Charged Particle Reactions and Production of Medic al/Industrial Radioisotopes Muhammad Shahid Supervised by: Prof. Guinyun Kim Department of Physics, Kyungpook National University Pakistan Nuclear Regulatory Authority, Pakistan Phy.knu@gmail.com
Nuclear Data Measurement Facilities Korea Charged particle Neutron Gamma HANARO, PNF: Thermal KIRAMS – 45 MeV (p,d, α ) KIRAMS, Jeong-eup, Gyeong-ju Gyeong-ju – 100 MeV (p) Pohang Accelerator Lab. , PAL Jeong-eup – 30 MeV (p) Fast neutron (p → Li, γ→ Be) KNU (Prof. G.N.Kim) Proton, Alpha & Deuteron Neutron Gamma/Bremstrahlung Photo-fission yield Charged particle induced rea Neutron total cross section Photo cross section ction cross section Resonance integral Isomeric yield ratio
Pohang Neutron Facility Pohang Neutron Facility based o Pohang Accelerator Laboratory n 100-MeV e-linac Pohang High Energy Radiation Facility with 3.0 GeV e-linac
Parameters of 100-MeV Proton Linac at KOMAC Energy (MeV) 20 100 Features of the PEFP 100 MeV linac Peak Current (mA) 0.1 ~ 20 0.1 ~ 20 � 50 keV Injector (Ion source + LEBT) 24 * Max. Duty (%) 8 � 3 MeV RFQ (4-vane type) Max. Ave. Current (mA) 4.8 1.6 � 20 & 100 MeV DTL Pulse Width (ms) 0.05 ~ 2 0.05 ~ 1.33 � RF Frequency: 350 MHz Max. Repetition Rate (Hz 120 60 � Beam Extractions at 20 or 100 MeV ) � 5 Beamlines for 20 MeV & 100 MeV Max. Beam Power (kW) 96 160 Emmitance (mm-mrad) 0.22(x), 0.25(y) 0.3 / 0.3 SRF TB 20 MeV DTL 50 keV Injector 100 MeV DTL S e m c i o n d u c t o r Neutron Isotope Isotope 3 MeV RFQ Med. Sci. Basic Sci. Therapy Basic Sci. Biology Space Energy Nucl. Phys. Material Material
MC 50 Cyclotron at KIRAMS for Proton, Deuteron and Alpha
MC-50 Cyclotron at KIRAMS MC-50 is the first cyclotron installed in Korea. It is available to support some research es which use proton, deuteron, He-3, and He-4 beams. The MC-50 cyclotron has beam energy from 18.0 MeV to 50.5 MeV and variety in beam current from 2 nA to 60 µA . 6
MC 50 Cyclotron at KIRAMS Proton ¡beam ¡energy 45 ¡MeV Beam ¡current 100-‑200 ¡nA Irradiation ¡time 1 ¡h–30 ¡min 7
Measured Results for Proton- and Alpha-induced Reaction Cross-sections Projectile Target Investigated radionuclides Publication Proton (45 MeV) nat Ni 55,56,57,58m+g Co, 56,57 Ni NIM B 269 (2011) 1140 Proton (45 MeV) nat Pd 103,104m,104g Ag NIM B 274 (2012) 148 86,88,89g Zr, 86m+g,87g,87m,88g Y, 85g Sr, 84g Rb NIM B 271 (2012) 72 Proton (45 MeV) 89 Y Proton (45 MeV) nat Er 165,166 Tm NDS 119 (2014) 249 Proton (45 MeV) nat Hf 173,175,176,177,178m,180g Ta, 173,175,179m2,180m Hf, 172g,173,177g Lu NIM B 322 (2014) 13 Proton (45 MeV) nat Fe 55,56,57 Co, 52 Fe, 52,54 Mn, 51 Cr NIM B 322 (2014) 63 Alpha (45 MeV) nat Cd 110,113g,117m Sn, 111m,115g Cd, 108m,g;109g,110m,g;113m,114m,115m,116m,117m,g In NIM B 333 (2014) 80 Proton (45 MeV) nat Cu 62,65 Zn, 61,64 Cu, 57 Ni, 56,57,58,60 Co NIM B 342 (2015) 305 Proton (45 MeV) nat Nd 141-150 Pm, 139m,147,149 Nd, 138m,142g Pr, 139 Ce NIM B 362 (2015) 142 Alpha (45 MeV) 89 Y 89g,m,90,91m,92m Nb, 88,89 Zr, 87g,m,88,90m,91m Y NIM B 342 ( 2015) 158 Alpha (45 MeV) 93 Nb 93m Mo, 91m,92m,95m,g Nb JKPS 67 (2015) 1474 Alpha (45 MeV) 93 Nb 94-96 Tc NPA 935 (2015) 65 Alpha (45 MeV) nat Cu 66,67,68 Ga, 62,63,65 Zn, 61,64 Cu 58,60 Co NIM B 358 (2015) 160 Alpha (45 MeV) nat Ag 108m,108g,109g,110m,110g,111g In, 109g,,111m Cd, 105g,106m,110m,111g Ag JRNC311(2017)1971 Proton (45 MeV) 93 Nb 90, 93m Mo, 90, 91m, 92m Nb, 88Zr, 89 Zr, 87gY, 87mY, 88 Y Proton (45 MeV) nat Ta 175,179,180 Hf, 176,177,178m,180g Ta, 177,178 W Proton (45 MeV) 57 Co 57 Ni, 58g,57, 56 Co, 54 Mn
Experimental Steps Preparation of sample (Material selection, Foils cutting, monitor selection, nuclear data tables etc.) SRIM calculations and stac k design (Sample and monitor positi Stack composition ons in the stack) Sample preparation Sample activation (Beam energy, current and time selection ) Measurement of radioactivi ty (cooling, counting with HPGe detector Activity measurement by HPG Activation by beam line of KIR , Analysis) e Detector AMS Measurements and calculat ions (cross sections and uncertainty, et c.) Data Evaluation (comparison, In clusion in nuclear data library, uses etc.) Gamma spectrum of irradiated sample foil
Calculation of Flux using Monitor 1039.35 keV (37.9%) nat Cu( α ,x) reaction
Associated Calculations The measured flux is substituted in the following formulae to determine the un known cross section of the sample foils: ¡ ! = #↓% '(↑(#↓% +↓, ) /( 1− (↑( − #↓% +↓% ) )( 1− (↑( − #↓% +↓/ ) )0↓1 2↓1 '↓+ 3 The contribution of interfering gamma lines that are within the resolution of de tector is determined using the following formulae: ¡ 4(5↓1 1 ) = 4(5↓1 2 ) × 0(5↓1 1 ) × 2↓1 1 /0(5↓1 2 ) × ¡ 2↓1 2 The production yield was calculated form the following formulae: 6 = 2↓7 '↓, ∫ 0 ↑5▒ σ( 5 ) / ( ,5∕,; ) ↓5 ,5 λ Where Ip is flux (p/cm 2 -sec), N d is number density (atoms/cm 3 ), (dE/dx) E is st opping power (MeV/cm) and dE is E in -E out (MeV). 11
Theoretical Calculations with TALYS TENDL-2013 Input TALYS is a useful computer code that predicts nuclear reactions by simulation within the energy range 1 keV projectile a element Y - 200 MeV. The neutrons, photons, protons, deuterons, mass 089 tritons, 3 He and alpha induced nuclear reactions at any Ltarget 000 target material (Z>12) can be simulated with this code energy Energies system. Available at http://www.talys.eu/ maxlevelstar 30 partable y bins 100 best y endf y endfdetail y Popeps 1.e-12 transeps 1.e-20 transpower 15 xseps 1.e-20 spherical y recoil y recoilaverage y isomer 0.1
Details of TALYS Parameters (selected) • Ltarget 000: The target is in its ground state • maxlevelstar 30: The number of included discrete levels for the target nucleus; default 20 • partable y: Flag to write the model parameters used in a calculation on a separate file; default n • bins 100: The number of excitation energy bins; default 40 • best y: Flag to use the set of adjusted nuclear model parameters that produces the optimal fit for mea surements of all reaction channels of the nuclide under consideration. default n • endf y: Flag for the creation of various output files needed for the assembling of an ENDF formatted f ile; default n • endfdetail y: Flag for detailed ENDF information; default no for charged particles • popeps 1.e -12 : The limit for considering population cross sections in the multiple emission calculation, in mb; default 1.e -3 • transeps 1.e -20 : A limit for considering transmission coefficients in the calculation; default 1.e -8 . The p robability flux of the transmitted wave relative to that of the incident wave • transpower 15: probability of a particle tunneling through a barrier: default 5 • xseps 1.e-20: The limit for considering cross sections in the calculation, in mb; default 1.e -7 • spherical y: Flag to enforce a spherical OMP calculation (for incident charged particles); default no • recoil y: Flag for the calculation of the recoils of the residual nuclides and the associated corrections t o the light particle spectra; default no • recoilaverage y: Flag to consider only one average kinetic energy of the recoiling nucleus per excitatio n energy bin; default no • isomer 0.1: The definition of an isomer in seconds default 1. In the discrete level database, the lifetime s of most of the levels are given. With isomer, it can be specified whether a level is treated as an isome r or not. 13
Reaction Products from nat Cu(p,x) and nat Cu( α ,x) Reaction ¡ 27 90 nat Cu(p,x) 58(m+g) Co nat Cu( α ,x) 58(m+g) Co 24 80 Williams et.al. 1967 S.S.Rattan et.al. 1986 21 70 Acerbi et.al. 1976 Cross Section (mb) M.J.Ozafran et.al. 1989 Greenwood et.al. 1984 Cross Section (mb) Kopecky et.al. 1985 V.N.Levkovskij et.al. 1991 60 18 Aleksandrov et.al. 1987 TENDL-2013 Mills et.al. 1992 This work 50 15 Ido et.al. 2002 Yashima et.al. 2003 40 12 ¡ TENDL-2013 This Work 30 9 20 6 63 Cu(p, α np) 58 Co 65 Cu(p, α tn) 58 Co 10 E th =16.5 MeV 3 65 Cu( α ,2 α 3n) 58 Co E th =26.0 MeV E th =36.2 MeV 0 0 15 20 25 30 35 40 45 50 30 32 34 36 38 40 42 44 46 48 50 Proton Energy (MeV) Alpha Energy (MeV) ¡ ¡ 4.0 nat Cu(p,x) 60 Co 14 nat Cu( α ,x) 60 Co 3.5 Williams et al. 1967 12 M.J.Ozafran et.al. 1989 Gruetter et al. 1982 3.0 This Work Greenwood et al. 1984 Cross Section (mb) Cross Section (mb) 10 TENDL-2013 Mills et al. 1992 2.5 Michel et al. 1997 TENDL-2013 8 2.0 This Work ¡ ¡ ¡ 6 1.5 4 1.0 65 Cu(p,t 3 He) 60 Co 65 Cu( α ,n2 α ) 60 Co E th =28.6 MeV 63 Cu(p,p 3 He) 60 Co 2 E th =17.1 MeV 0.5 E th =19.2 MeV 0.0 0 20 24 28 32 36 40 44 48 5 10 15 20 25 30 35 40 45 50 Proton Energy (MeV) Alpha Energy (MeV) ¡
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