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Detectors for the measurement of ionizing

For the measurement of radiation, the following reactions during the irradiation of matter are predominantly utilized:

Ionization in gases (, proportional flow counter, release counter)

Scintillation in solids and liquids (- and - scintillation counters)

Ionization in solids (semiconductor-detectors)

1 Detectors for the measurement of

Ionization of gases (gas-filled detectors)

Ionization chamber: 50 – 300 V, air, no secondary ionization

2 Detectors for the measurement of ionizing radiation

Geiger-Müller Counter

GM counter: ≥ 800 V, Argon, cascade is generated (1010 electron pairs)

Quench gas is needed (Cl2) Only count information can be recorded, no energy Dead time: time interval after a pulse during which the counter is insensitive to further ionizing events Higher count rates mean more counts will be missed Geiger-Müller counters are most suitable for measuring

high-energy  radiation (Emax >1MeV)

3 Detectors for the measurement of ionizing radiation

Proportional Flow Counter

Count rate and energy information on the incident radiation can be obtained : 300 – 800 V, argon or , electron cascade is Discerning of alpha from beta generated (106 electron pairs) radiation

Total charge is proportional to the Especially suited for measuring energy deposited - and -emitters 4 Detectors for the measurement of ionizing radiation

Scintillation

Conduction Band

Band Scintillation gap

Valence Band

Scintillation is the property of Inorganic contain luminescence when exited by dense high Z materials ionizing radiation  They are very efficient at detecting X- and -rays The energy of the original signal is preserved through the PMT, but precision is lost  poor energy resolution 5 Detectors for the measurement of ionizing radiation

Solid Scintillation Detectors

In order to absorb the largest possible amount of the -radiation, thick crystals with large densities are used; e.g. crystals doped with (ρ =3,67g·cm-3).

By using organic crystals like , trans-stilbene or p-terphenyl,  radiation can be detected.

6 Detectors for the measurement of ionizing radiation

Scintillation / - (COBRA 5002)

Analytical Method: Quantitative

Detector: Thallium-activated sodium iodide crystal (through-hole design)

Manual Region: 15 – 2000 keV (e.g. Tc-99m 140 keV)

Efficiency: >72% for I-125 (others have to be distinguished)

7 Detectors for the measurement of ionizing radiation

Liquid Scintillation Detectors Primary Secondary Scintillators: Scintillators: 320 – 360 nm 410 – 470 nm

O N N PM Tube

Counter

O

N

Aromatic solvent in the scintillation cocktail: Absorbs the kinetic energy from a charged particle and transfers the energy to the primary molecules. 8 Detectors for the measurement of ionizing radiation

Liquid Scintillation Detectors

Quenching is the loss of counts due to sample or cocktail characteristics

Chemical Quenching Color Quenching Chemical quenchers absorb Color quenchers absorb light in radioactive energy before it is the range of the wavelength converted to light. emitted by the scintillator. Chemical quenchers reduce The number of emitted is the number of photons not changed, but the number generated by each β-particle. reaching the is reduced.

9 Detectors for the measurement of ionizing radiation

Liquid Scintillation Detectors

Analytical Method: Quantitative / “Qualitative”

Scintillation Cocktail: ULTIMA Gold XR Compatible with alkaline samples High holding capacity (up to 50%) High quench resistance High (up to 50% for H-3) -Spectra are recorded

10 Detectors for the measurement of ionizing radiation

Semiconductor Detector

Ionizing radiation produces electron-hole pairs as it passes through a

The number of electron-hole pairs is proportional to the energy transmitted by the radiation to the semiconductor http://nsspi.tamu.edu/NSEP

Measuring the number of electron-hole pairs (pulse height) allows the energy of the incident radiation to be found

Excellent energy resolution

11 Detectors for the measurement of ionizing radiation

Semiconductor Detector

Measurement of natural probes (Elemental Analysis)

Measurement of probes after activation

12 Detectors for the measurement of ionizing radiation

Semiconductor Detector

Measurement of natural probes (Elemental Analysis)

Measurement of probes after neutron activation

Aeroradiometrics Whole-body counter @ PSI

13 Detectors for the measurement of ionizing radiation

Relationship between activity and counting rate?

The net counting rate (RN) is proportional to the activity (A) of the sample and the average number of the emitted quanta per decay ()

RN = f · A · 

f = fG · fA · fS · fR · fi

fG: Geometric factor

fA: Absorption factor

fS: Self absorption factor

fR: Backscattering factor

fi: Response probability 14 Nuclear Forensic Science

„Analysis of intercepted illicit nuclear or radioactive material and any associated material to provide evidence for nuclear attribution.“ Nuclear Forensics Support, 2006. IAEA Nuclear Security Series No. 2. http://www-pub.iaea.org/MTCD/publications/PDF/Pub1241_web.pdf

“Scientific analysis of nuclear or other radioactive material, or of other evidence that is contaminated with radioactive material in the context of legal proceedings, including administrative, civil, criminal or international Law.” Nuclear Forensics in Support of Investigations, IAEA Nuclear Security Series No.2

“Analysis of nuclear material of unknown origin.”

K. Mayer, M. Wallenius, and Z. Varga, Chem. Rev. 2013, 113, 884−900

15 Nuclear Forensic Science

How to provide evidence for nuclear attribution?

What can be analyzed?

Isotopic Signatures of Plutonium and Uranium

Age Dating

Chemical Impurities

Morphology of Nuclear Material Powders

16 Nuclear Forensic Science

Isotopic Signatures Uranium and plutonium are the materials of primary concern

- - 238U (n, ) 239U  239Np  239Pu (n, )(n,240Pu ) 241Pu (n, ) 242Pu

-

(n,2n) fission 241Am

- 237U  237Np (n, ) 238Np 238Pu

(n, )

(n, ) 235U 236U The probability of the different neutron reactions (capture and fission) is a function of the neutron energy Different types of reactor show different neutron energy distributions The isotopic profile of plutonium can serve as signature of the type of reactor it was produced from 17 Nuclear Forensic Science

Isotopic Signatures Uranium and plutonium are the materials of primary concern

- - 238U (n, ) 239U  239Np  239Pu (n, )(n,240Pu ) 241Pu (n, ) 242Pu

-

(n,2n) fission 241Am

- 237U  237Np (n, ) 238Np 238Pu

(n, )

(n, ) 235U 236U Determination of the reactor class (242Pu compared to 240Pu)

Date of discharge (241Pu relationship to 240Pu and 242Pu)

Time since the last chemical processing (241Am compared to 241Pu) 18 Nuclear Forensic Science

Production date or age

Time elapsed since the last chemical processing of the material

Can be distinguished by daughter/ parent ratio measurements (s. radio chemical equilibrium)

sample type chronometer highly enriched 214Bi/234U uranium 230Th/234U 231Pa/235U uranium oxides 230Th/234U uranium ore 228Th/232Th concentrates

19 Synthesis of Elements

Heaviest stable element is Bismuth Holes in the periodic Table: Technetium, Promethium 20 Synthesis of Elements

Artificial elements

96 2 97 1 42Mo 1H 43Tc0 n Molybdenum Technetium

209 4 211 1 83Bi 2 He 85 At 20 n Bismuth Astatinium

230 1 223 4 Thorium Francium 90Th1H 87 Fr 22 He

21 Synthesis of Elements

Synthesis of Trans-Uranium Elements

n, - 238 239 239 McMillan 1940 U U Np (fission product)

n,2n - 238U 237U 237Np - 235U n, n, 237U 237Np

d,2n - 238U 238Np 238Pu Seaborg 1940

- 239Pu n, n, 241Pu 241Am Seaborg 1944

n, - 241Am 242Am 242Cm Seaborg 1944

n 242Cm 245Cf Thompson 1950

22 Synthesis of Elements

Synthesis of Trans-Uranium Elements

26Mg 248Cm 274Hs 270Hs

1·1017 1·1016 5·106 1 projectiles on target compound nuclei atom

23 Synthesis of Elements

Synthesis of Trans-Uranium Elements

24 Synthesis of Elements

Synthesis of Trans-Uranium Elements

atomic no. element name symbol

101 mendelevium Md 102 No

103 Lr 104 rutherfordium Rf

105 dubnium Db

106 seaborgium Sg

107 bohrium Bh

108 Hs 109 meitnerium Mt Current Periodic Table of the Elements with IUPAC approved 110 darmstadtium Ds numbering of groups and element symbols. The names for 111 roentgenium Rg elements 114 (, Fl) and 116 (Livermorium, Lv) suggested by the team of discoverers have recently been 112 Cn officially accepted by IUPAC. 113 ununtrium Uut 114 flerovium Fl 115 ununpentium Uup 116 livermorium Lv 117 ununseptium Uus 118 ununoctium Uuo

Andreas Türler; Valeria Pershina; Chem. Rev. 2013, 113, 1237-1312. 25