FUDMA Journal of Sciences (FJS)

EVALUATION OF 67Ga CRSS SECTIONS … Usman

ISSN et 2616-1370
online: al., FJS
ISSN print: 2645 - 2944
Vol. 6 No. 3, June, 2022, pp 113 - 118
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DOI: https://doi.org/10.33003/fjs-2022-0603-987

EVALUATION OF 67Ga CROSS SECTIONS USING EXIFON CODE FOR MEDICAL APPLICATIONS

*Ahmed Rufai Usman and Ahmad Ahmad Ahmad

Department of Physics, Umaru Musa Yar’adua University, Katsina – Nigeria

*Corresponding authors’ email: [email protected]; [email protected]

ABSTRACT
Radioisotopes play very important roles in nuclear medicine for imaging and therapeutic applications. In the
present studies, model calculation of excitation function for production of 67Ga radioisotope was performed
using the EXIFON code, a nuclear reaction cross sections theoretical model code, for the reaction 65Cu(α,
2n)67Ga. The work was performed in the incident alpha energy range of 0 - 40 MeV. Similarly, the Q-value
software (interface) was used for the calculation of reaction threshold and Q-value energies of the reaction of
interest and were respectively found to be 14.97 MeV and -14.10 MeV. The calculated excitation function has
a peak value of 1025 mb around 25 MeV incident energy. The results from the EXIFON code were compared
with the experimentally measured cross sections data retrieved from IAEA database, the EXFOR database, as
well as the theoretical data from Talys code via its library, the TENDL-2019. Our results partially agree with
the theoretical data from Talys code (via the TENDL-2019 library) within the investigated energy region. The
results however overestimated the measured (experimental) data and only agree in shape of the excitation
function. The present work does not consider the effect of shell structure during the execution of the EXIFON
model code. This work could be of importance to the developers and users of nuclear reaction model codes for
new developments and enhancements of the existing codes, as well as to serve as a rough guide for
experimentalists during production of radioisotopes for nuclear medicine applications.

Keywords: Cross sections, Excitation function, 67Ga, Nuclear reaction, Nuclear reaction model

INTRODUCTION The process basically determines pairs of gamma rays emitted

Despite significant improvement in the knowledge of nuclear indirectly by a positron-emitting radionuclide (tracer), which
reaction theory and in turn, improved size for the nuclear is introduced into the body on a biologically active molecule.
reaction database, the importance of new experimental data PET producer requires the combination of a number of factors
as well as the data from theoretical codes calculations, using before it can become an important clinical tool. These factors
reliable parameters, cannot be overemphasized. Several new include (Alharbi et al., 2012; Hod et al., 2021; Manhas et al.,
radioisotope candidates for diagnosis and therapy have been 2020; Ogawa et al., 2021):
emerging, leading to the quest for sufficient experimental and i. An imaging device must give good performance for
theoretical data for their effective validation and optimized isotope of choice.
production. The need for further nuclear data measurements ii. The necessary radioisotope has to be readily available as
(and model calculations) can also be seen in several other at the time of need.
applications such as in alpha– and deuteron–induced iii. The combination of a radiopharmaceutical and a patient
reactions, high-energy accelerators as well as in low energy tissue for which the PET scan provides significant
cyclotrons (Tarkanyi et al., 2014). Moreover, the database for diagnostic information which is not readily available with
the proton-induced reactions routes are well established, other techniques.
relative to the higher charged particles. However, following SPECT imaging scan shows how blood flows to tissues and
the advent of new candidate radioisotopes and additional organs, capable of diagnosing tumors, infections, seizures,
production routes for radioisotope production optimization, stroke and stress fractures in the spine. Usually, a particular
there is recent surge of studies using the higher charged radiolabeled pharmaceutical is injected into the blood stream,
projectiles, especially the deuterons and alpha particles depending on the medical issue to be investigated. Some of
(Khandaker et al., 2014; Otuka et al., 2017; Usman et al., the popular radioisotopes for this procedure include
2017a; Usman et al., 2016a; Usman et al., 2017b; Usman et technium-99m, iodine-123, xeno-133, fluorine-18 and
al., 2020; Usman et al., 2016b). thallium-201. A radiolabeled glucose (Fluorodeoxyglucose,
The artificially produced new candidate radioisotopes are FDG) may be used for the examination of a tumor in brain.
gradually finding a large number of potential applications in As gamma rays are emitted by the active isotope in the tracer,
numerous fields of human endeavor (Art and Ayetkin, 2015). they are detected by a scanner, which are then collected by a
In nuclear medicine, radioisotopes mostly find very specific computer, process and add them as 3D images of the
and important applications in diagnosis and therapy (Alharbi investigated organ, such as the brain. Unlike the PET scan, in
et al., 2012). The use of these radioisotopes for imaging or as SPECT procedure, the tracer stays in the blood stream rather
therapeutic agents depends on their respective properties than being absorbed in the surrounding body tissues, thus
suitable for the application of interest. Two very popular limiting the images to only the areas where blood flows.
modalities, the Positron Emission Tomography (PET) and SPECT scans are said to be cheaper and more readily
Single Photon Emissions Computed Tomography (SPECT) available than PET scans (Hod et al., 2021; Manhas et al.,
are both used for diagnosis. The PET modality is a nuclear 2020; Ogawa, et al., 2021), even though the PET scan are
medicine imaging technique capable of producing a three- also. SPECT use common radiopharmaceuticals of nuclear
dimensional (3D) image of organs in the body. Emerging medicine, in contrast to PET, which use positron emitters and
evidences indicate that PET has the promise of higher-quality followed by formation of two annihilation 511-keV photons.
images and greater diagnostic accuracy relative to SPECT.

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Gallium-67 (67Ga) has several important applications in BACKGROUND AND THEORETICAL

nuclear medicine. It is popularly known for its usage in FRAMEWORK
imaging and localization of infections (inflammatory EXIFON, a nuclear reaction code, is an analytical and multi-
lesions). Its usage in imaging is because of its emission of step statistical model code. This code has the ability to
four (4) suitable gamma rays (93, 184, 296, 388 keV) (Van de uniquely describe angular distributions, reaction cross
Wiele, 2008) for this purpose. For localizing infection sections and emission spectra for pre-equilibrium,
purpose, the 67Ga radioisotope has been labeled in the form of equilibrium and the collective the no-collective direct theory
67Ga-citrate for more than three (3) decades with very processes (Kalka, 1991; Chad-Umoren and Ebiwonjumi,
efficient results (Van de Wiele, 2008). 2014). However, a slight drawback of the code is its limitation
Furthermore, 67Ga is Auger—electron emitting radioisotope to few projectiles which are: neutron-, proton-, and alpha-
similar to 125I, with cancer therapeutic property following induced reactions, with the outgoing or emitted particles
their significant level of cytotoxicity (Koumarianou et al., being neutrons, protons, alphas or photons in the outgoing
2014; O'Donoghue and Wheldon, 1996). The emissions from channels. The development of statistical multi-step theory
this radioisotope are also found to be short-range in biological from the simple compound nucleus and single step direct
tissues, thus minimal damage to neighboring healthy cells models, were influenced by mainly three basic ideas, which
(Usman et al., 2016b). Comparatively, the emission of 4.7 include; the classification of nuclear states by their
Auger and Coster-Kronig electrons per decay and the shorter complexity or exciton numbers as proposed by Griffin,
half-life of 67Ga (𝑇1/2 = 3.2617 d) relative to 125I (T1/2 = 59.4 (1967), the distinctive configurations of bound and unbound
d) makes the 67Ga-labeled radiopharmaceuticals clinically state proposed by Feshbach et al. (1980) and the possible
more desirable to patients than the later (Koumarianou et al., consideration of the chaotic nuclear Hamiltonian as a random
2014). matrix proposed by Agassi et al. (1975).
Experimentally, the 67Ga radioisotope is usually produced in The concept of statistical multistep theory is becoming more
cyclotron machines and various production channels are relevant for a better comprehension of the mechanism of
available for this important radioisotope. Cyclotron-based nuclear reactions, especially beyond 20 MeV energy. It
radioisotope production is one of the most sophisticated involves the application of analytical model, for both
technologies that allows the production of a number of processes of statistical multistep direct (SMD) and statistical
isotopes of immense potential applications in the medical multistep compound (SMC), to describe the nuclear reactions
field (Usman et al., 2017b). Several studies in the literature up to 30 MeV energy. The generalization of this concept can
have reported the production of the 67Ga from induced nuclear be possible to some respect: The extension to higher energies
reactions using proton, deuteron, tritium or alpha particles as is performed including s-step direct processes for s = 1 up to
activation projectiles. We have recently reported measured 5. The same residual interaction is used for computing both
experimental cross section of the 67Ga via the alpha particles formation and decay of the compound nucleus within SMC as
production route in one of our previous studies (Usman et al., well as SMD processes. Thus, there is no reference to the
2016b). optical model (OM) reaction cross section. The OM cross
Model predictions of nuclear reactions are important in section for charged particles was used to simulate coulomb
radioisotopes production as they provide reasonably reliable effects only within the threshold region (Polster and Kalka,
data where experimental data is not readily available, or, 1992). The α and γ processes are included in spin-isospin
where the available data is scanty and insufficient. Moreover, conservation when the two-body collision is considered. The
the theoretical data serves as a guide to experimentalist in calculation of Multiple Particle Emission (MPE) is
some cases. There are a number of nuclear reactions models generalized. Up to three decays of the compound nucleus are
capable of predicting nuclear reaction cross sections. These considered. The detailed formulation of this model makes it
models include Talys code (Koning and Rochman, 2012), capable of predicting spectral emissions of photons, neutrons,
Empire code (Herman et al., 2007), ALICE code (Alharbi & protons and alphas, including pre-equilibrium, equilibrium,
Azzam, 2012), Exifon code and few others. Each of these direct and also the MPE processes in a consistent mode. For
models have their strength and limitations, with some more several reaction types, nuclei and energies, calculations can
powerful than others. The Exifon code is a simple to use code be performed with one physical parameter set.
for the prediction of nuclear reactions cross sections for For the pure statistical multi step reaction model, a proposal
uncharged neutron and gamma rays and also for the charged was made for a unique description (a,xb) emission spectra
proton and alpha particles. Though relatively old (as it has not where a,b = n,p,α and γ (Neutron, Proton, Alpha and Gamma-
been having significant updates in recent years) and not as Ray), as well as the excitation function (activation cross
sophisticated as other codes such as the Talys code, the section). This technique is based on many body theory (Green
Exifon code can predict the cross sections of nuclear reactions Function Formalism) and random Matrix Physics. The
in a fraction of a minute or in few minutes, depending on the (Version 2.0) EXIFON Code is a generalization of energies
maximum energy of interest. The code hold the advantage of up to 100 MeV, and is capable of performing fast calculations
being easy to understand and run, without requiring of cross section from one global parameter set (Kalka, 1991).
cumbersome activities and heavy task. There are several Detailed theoretical description of underlaying theory to
studies in the literature for detailed theory on the Exifon code, Exifon such as the Statistical Multistep Direct (SMD), the
as well as several previous works which use the code for the Statistical Multistep Compound (SMC) cross Section and
calculations of cross sections (Ahmad et al., 2017; Ahmad et many more can be found in the literature (Ahmad et al., 2017;
al., 2019; Chad-Umoren and Ebiwonjumi, 2014; Dauda, Kalka, 1991; Polster and Kalka, 1991). The SMD and SMC
2011; Dauda et al., 2017; Jonah, 2004; Hauser and Feshback, theories are very vital in the understanding of the basis of the
1952; Kalka et al., 1990; Kalka, 1991; Muhammed et al., formation of the cross section.
2011; Murata, 1997; Polster and Kalka, 1991).
METHODOLOGY
The theoretical model code EXIFON (version 2.0) was used
to calculate the cross section of the reaction 65Cu (α, 2n) 67Ga.
The theoretical model is based on optical potentials, which

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EVALUATION OF 67Ga CRSS SECTIONS … Usman et al., FJS

comprises of both statistical multistep (SMD) and statistical calculation with or without shell effect corrections. For the
multistep compound (SMC). The code can make calculations present study, the calculations were performed with default
for incident energies up to 100 MeV in a very fast mode and settings of the code. Other parameters, such as decay
has the capacity to predict cross sections using global properties, relevant to the investigated radioisotope are
parameter set, with its output capable of being arranged in summarized in in Table 2.
ENDF-6 format (Kalka, 1991).
To properly run the program, the first important step is to RESULTS AND DISCUSSION
ensure that the existing Exifon code version on a system is The output results for the Exifon calculation can be found as
working efficiently. The code is usually used or installed on the output data in the Exifon output directory as OUTEXI.
a 32-bit computer operating system. In addition to specifying Similarly, other DATA files such as A2N, ALF and AP (for
the target of material, the parameters of inputs as well as the Alpha-Neutron, Alpha-Alpha, and Alpha-Proton) in same
outputs were properly defined. The input parameters for this output directory, each representing an exit channel or decay
study include use of alpha particles as projectile or incident channel for production of a radioisotope, depending on the
particles, and the (65Cu) isotope of copper as the target bombarded target.
material. This is usually followed by prompt selection of The calculated cross section data were plotted as a function
‘excitation function’ in the general option of the code. The of alpha energy and the excitation curve obtained was
investigation was performed in the medium energy range of compared with the Talys code data obtained from TENDL
0 to 40 MeV. The incident energies of the bombarding alpha 2019 library (Koning et al., 2019), as well as the experimental
particles were specified in steps of 1 MeV in the present work. literature data from EXFOR Data Library (Otuka et al., 2014).
There exists a modification option, where one can make the The results are discussed in the subsequent section.

Table 1: Cross-Sections for 65Cu(α, 2n)67Ga Obtained using EXIFON Code.

Incident Energy (MeV) Cross Section δ (mb)
16 118.73
17 355.5
18 617.47
19 791.09
20 876.31
21 945.72
22 984.38
23 1007.7
24 1017.8
25 1025
26 962.79
27 653.53
28 363.04
29 212.6
30 116.54
31 62.984
32 35.196
33 22.581
34 14.599
35 9.8236
36 7.4984
37 5.8638
38 4.7729
39 3.9799
40 3.5464
Similarly, the graphical plot of cross section δ (mb) against incident alpha energy (MeV) is given below.

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EVALUATION OF 67Ga CRSS SECTIONS … Usman et al., FJS

1200
65Cu(α,2n)67Ga

1000
Cross Section δ (mb)

This work (EXIFON)

Navin 2004 (EXFOR)

800
TENDL 2019

600

400

200

0
10 15 20 25 30 35 40 45
Incident Energy E (MeV)

Figure 1: Excitation Function for the 65Cu (α, 2n) 67Ga Reaction

Evaluated cross section of Ga-67 energy. Generally, this work predicts higher cross sections up
Table 1 shows numerical values of the evaluated cross to around 27 MeV incident alpha energy. As indicated in Fig.
sections of 67Ga from alpha bombardment of 65Cu using 1, the fine shape of the excitation function has its Ga-67
Exifon model code. The prediction of the cross sections by production peak at about 25 MeV and corresponding cross
the code in the present work shows partial agreement with the sections values of 1025 mb, which indicates that the possible
advanced Talys code data from TENDL 2019 library, region of the higher yield production prospect. Both Exifon
especially up to about 20 MeV, beyond which the estimated and Talys codes (TENDL-2019) could not accurately
cross sections from the Exifon code look larger than the reproduce the experimental work of Navin et al. (2004), even
TENDL-2019 data, up to about 26 MeV. A sharp decrease or though all the three (3) share similar shape rather than
fall in magnitude of the present cross sections relative to those magnitude.
reported in TENDL-2019 are observed beyond the 26 MeV

Table 2: Decay Data of Ga-67 Retrieved from Nudat 2.6 (NuDat 2.6, 2011)and Q-Value Software (QCalc, 2016).
Nuclide Half-Life Decay Eγ Iγ Contributing Q-Value Threshold
(Hours) Mode (KeV) (KeV) Reaction (MeV) (MeV)
(%)
67Ga 65Cu (α,2n) 67Ga
78.3 EC 93.31 39.2 -14.102 14.971
(100) 184.5 21.2
300.2 16.8
393.5 4.68

CONCLUSION reaction codes, as well as providing a useful information for

The excitation function for the theoretical production of 67Ga, production of 67Ga radioisotope to experimentalist.
an important radionuclide in nuclear medicine procedure was
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