CURRENT AND FUTURE RESEARCH IN CBRN DEFENSE AT THE IAP NAS OF UKRAINE

V. Yu. Storizhko

Round-table on WMD and Dual-use Expertise/KnowledgeRedirection and Prevention

17-18 April, 2012, Kyiv, Ukraine

Accelerator based nano-analytical facilities for material characterization

2

2 MeV electrostatic accelerator with analytical end stations (RBS, PIXE, uPIXE, PIGE, ERDA)

3

Scanning Nuclear Microprobe

Beams: H+, He+ with energy 0.2…2 MeVResolution: 2 μm with current ≈100 pAAnalytical techniques: μPIXE, μRBS, IBIC

4

Detection limits and lateral resolution of some resonant nuclear reactions

Element Nuclear reaction

Resonance energy(keV)

Resonance width(eV)

Resolution (nm)

Detection limitsppm

Hydrogen 1H(15N,αγ)15C1H(19F,αγ)16O

63856421

600045000

423

30100

Lithium 7Li(p,γ)8Be 441 12200 220 0.15

Boron 10B(α.p)13C11B(p,γ)12C

11B(p,α)8Be

1507163660

180005200

300000

3013050

500050

100

Nitrogen 14N(α,γ)18F 1531 600 2

Oxygen 18O(p,γ)15N 898633

22002100

520

5

Fluorine 19F(p,γ)16O 340 2300 25 0.1

Magnesium

24Mg(p,γ)25Al 223 <32 0,6

Aluminium 27Al(p,γ)28Si 405992

87105

1,110

100

Phosphorus 31P(p,γ)28Si31P(p,γ)32S

10181147

<300<160

10 10050

Тitanium 48Ti(p,γ)49V 1361 50 10 20

Chrome

52Cr(p,γ)53Mn 1005 9 100 5

Accelerator based isotope mass-spectrometer «Tandetron» by HVEE (The Netherlands) 6

Some applications of AMS «Tandetron»

Ratio Sensitivity Error

14C/12C 3 x 10-15 0.5 %

13C/12C 1 x 10-14 0.3 %

10Be/9Be 3 x 10-14 3 %

26Al/27Al 5 x 10-14 3 %

129I/127I 1 x 10-12 5 %

Isotopes 14CIsotopes to define: 10Be, 26Al, 129I

Possible fields of investigationsNuclear power engineering and nuclear safety environment monitoring 14C, 129IArcheology and geology objects dating 14CRadiation ecology Chornobyl accident – detection of late radiative effects in the organisms, water circulation 14C, 10Be, 129I

• Nuclear fuel-processing waste (85Kr, 99Tc, 129I)• Half-life measurement (32Si, 41Ca, 44Ti, 60Fe, 79Se, 126Sn)• Fusion plasma temperature measurement (26Al)• Neutron flux of Hiroshima bomb (36Cl, 41Ca, 63Ni (100 a))• Nuclear safety (233U(1.59 x 105 a), 236U, 237Np (2.14 x 106 a), 239Pu (2.41 x 104 a), 240Pu (6.56 x 103 a), 242Pu (3.73 x 105 a), 244Pu)

7

Complementary analytical techniques:

• X-ray diffractometers and X-ray devices for phase structural characteristics;

• Scanning electron microscope with electron probe microanalysis;

• Laser mass-spectrometers;• ICP mass-spectrometer;• ICP emission spectrometer;• Atomic absorption spectrometers for the

determination of the ppm/ppb content of minor metal impurities in samples.

8

Results of collaboration between the IAP NAS of Ukraine CERN under the CLIC Programme

Optical spectra from DC-sparc CLIC setup

Sample Cu 9(7)Strong optical line Н2 (462.9 nm)

9

Laser isotope mass-spectrometer with coordinate-sensitive detector

0 100 200 300 400

0

50

100

150

200

250

300

С(121Sb)=0,0014%

Образец М161,часть спектра олова и сурьмы

С(Sn)=0,08%, C(Sb)=0,0024%,

Интенсивность

канал

124Sn+

123Sb+

122Sn+

121Sb+

120Sn+

119Sn+

10

IAP NASU

• P464 “Development of identification techniques of uranium ores in Ukrainian deposits and their concentrates by consistent phase-chemical and radioactive balance data”

• P465 “Study of Attribution Signatures of Various Uranium Bearing Materials”

• 5728 “Development of single-ion and X-ray microbeams using an electrostatic accelerator to investigate radiation damage in cells”

Current Research in Nuclear Forensics Field

• RER 0/0/34 “Enhancing the Characterization, Preservation and Protection of Cultural Heritage Artefacts”

• CRP 17089 “Heavy Metal Transformation Dynamics in Biochemical Complexes in Trophic Chains”

• CRP 17240 “In Situ Study of Materials for Energy Applications by Means of Real-Time Ion Beams Analysis”

SCIENCE & TECHNOLOGY CENTER

IN UKRAINE

11

Investigation of final products of chemical enrichment of uranium ore

Final products of chemical enrichment of uranium ore have been studied with the scanning electron microscopy. The product is uranium oxide crystals of prismatic form. Monoclinic system of crystals is the most probable. X-ray investigation of samples with Debye technique and their elemental analysis show that crystals are identical to oxidated uraninite U4O9

SEM image of uranium oxide crystals

Debyegram of fine uranium oxide crystals mixture

12

A Study of Uraninite by PIXE Technique μ-PIXE measurements were carried out at the Scanning Nuclear Microprobe facility of the Institute of Applied Physics of the National Academy of Sciences of Ukraine, Sumy. Scanning of sections of all seven fragments of characteristic size of 100…200 μm was performed by proton beam with energy E=1.5 MeV with scan region of 50×50 pixels, step of scanning of 2 μm and 4 μm.

The maps of different elements distribution on the same area of

uraninite obtained by PIXE.

The collective PIXE spectra (in logarithmical scale) of uraninite fragment

Element

μ-PIXE

С, mass %

error, %

Na 0.057 0.01

Al 0.94 0.16

Si 3.74 0.55

P 0.99 0.26

S 0.32 0.07

Ca 9.41 0.74

V 1.08 0.1

Fe 0.08 0.03

Pb 1.27 0.11

U 63.87 0.99

Cu 0.1 0.03

Mg 0.17 0.05

The composition of Uraninite

13

Efforts in Monitoring of Trace Amounts of Transuranium Elements Isotopes

• The isotopes of transuranium elements are the most toxic and is usually the most long-lived component of the emissions of the Chernobyl accident and other radioactive waste storage facilities in Ukraine and neighboring countries of former Soviet Union.

• Of all the methods for determining the main dose-forming radionuclides (238,239,240 Pu, 241,243 Am) radiochemical separation of plutonium and, especially, americium is technically the most difficult, time-consuming and expensive task.

• In this regard, radioecological studies of pollution by isotopes of transuranium elements in Ukraine were carried out in a very limited scale: both in localisation and on isotopes content.

14

Map of Ukraine pollution americium (241Am)

2008

15

We can solve this problem!

The Institute of Applied Physics of the National Academy of Sciences of Ukraine has unique (for countries of former USSR) high-sensitive accelerator mass spectrometer AMS-1MV «Tandetron» (by HVEE , the Netherlands) with isotopic sensitivity of 10-15.The AMS allows determining the content of all transuranium elements in any samples.

This device enables us to define all known isotopes of plutonium and other actinides (238, 239, 240Pu, 241, 243Am, 237Np) that are in the samples, to determine their contents, ratio, and, hence, to clarify their origin.

16

Relevance of Establishment of Laboratory Transuranium Elements in Ukraine

• Establishment of Center for collective use for determination of Trace Amounts of Transuranium Elements on the basis of accelerator mass spectrometry laboratory in Institute of Applied Physics NAS of Ukraine will permit:

• to promote prevention of nuclear terrorism, illicit traffic and/or use of nuclear materials in Ukraine (Nuclear Forensics Program, CBRN Defense);

• to identify nuclear materials through the isotopic composition and concomitant elements;

• to study the harmful effects of the Chernobyl disaster and to provide pollution monitoring of transuranium elements in Ukraine and neighboring countries.

17

The Method of Project Implementation• Use of accelerator mass spectrometry allows simplifying the

sample preparation procedure without pre-concentration and separation of isotopes of transuranium elements.

• Using AMS for studies of environmental pollution permits reaching detection limit of 1.3 ppq for 240Pu (Reports of Lawrence Livermore National Laboratory (LLL) and other literature sources).

Project provides:• Training specialists of the IAP at LLL for 6 months.• Collaboration of specialists LLL and IAP in the optimization of

the analytical mode of the accelerator mass spectrometer and improving of analytical techniques in the IAP.

The proposed term of the project - 2 years.

18

Expected results and perspective

• Laboratory of transuranium elements will allow reliably identify nuclear materials, will improve the radioisotope researches. The Laboratory will be a deterrent for illicit traffic of any potentially dangerous nuclear materials in the territory of Ukraine and neighboring countries.

• The project provides the adaptation of existing techniques and development of new methods for determination of the isotopes concentrations of transuranium elements in the IAP NASU in collaboration with Lawrence Livermore National Laboratory (USA).

19

Thank you for your attention

V.Yu. StorizhkoDirector of the Institute of Applied Physics NAS of Ukraine,

Academician NAS of Ukraine, Professor, Doctor of Physics and Mathematics, Tel. +380 (542) 222-794, Fax: +380 (542) 223-760

E-mail: ipfmail@ipfcentr.sumy.ua