Charged Particle Reactions and Production of Medic al/Industrial - - PowerPoint PPT Presentation

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

KNU (Prof. G.N.Kim)

Neutron Gamma/Bremstrahlung Proton, Alpha & Deuteron

Charged particle induced rea ction cross section Neutron total cross section Resonance integral Photo-fission yield Photo cross section Isomeric yield ratio

Neutron Gamma Charged particle

KIRAMS – 45 MeV (p,d,α) Gyeong-ju – 100 MeV (p) Jeong-eup – 30 MeV (p) HANARO, PNF: Thermal KIRAMS, Jeong-eup, Gyeong-ju , PAL Fast neutron (p→Li, γ→Be) Pohang Accelerator Lab.

Korea

Pohang Accelerator Laboratory Pohang Neutron Facility based o n 100-MeV e-linac Pohang High Energy Radiation Facility with 3.0 GeV e-linac

Pohang Neutron Facility

50 keV Injector 3 MeV RFQ 20 MeV DTL 100 MeV DTL SRF TB

Isotope S e m i c

• n

d u c t

• r
• Med. Sci.

Biology Energy Material Isotope Therapy Neutron Basic Sci. Space

• Nucl. Phys.

Material Basic Sci. Energy (MeV) 20 100 Peak Current (mA) 0.1 ~ 20 0.1 ~ 20

• Max. Duty (%)

24* 8

• Max. Ave. Current (mA)

4.8 1.6 Pulse Width (ms) 0.05 ~ 2 0.05 ~ 1.33

• Max. Repetition Rate (Hz

) 120 60

• Max. Beam Power (kW)

96 160 Emmitance (mm-mrad) 0.22(x), 0.25(y) 0.3 / 0.3

Features of the PEFP 100 MeV linac

50 keV Injector (Ion source + LEBT) 3 MeV RFQ (4-vane type) 20 & 100 MeV DTL RF Frequency: 350 MHz Beam Extractions at 20 or 100 MeV 5 Beamlines for 20 MeV & 100 MeV

Parameters of 100-MeV Proton Linac at KOMAC

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

Projectile Target Investigated radionuclides Publication

Proton (45 MeV)

natNi 55,56,57,58m+gCo, 56,57Ni

NIM B 269 (2011) 1140 Proton (45 MeV)

natPd 103,104m,104gAg

NIM B 274 (2012) 148 Proton (45 MeV)

89Y 86,88,89gZr, 86m+g,87g,87m,88gY, 85gSr, 84gRb

NIM B 271 (2012) 72 Proton (45 MeV)

natEr 165,166Tm

NDS 119 (2014) 249 Proton (45 MeV)

natHf 173,175,176,177,178m,180gTa, 173,175,179m2,180mHf, 172g,173,177gLu

NIM B 322 (2014) 13 Proton (45 MeV)

natFe 55,56,57Co, 52Fe, 52,54Mn, 51Cr

NIM B 322 (2014) 63 Alpha (45 MeV)

natCd 110,113g,117mSn, 111m,115gCd,108m,g;109g,110m,g;113m,114m,115m,116m,117m,gIn

NIM B 333 (2014) 80 Proton (45 MeV)

natCu 62,65Zn, 61,64Cu, 57Ni, 56,57,58,60Co

NIM B 342 (2015) 305 Proton (45 MeV)

natNd 141-150Pm, 139m,147,149Nd, 138m,142gPr, 139Ce

NIM B 362 (2015) 142 Alpha (45 MeV)

89Y 89g,m,90,91m,92mNb,88,89Zr, 87g,m,88,90m,91mY

NIM B 342 ( 2015) 158 Alpha (45 MeV)

93Nb 93mMo, 91m,92m,95m,gNb

JKPS 67 (2015) 1474 Alpha (45 MeV)

93Nb 94-96Tc

NPA 935 (2015) 65 Alpha (45 MeV)

natCu 66,67,68Ga, 62,63,65Zn, 61,64Cu 58,60Co

NIM B 358 (2015) 160 Alpha (45 MeV)

natAg 108m,108g,109g,110m,110g,111gIn, 109g,,111mCd, 105g,106m,110m,111gAg

JRNC311(2017)1971 Proton (45 MeV)

93Nb 90, 93mMo, 90, 91m, 92mNb, 88Zr, 89Zr, 87gY, 87mY, 88Y

Proton (45 MeV)

natTa 175,179,180Hf, 176,177,178m,180gTa, 177,178W

Proton (45 MeV)

57Co 57Ni,58g,57, 56Co, 54Mn

Measured Results for Proton- and Alpha-induced Reaction Cross-sections

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

• ns in the stack)

Sample activation

(Beam energy, current and time selection )

Measurement of radioactivi ty (cooling, counting with HPGe detector

, Analysis)

Data Evaluation (comparison, In

clusion in nuclear data library, uses etc.)

Measurements and calculat ions (cross sections and uncertainty, et

c.)

Gamma spectrum of irradiated sample foil Activity measurement by HPG e Detector Activation by beam line of KIR AMS Sample preparation Stack composition

1039.35 keV (37.9%)

natCu(α,x) reaction

Calculation of Flux using Monitor

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↓11 )=4(​5↓12 )×​0(​5↓11 )×​2↓11 /0(​5↓12 )× ¡​2↓12 The production yield was calculated form the following formulae:

6=​2↓7 ​'↓, ∫0↑5▒​σ(5)/​(,5∕,;) ↓5 ,5λ

Where Ip is flux (p/cm2-sec), Nd is number density (atoms/cm3), (dE/dx)E is st

• pping power (MeV/cm) and dE is Ein-Eout (MeV).

11

Theoretical Calculations with TALYS

TENDL-2013 Input projectile element mass Ltarget energy maxlevelstar partable bins best endf endfdetail Popeps transeps transpower xseps spherical recoil recoilaverage isomer a Y 089 000 Energies 30 y 100 y y y 1.e-12 1.e-20 15 1.e-20 y y y 0.1

TALYS is a useful computer code that predicts nuclear reactions by simulation within the energy range 1 keV

• 200 MeV. The neutrons, photons, protons, deuterons,

tritons, 3He and alpha induced nuclear reactions at any target material (Z>12) can be simulated with this code

• system. Available at http://www.talys.eu/

Details of TALYS Parameters (selected)

13

• 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
• 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.

15 20 25 30 35 40 45 50 10 20 30 40 50 60 70 80 90

65Cu(p,αtn) 58Co

Eth=26.0 MeV

63Cu(p,αnp) 58Co

Eth=16.5 MeV

Proton Energy (MeV) Cross Section (mb)

natCu(p,x) 58(m+g)Co

Williams et.al. 1967 Acerbi et.al. 1976 Greenwood et.al. 1984 Kopecky et.al. 1985 Aleksandrov et.al. 1987 Mills et.al. 1992 Ido et.al. 2002 Yashima et.al. 2003 TENDL-2013 This Work

20 24 28 32 36 40 44 48 2 4 6 8 10 12 14

65Cu(p,t 3He) 60Co

Eth=28.6 MeV

63Cu(p,p 3He) 60Co

Eth=19.2 MeV

¡ ¡

natCu(p,x) 60Co

Proton Energy (MeV) Cross Section (mb)

¡ ¡

Williams et al. 1967 Gruetter et al. 1982 Greenwood et al. 1984 Mills et al. 1992 Michel et al. 1997 TENDL-2013 This Work

5 10 15 20 25 30 35 40 45 50 0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0

65Cu(α,n2α) 60Co

Eth=17.1 MeV natCu(α,x) 60Co

M.J.Ozafran et.al. 1989 This Work TENDL-2013

¡ ¡

Cross Section (mb) Alpha Energy (MeV)

30 32 34 36 38 40 42 44 46 48 50 3 6 9 12 15 18 21 24 27

65Cu(α,2α3n) 58Co

Eth=36.2 MeV natCu(α,x) 58(m+g)Co

S.S.Rattan et.al. 1986 M.J.Ozafran et.al. 1989 V.N.Levkovskij et.al. 1991 TENDL-2013 This work

¡ ¡

Cross Section (mb) Alpha Energy (MeV)

Reaction Products from natCu(p,x) and natCu(α,x) Reaction

5 10 15 20 25 30 35 40 45 50 10 20 30 40 50 60 70 80 90

63Cu(p,2n) 62Zn

Eth=13.5 MeV

65Cu(p,4n) 62Zn

Eth=31.6 MeV

Proton Energy (MeV) Cross Section (mb)

natCu(p,x) 62Zn

Williams et al. 1967 Kopechky et al. 1985 Aleksandrov et al. 1987 Mills et al. 1992 Michel et al. 1997 Hermanne et al. 1999 Szelecsenyi et al. 2001 Takacs et al. 2002 Uddin et al. 2004 Al-Saleh et al. 2006 Khandaker et al. 2007 Siiskonen et al. 2009 Jost et al. 2013 NDS-IAEA TENDL-2013 This work

5 10 15 20 25 30 35 40 45 50 20 40 60 80 100 120 140 160

65Cu(p,np) 64Cu

Eth=10.1 MeV

65Cu(p,d) 64Cu

Eth=7.8 MeV natCu(p,x) 64Cu

Proton Energy (MeV) Cross Section (mb)

Cohen et al. 1955 Meghir et al. 1962 Newton et al. 1973 Brinkman et al. 1977 Gruetter et al. 1982 Greenwood et al. 1984 Mills et al. 1992 Le Van So et al. 2008 TENDL-2013 This work

15 20 25 30 35 40 45 50 20 40 60 80 100 120 140 160 180 200

63Cu(α, 3He) 64Cu

Eth=13.5 MeV natCu(α,x) 64Cu

K.G.Porges et.al. 1956 N.T.Porile et.al. 1959 E.A.Bryant et.al. 1963 S.S.Rattan et.al. 1986 J.Zweit et.al. 1987 V.N.Levkovskij et.al. 1991 A.Navin et.al. 2004 This Work TENDL-2013

¡ ¡

Cross Section (mb) Alpha Energy (MeV) 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 0.0 0.2 0.4 0.6 0.8 1.0 1.2

63Cu(α,t2n) 62Zn

Eth=35.2 MeV

n

natCu(α,x) 62Zn

This Work TENDL-2013

¡ ¡

Cross Section (mb) Alpha Energy (MeV)

Reaction Products from natCu(p,x) and natCu(α,x) Reaction

20 22 24 26 28 30 32 34 36 38 40 42 44 46 48 50 10 20 30 40 50 60 70 80 90 100 110

65Cu(α,4nα) 61Cu

Eth=39.9 MeV

63Cu(α,2nα) 61Cu

Eth=21.0 MeV natCu(α,x) 61Cu

S.J.Nassiff et.al. 1983 S.S.Rattan et.al. 1986 H.D.Bhardwaj et.al. 1988 V.N.Levkovskij et.al. 1991 F.Szelecsenyi et.al. 2001 This Work TENDL-2013

¡ ¡

Cross Section (mb) Alpha Energy (MeV)

15 20 25 30 35 40 45 50 50 100 150 200 250

Proton Energy (MeV) Cross Section (mb)

natCu(p,x) 61Cu

J.W. Meadows et al. 1953 I.R. Williams et al. 1967

• A. Gruetter et al. 1982

L.R. Greenwood et al. 1984 V.N. Aleksandrov et al. 1987 V.N. Levkovskij et al. 1991 S.J. Mills et al. 1992

• R. Michel et al. 1997

F.S. Al-Saleh et al. 2006 Le Van So et al. 2008 TENDL-2013 This Work

Reaction Products from natCu(p,x) and natCu(α,x) Reaction

10 20 30 40 50 1 2 3 4 5 6

178Hf(p,2p) 177gLu

Eth=7.4 MeV

¡ ¡

Proton Energy (MeV) Cross Section (mb)

natHf(p,x) 177gLu

¡ ¡

Siiskonen et al. 2009 Takacs et al. 2011 TALYS-1.4 This Work

Reaction Products from natHf(p,x) Reaction

Thank you

Charged Particles’ Energy Loss in Materials

• The computer program SRIM (The Stopping a

nd Range of Ions in Matter) is normally used t

• calculate the stopping power of charged parti

cles in the foil.

ABSOLUTE EFFICIENCY: The ratio between the number of pulses recorded by the detector to the number of radiation quanta emitted by the source. where N(E) is the net area under the peak at energy (E), (tl) is the live time of the count, (tr) is the real time of the count, (λ) is the decay constant, (A) is the activity in Bq at the starting time of data acquisition, Iγ(E) is the relative gamma intensity at energy (E) (which is equal to ratio of the gamma emission rate at energy (E) to the disintegration rate), INTRINSIC EFFICIENCY: It is the ratio of the number of signals recorded by the detector to the number of photons striking the detector. (r) is the radius of the detector window, and (R) is the source-detector distance.

Data Analysis and Corrections in the Detector

The correction for the systems dead time was done using the following formulae:

<(=, ¡+%>( ¡(%)=​?@A( ¡+%>( ¡(B)−C%D( ¡+%>( ¡(B)/?@A( ¡+%>( ¡(B) ×100 ¡%

The energy resolution of a detector can be calculated from the following mathematical r elation:

5E(@FG ¡H(BIJA+%IE ¡(H)=KLMN×​5↓2 −​5↓1 /​4↓2 −​4↓1

(E2-E1) provides the peak energy difference between two closely spaced peaks and (C2- C1) gives the corresponding channel difference.

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Sources of Uncertainties

• The measured results are an estimate of outcome and for complete picture the state

ment of the uncertainty of that estimation should be described with the main value.

• Following sources of uncertainties were considered:

① Projectile energies and beam fluctuation (dependent on the irradiation circumsta nces and the foil position in the stack) ② Net gamma peak area and decay data (detection of product with strongest gam ma lines should be preferred) ③ Flux density (due to uncertainties in the monitor cross-section and projectile en ergy) ④ Sample thickness (due to measured mass, area and density of the foils) ⑤ Absolute efficiency, time factor, and dead time (Due to standard source calibrati

• n activity, irradiation time, cooling time and measurement time)

⑥ Irradiated nuclei, impurities, recoil contaminations (can be avoided with the use

• f high purity target foils)

⑦ g-Interference, g-self absorption, and g-attenuation (negligible for thin, light an d medium weight-target elements)

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Data Analysis and Corrections in the Detector

The efficiency (Ɛ) of the detector HPGe (OR TEC, GMX20) coupled to a 4096 multi-chan nel analyzer (MCA) was calculated using the following formulae: 0=​4OP/​Q↓0 ​(↑−#+ ​2↓1

AMP. HV(-3.5kV)

HPGe

Irradiated sample Pb bricks MCA

The spectrum analysis was d

• ne using the program Gam

maVision 5.0 (EG&G Ortec) .

Recommended Monitor Reactions

Monitor Reactions for natCu(p,x) and natHf(p,x) Reactions

natNi(p,x)57Ni natCu(p,x)62Zn natCu(p,x)65Zn

Monitor Reactions for natCu(α,x) and 89Y(α,x) Reactions

natCu(α,x)66Ga natCu(α,x)67Ga natCu(α,x) 65Zn

The cross section are recommended by IAEA-NDS available at https://www-nds.iaea.org

Measurement of Uncertainties

Sources of Uncert ainty

natCu(p,x)

8-43 MeV

natHf(p,x)

7.5-45 MeV

natCu(α,x)

15-42 MeV

89Y(α,x)

11-43 MeV Projectile energy (MeV) ±0.2 - ±0.7 ±0.1 - ±0.4 ±0.5 - ±1.0 ±0.5 - ±1.3 Statistical uncertai nty (%) 0.2 - 17 1 - 12 0.5 - 15 4 - 25 Uncertainty in mo nitor flux (%) 3 - 4.8 5.2 - 8.2 5 - 6 5 - 6 Uncertainty in det ector eff. (%) 3 - 4 3 - 4 3 - 4 3 - 4 Uncertainty in sam ple thick. (%) 2 - 3 1 - 2 1 - 2 1 - 2 Overall uncertain ty (%) 4.7 - 18.4 6.2 - 15.3 5.9 - 16.8 8 - 26

AMP. HV(-3.5kV)

HPGe

Irradiated sampl e

Pb bricks MCA

Gamma-ray Spectroscopy

25

400 800 1200 1600 1E -­‑4 1E -­‑3 0.01

¡ ¡ ¡ ¡ ¡39c m

¡21c m ¡5c m ¡2c m ¡1c m E nerg y ¡(MeV) E ffic ienc y

Nuclide Half-life Energy Activity

133Ba

10.551Y 53.16 keV 80.99 keV 275.9 keV 302.85 keV 356 keV 383.8 keV 10.62 uCi

137Cs

30.07Y 661.657 keV 10.49 uCi

152Eu

13.537Y 121.78 keV 244.70 keV 344.28 keV 411.12 keV 778.90 keV 867.38 keV 964.03 keV 1085.74 keV 1112.07 keV 1408.01 keV 0.902 uCi

t

CPS A e I

λ γ

ε

−

= ×

Efficiency Calculation

26