. Phys. A733 (2004) 3 Phys. Rev. C69 (2004) R ; Nucl. Phys. A740 (2004) 3

7 Accurate standards 10 B(n,α) comparison with previous measurements and evaluated data files collaboration with IPPE, Obninsk Cross-section (barn) 0,7 0,6 0,5 0,4 0,3 0,2 10 B(n,α) 7 Li = 10 B(n,α 0 +α 1 ) 7 Li - ENDF/B-VI=JEFF-3.0 (eval) - JEF-2.2 (eval) - JENDL-3.3 (eval) - Friesenhahn (1974) (exp) - Davis (1961) (exp) - Bichsel (1957) (exp) - Zhang (2002) (exp) - Giorginis-Khriatchkov IRMM (2002) (exp) - Giorginis-Khriatchkov IRMM (2004) (exp) 0,1 0,0 0,5 1,0 1,5 2,0 2,5 3,0 3,5 4,0 4,5 5,0 5,5 6,0 Neutron energy (MeV) Data are being included in IAEA-CRP F "Improvement of the standard cross-sections for light elements"

Laser induced nuclear reactions fission products Objectives γ with energy 1-30MeV photofission of U, Th, Np, Am, Pa, and Pu isotopes (γ, xn) reaction on long-lived fission products such as 99 Tc and

8 Laser induced nuclear reactions fission products Objectives γ with energy 1-30MeV photofission of U, Th, Np, Am, Pa, and Pu isotopes (γ, xn) reaction on long-lived fission products such as 99 Tc and 135 Cs, 129 I neutrons Target Nucleus e.g. U, Th Experiments performed laser induced-photofission of 238 U and 232 Th. Photo-transmutation of 129 I. (Appl. Phys. B. (2003) J. Magill et al. «Laser transmutation of 129 I») (J. Phys. D: Appl. Phys. 36 (2003) L79 L82. K.W.D. Ledingham et al. «Laser-driven photo-transmutation of 129 I - a long-lived nuclear waste product») (Europhys. Lett (2003) H. Schwörer et al. «Fission of actinides using a tabletop laser») first trials on 99 Tc

cm -2 VULCAN giant pulse laser at Rutherford lab.

9 The Lasers David vs. Goliath.. Tabletop laser at Jena 15 TW Ti:sapphire laser energy on target about 0.5 J, within a pulse duration of 80fs High repetition rate 10 Hz W.cm -2 VULCAN giant pulse laser at Rutherford lab. Glass laser system operating at over 100 TW can deliver pulses with energy on target up to 100 J with pulse length about 1ps Repetition rate: one shot every 20 minutes W.cm -2

10 Potential Medical Applications: GSI heavy ion radiotherapy. The Tumour situated in the centre of the brain is treated directly by depositing the energy in this region

11 Potential Medical Applications: Ion beam Therapy: Lead ions (430 MeV), C ions (80 MeV), protons (40 MeV) have been produced. GSI heavy ion radiotherapy. The Tumour situated in the centre of the brain is treated directly by depositing the energy in this region

12 Potential Medical Applications: Ion beam Therapy: Lead ions (430 MeV), C ions (80 MeV), protons (40 MeV) have been produced. GSI heavy ion radiotherapy. The Tumour situated in the centre of the brain is treated directly by depositing the energy in this region

13 Potential Medical Applications: Ion beam Therapy: Lead ions (430 MeV), C ions (80 MeV), protons (40 MeV) have been produced. GSI heavy ion radiotherapy. The Tumour situated in the centre of the brain is treated directly by depositing the energy in this region

Production of short-lived isotopes for PET ( 18 F) (need 1 khz repetition rate and 1 J per

14 Potential Medical Applications: Ion beam Therapy: Lead ions (430 MeV), C ions (80 MeV), protons (40 MeV) have been produced. Production of short-lived isotopes for PET ( 18 F) (need 1 khz repetition rate and 1 J per pulse =>10 9 Bq) GSI heavy ion radiotherapy. The Tumour situated in the centre of the brain is treated directly by depositing the energy in this region

15 2. Challenges and opportunities in nuclear science and measurements 2.1 Basic Nuclear Physics 2.2 Basic Materials Science 2.3 Examples of nuclear measurements for different applications

16 Magnetism versus superconductivity in groups of elements with partially-filled d- and f-shells Courtesy: Smith, LANL

17 Atomic volume of d and f series Notice how light actinides are smaller than rareearths (4f) and follow a curve like the d series. The heavier actinides are more rare-earth like.

18 Discovery of Pu-based superconductivity above 18K in PuCoGa 5 Sarrao et al., Nature 420 (2002) 297 Why Pu? Plutonium is at a crossover in electronic properties PuCoGa 5 sample mounted for electrical resistivity measurements Question: Is the superconductivity in this system magnetically mediated? 0 30 Magnetic Susceptibility (emu/mol) PuCoGa 5 Bulk material Magnetic Susceptibility Magnetic Susceptibility Electrical Resistivity ZFC FC Electrical Resistivity (??? cm) Critical Temperature (K) High-temperature superconductors PuCoGa 5 Heavy Fermion superconductors Temperature (K) PuCoGa as the missing step between 5 magnetically mediated/heavy- fermion superconductors and high-temperature copper-oxide superconductors? 15

19 Compressibility of actinide elements new Cm (III) phase Note major difference between uranium and Cm and Am, especially at low P Experiments done on a few µg at world s most advanced synchrotron in Grenoble, France it was demonstrated that this new phase (Cm (III)) is stabilized by magnetism, as has been found previously in only two other cases (Fe, Co) S. Heathman et al. Science 309 (2005) 110

Fission products & uranium vapour release from irradiated UO 2 (65 GWd/t) during an accident 1.1 137 Cs 1.

20 Fission products & uranium vapour release from irradiated UO 2 (65 GWd/t) during an accident Cs Te Fraction released/vaporised LaO 129 I 136 Xe 138 Ba 90 Sr UO Temperature, K

21 THERMAL CONDUCTIVITY OF IRRADIATED UO 2 AS A FUNCTION OF BURNUP AND TEMPERATURE Conductivity, Wm -1 K temperature during previous burn-up accumulation T irr = 1500K T irr = 600 K Fresh Fuel The fuel thermal conductivity dramatically decreases with burnup. The effect is stronger if the fuel is irradiated at low temperature Temperature(K) at the considered instant Burnup (GWd/t) 0 Most of this damage effect is permanent and only a small part of it is recovered by thermal annealing

22 Fission gas release effects during a fuel T-transient ABSOLUTE 136 Xe AMOUNT (normalised) Centre Median Rim Rim structure Cladding+corrosion products Ordinary fuel structure Sample position ANNEALING TEMPERATURE, K Burn-up (GWd/t) ~Irrad. Temp. ( 0 C) H diff (ev/atom) Periphery 88 ~ ± 0.2 Median 72 ~ ± 0.3 Center ~ ± 0.4 Atomic migration energy

23 Safety of Nuclear Fuel mechanical examination of irradiated fuel

24 Safety of Nuclear Fuel mechanical examination of irradiated fuel

25 Safety of Nuclear Fuel mechanical examination of irradiated fuel Microstructure, micro-hardness and lattice parameter variations at the fuel periphery (rim zone) LWR-fuel (67 GWd/tM) - Initial enrichment: 4.2 % 235 U

26 Safety of Nuclear Fuel mechanical examination of irradiated fuel Microstructure, micro-hardness and lattice parameter variations at the fuel periphery (rim zone) LWR-fuel (67 GWd/tM) - Initial enrichment: 4.2 % 235 U

27 Safety of Nuclear Fuel mechanical examination of irradiated fuel Microstructure, micro-hardness and lattice parameter variations at the fuel periphery (rim zone) LWR-fuel (67 GWd/tM) - Initial enrichment: 4.2 % 235 U

28 Safety of Nuclear Fuel mechanical examination of irradiated fuel 1 0 µm Microstructure, micro-hardness and lattice parameter variations at the fuel periphery (rim zone) LWR-fuel (67 GWd/tM) - Initial enrichment: 4.2 % 235 U

29 Safety of Nuclear Fuel mechanical examination of irradiated fuel 1 0 µm Microstructure, t micro-hardness and lattice parameter variations at the fuel periphery (rim zone) LWR-fuel (67 GWd/tM) - Initial enrichment: 4.2 % 235 U

30 2. Challenges and opportunities in nuclear science and measurements 2.1 Basic Nuclear Physics 2.2 Basic Materials Science 2.3 Examples of nuclear measurements for different applications

31 The criticality accident at the JCO nuclear fuel plant in Tokai-mura, 1999 Thermal neutrons fluence values (106 cm-2) at the sampling positions, for 20 hours exposure. Normal value is 180 cm m: evacuation zone m N 500 m 300 m 100 m JCO < < <24 <14 7 <58 The Japanese investigation team requested support with measurements of 51Cr, 60Co and 59Fe in table spoons.

2003-2-3 kg radioactive material was detected in a scrap metal shipment in Rotterdam harbour.

32 Illicit traffic of nuclear materials Nuclear forensic science Case Study Illicit Trafficking - Case Study : Find 26 Rotterdam On 16 th Dec kg radioactive material was detected in a scrap metal shipment in Rotterdam harbour. The shipment arrived from a dealer in Jordan. Materials sent to JRC/ITU on 10 th March 2004 and consisted of 2 bulk samples and 3 swipes.

33 Gamma spectrometry U-235 enrichment 0,7 % TIMS and MC-ICP-MS U-234 = 0,0052 % U-235 = 0,712 % U-238 = 99,283 % natural uranium, no indication of an enriched or irradiated uranium Titration U-content ~70 % Illicit traffic of nuclear materials Nuclear forensic science Results - bulk

34 Illicit traffic of nuclear materials Nuclear forensic science Results - bulk Gamma spectrometry U-235 enrichment 0,7 % TIMS and MC-ICP-MS U-234 = 0,0052 % U-235 = 0,712 % U-238 = 99,283 % natural uranium, no indication of an enriched or irradiated uranium Titration U-content ~70 % Lead isotopics Pb-204 = 1.47 % Pb-206 = % Pb-207 = % Pb-208 = % resembles natural lead, no radiogenic lead Anions (qualitative) (NO 3 ) - and (CO 3 ) 2- ICP-MS Main impurities (>1000 ppm): Al, Ca, Cr, Fe, Mg, Mo, Na, Ni, P

35 Illicit traffic of nuclear materials Nuclear forensic science Find-26: Rotterdam

36 Bulk material: natural uranium oxides with 70% U presence of (CO 3 ) 2- main impurities: Al, Ca, Cr, Fe, Mg, Mo, Na, Ni, P lead isotopic composition Illicit traffic of nuclear materials Nuclear forensic science Find-26: Rotterdam Swipes: natural uranium, Cs-137, Eu-154 and Am-241 (evidence of nuclear activities)

37 Bulk material: natural uranium oxides with 70% U presence of (CO 3 ) 2- main impurities: Al, Ca, Cr, Fe, Mg, Mo, Na, Ni, P lead isotopic composition Illicit traffic of nuclear materials Nuclear forensic science Find-26: Rotterdam What information did the analysis yield? Swipes: natural uranium, Cs-137, Eu-154 and Am-241 (evidence of nuclear activities)

38 Illicit traffic of nuclear materials Nuclear forensic science Find-26: Rotterdam Bulk material: natural uranium oxides with 70% U presence of (CO 3 ) 2- main impurities: Al, Ca, Cr, Fe, Mg, Mo, Na, Ni, P lead isotopic composition Swipes: natural uranium, Cs-137, Eu-154 and Am-241 (evidence of nuclear activities) What information did the analysis yield? Intermediate product, possibly (NH 4 ) 4 (UO 2 )(CO 3 ) 3 Impurities point to phosphate rich ores (North Africa, Middle East, USA, South Africa, Brazil) Pb isotopic composition (natural) indicates low uranium content in the ore, which is the case for P-rich ores evidence of nuclear activities corroborated intelligence information on the source of the material

39 Neptunium Flow-Sheet Verification Am 100% Np 100% HKED (XRF) [Np], [Am] Accountancy Tank HKED [U], [Pu], [Am] HLLW > 99% 1 st Extraction FP Separation With TEVA HRGS [Np]/[Pu ] Ratio % % % U-Pu Separation U Purification Pu Purification < 0.01 % U Product % % % Pu Product HRGS/XRF [Np], [Am] Purification Raffinates Legend: Process Line Key Measurement Point Analytical Determination

40 Neptunium Flow-Sheet Verification HKED (XRF) [Np], [Am] Am 100% Np 100% Accountancy Tank Np in input solution measured by γ-spec. 1.0E+07 HKED 238 Pu [U], [Pu], [Am] 241 Am TEVA-Column 42 days after separation % HLLW > 99% 1 st Extraction % % 1.0E E+05 FP Separation With TEVA HRGS [Np]/[Pu ] Ratio 237 Np 241 Pu 125 Sb 241 Pu U-Pu Separation 154 Eu 238 Pu 1.0E Pu < 0.01 % U Product U Purification % % Pu Purification 1.0E % 40 Pu Product 80 HRGS/XRF 120 [Np], [Am] Energy (kev) Purification Raffinates Legend: Process Line Key Measurement Point Analytical Determination

41 Neptunium Flow-Sheet Verification HKED (XRF) [Np], [Am] Am 100% Np 100% Accountancy Tank Np in input solution measured by γ-spec. 1.0E+07 HKED 238 Pu [U], [Pu], [Am] 241 Am TEVA-Column 42 days after separation % HLLW < 0.01 % U Product > 99% 1 st Extraction % % U-Pu 8.0E+04 Separation U Purification 6.0E % 4.0E E E E+04 FP Separation With TEVA HRGS [Np]/[Pu ] Ratio 237 Np 154 Eu 239 Pu Pu Simulated HLLW Purification NpKα 1 U = 0.48 mg/ml AmKα 1.0E+03 1 Np = 0.94 mg/ml % % Am = 1.41 mg/ml UKα 1 40 Pu 80 HRGS/XRF NpKα 2 AmKα 2 Product [Np], [Am] Energy (kev) 241 Pu 238 Pu 125 Sb 241 Pu UKα 2 Purification Raffinates 2.0E+04 U, Np, AmKβ X-Rays Legend: 0.0E+00 Process Line Energy (kev) Key Measurement Point Np in HALW measured by XRF. Analytical Determination

72 wt % of 235 Find a Needle in the Hay Stack swipe sample: billions of dust particles with low

42 Application of the method for Routine Safeguards High Performance Trace Analysis for the detection of U and Pu particles Natural U, 0.72 wt % of 235 Find a Needle in the Hay Stack swipe sample: billions of dust particles with low enriched uranium particles Strengthened Safeguards: Particle Analysis Nuclear fuel, wt% of 235 Weapons grade U, wt % of U 238 U U-235 SIMS image U-238 SIMS image

Traditional Safeguards COMPUCEA 2 nd generation : on-site U-enrichment measurements (Under IAEA SP Task A1507) Basic hardware components - Mini X-ray system, 30 kv/100 µa (Amptek, Eclipse II) - Si

43 Traditional Safeguards COMPUCEA 2 nd generation : on-site U-enrichment measurements (Under IAEA SP Task A1507) Basic hardware components - Mini X-ray system, 30 kv/100 µa (Amptek, Eclipse II) - Si drift detector, Peltier-cooled, with integrated electronics (KETEK) - Digital signal processor (Canberra DSA 1000) Digital Signal Analyser XRF Adapter X-ray controller X-ray tube Peltier cooled Si detector L-edge Adapter Total weight: ~ 6 kg

Control of Actinides in a Pyrochemical Partitioning Process Quantitative analytical methods are required in order to establish a material balance: 1) for process development and at a later stage 2)

44 Control of Actinides in a Pyrochemical Partitioning Process Quantitative analytical methods are required in order to establish a material balance: 1) for process development and at a later stage 2) for accountancy and control purposes FP Gaz (Xe, Kr) Power supply Exotic Samples Solid Cathode Argon atmosphere 773 K U deposit U, TRU U Anod e Liquid Cd cathode FP (AL, ALE, RE) LiCI - KCI Sa lt Noble metal FP, Zr Liq uid Cd

45 Application of radiometric techniques for Minor Actinides Technique K-XRF NCC Element/ isotope measured Np Am Cm Cm Isotope contribution to response* Cm % 246 Cm: 5-10% Minimum amount for assay 50 µg 70 µg Application Any sample type in liquid form mass fractions of analyte 0.02 %. 100 µg 200 ng For any type of Cm-containing samples (liquid or solid) with Pu/Cm ratios 1000 HRGS Calorimetry 237 Np 241 Am 243 Am Am Cm Am: 98% 243 Am: 2% 244 Cm: 99% 243 Cm: 1% 500 µg 10 ng 100 ng 5 mg** 200 µg** Liquid samples for absolute measurements. Low FP content for 237 Np assay. Refractory MA fuels for transmutation. Combined with NCC/HRGS for interpretation. * For typical MA isotopic composition in spent LWR/FBR fuels ** Can be lowered by factor of 10 when using microcalorimeters

46 Conclusions Nuclear science and measurement technology have made considerable progress Remains an attractive field for young scientists and engineers Need to maintain competences and facilities: strengthen cooperation with universities Materials Science: trend goes to micro-measurements of axial/radial dependence of properties (10-20µm) Laser technology opens new and innovative areas of fundamental science and applications Nuclear measurements: trend goes towards higher detection efficiency and capability to measure short-lived isotopes in very low quantities

The analysis of particles of nuclear material finding the proverbial needle in a hay stack

San Diego, 18-22 February 2010 AAAS Annual Meeting 1 The analysis of particles of nuclear material finding the proverbial needle in a hay stack AAAS Annual Meeting San Diego, February 19, 2010 Klaus Luetzenkirchen