Radiochim. Acta 2016; 104(9): 601–624

Syed M. Qaim*, Ingo Spahn, Bernhard Scholten, and Bernd Neumaier Uses of alpha particles, especially in nuclear reaction studies and medical radionuclide production

DOI 10.1515/ract-2015-2566 1 Introduction Received December 15, 2015; accepted April 21, 2016; published online June 8, 2016 1.1 General Abstract: Alpha particles exhibit three important charac- teristics: scattering, ionisation and activation. This article An alpha particle is a helium nucleus, i.e. it is a bound en- briefly discusses those properties and outlines their ma- tity of two protons and two neutrons. The strong binding jor applications. Among others, -particles are used in el- of an alpha particle makes it behave more like a nucleon emental analysis, investigation and improvement of ma- rather than a complex particle, except that it has double terials properties, nuclear reaction𝛼𝛼 studies and medical the charge of a proton, which leads to a much stronger radionuclide production. The latter two topics, dealing Coulomb interaction than in the case of a proton. The al- with activation of target materials, are treated in some pha particle, however, has a spin of in comparison to the detail in this paper. Measurements of excitation func- value of ½ for a neutron and a proton. tions of -particle induced reactions shed some light on The alpha particle was originally0 detected in the natu- their reaction mechanisms, and studies of isomeric cross ral radioactive decay of heavy mass nuclei. Subsequently, sections𝛼𝛼 reveal the probability of population of high- a large number of artificially produced heavy mass spin nuclear levels. Regarding medical radionuclides, an -particle emitting radionuclides were characterised. overview is presented of the isotopes commonly produced Their half-lives differ considerably but the -particle en- using -particle beams. Consideration is also given to 𝛼𝛼ergies are usually between and . In general, the some routes which could be potentially useful for pro- -particle energy increases slowly with the𝛼𝛼 increasing duction𝛼𝛼 of a few other radionuclides. The significance of of the radioactive nucleus. On4 the7 other MeV hand, some syn- -particle induced reactions to produce a few high-spin 𝛼𝛼thetically produced neutron-deficient nuclides of medium𝑍𝑍 isomeric states, decaying by emission of low-energy con- lifetime in the region of lanthanides emit low-energy - version𝛼𝛼 or Auger electrons, which are of interest in lo- particles ( – ), and strongly neutron deficient ones calised internal radiotherapy, is outlined. The -particle up to . 𝛼𝛼 beam, thus broadens the scope of nuclear chemistry re- Three1 important4 MeV properties of -particles were estab- search related to development of non-standard𝛼𝛼 positron lished7.4 rather MeV early: emitters and therapeutic radionuclides. a) ionisation (and excitation)𝛼𝛼 of the surrounding medium Keywords: -particle beam, elemental analysis, materials b) scattering research, nuclear reaction studies, medical radionuclide c) nuclear interaction production.𝛼𝛼 The property of the -particle to highly ionise and excite atoms (resulting in chemical and biochemical changes) causes rapid loss of its𝛼𝛼 energy in the surrounding medium. Consequently, the ranges of -particles with in the matter involved are rather low. This property makes *Corresponding author: Syed M. Qaim, Institut für Neuro- the -particle very attractive𝛼𝛼 for internal radionuclide𝐸𝐸 퐸 𝐸𝐸� ther- wissenschaften und Medizin, INM-5: Nuklearchemie, apy. On the other hand, the loss of the intensity of high- Forschungszentrum Jülich, D-52425 Jülich, Germany, energy𝛼𝛼 -particles is more concentrated towards the end e-mail: [email protected] Ingo Spahn, Bernhard Scholten, Bernd Neumaier: Institut für of the path length, resulting in the so-called “Bragg Peak”. Neurowissenschaften und Medizin, INM-5: Nuklearchemie, This characteristic𝛼𝛼 renders the -particle beam very useful Forschungszentrum Jülich, D-52425 Jülich, Germany for external radiation therapy, especially for treatment of 𝛼𝛼

Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 602 | S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production deep-lying tumours. Another important use of the highly cyclotrons are used for nuclear reaction studies as well as ionising character of the -particleis in materials research. for radionuclide production. Properties of many synthetic and semiconductor materials This review briefly mentions the various applications are improved on irradiation𝛼𝛼 with -particles. of alpha particles but deals in more detail with nuclear re- The scattering of the -particle, initially observed be- action studies and medical radionuclide production. low the Coulomb barrier, is a very𝛼𝛼 specific property for identifying various elements.𝛼𝛼 It is utilized today for exten- sive elemental analyses of thin layers of materials using 2 Applications in materials both low and intermediate energy -particle beams. The interaction of an -particle with another nucleus research may cause Coulomb excitation or𝛼𝛼 may induce a nuclear Materials research involves on one hand analysis and reaction. Since the interaction𝛼𝛼 involves transfer of a large study of known materials and, on the other, development amount of angular momentum, often high-lying high-spin of new materials. Ion beams in general, and -particle nuclear levels are populated. Studies of -particle in- beams in particular, are useful in both cases. duced interactions are thus of considerable interest from 𝛼𝛼 the viewpoints of nuclear astrophysics, nuclear𝛼𝛼 reaction mechanisms and formation of radioactive products. In nu- 2.1 Elemental analysis clear astrophysics, an understanding of the occurrence of alpha-clustering is of great importance. The formation of Small accelerators of different designs and capabilities, from two -particles provides an intermediate step in named as Pelletron, Tandem, Tandetron, etc. are avail- 8the synthesis of . Similarly, the synthesis of other light able in many parts of the world. They generally accelerate massBe nuclei is𝛼𝛼 interesting,12 e.g. of via the ( ,n)- charged particles to energies between a few hundred reaction and of C via the 26( ,p)-process.23 Further- and several ; in special cases -particles of energies more, in the medium26 and heavy23 massAl regions, thereNa 𝛼𝛼 are up to can be accelerated. Ion-beam analysisk eV is some stable protonMg rich isotopesNa whose𝛼𝛼 nucleosyntheses done using theMeV following techniques𝛼𝛼 (for early detailed re- cannot be satisfactorily explained via neutron-induced re- views cf.25 [ MeV1, 2]). actions: it is postulated that -particle induced reactions i) Ion back scattering (IBS) play an important role. As regards nuclear reaction mech- ii) Elastic recoil detection analysis (ERDA) anisms, experimental measurement𝛼𝛼 of an excitation func- iii) Particle induced X-ray emission (PIXE) tion and its comparison with the results of nuclear model iv) Particle induced -ray emission (PIGE) calculations provides very useful information. Finally, the v) Charged particle activation analysis (CPAA) formation of radioactive products in -particle induced re- 𝛾𝛾 actions is of great practical value since many unique ra- The ion back scattering (IBS) at low energies mainly con- dionuclides are obtained. 𝛼𝛼 sists of Rutherford back scattering (RBS) which is scatter- ing below the Coulomb barrier. The technique is based on the energy exchange between the elastically colliding 1.2 Availability of -particles particles, the slowing down of the ion in the target mate- rial, and the probability of the elastic scattering reaction. In contrast to isotropically emitted -particles from ra- 𝛼𝛼 The energy and angle of the back-scattered radiation thus dioactive nuclei, the accelerated -particles move in one give important information on the charge and thickness of direction and are termed as a beam. Tremendous𝛼𝛼 advances the target material. It is probably the most widely adopted have been made in charged particle𝛼𝛼 accelerator technol- single technique in multielement characterisation of ma- ogy over the last . The types of particles accel- terials with -particle beams of energies between and erated, their energies, beam currents and the beam qual- . The detection sensitivities are high for heavy mass ity constitute a very100 broad years spectrum of modern engineer- elements, and𝛼𝛼 quantities on the order of a few ng can2 be ing. Alpha particle beams of well-defined shapes and high 4easily MeV detected. The light elements, on the other hand, are intensities are now commonly available for applications difficult to detect. in diversified fields. The main use of low-energy acceler- In recent years, intermediate energy -particles of en- ators is in elemental analysis. For radionuclide produc- ergy up to about have also been increasingly used tion high-intensity small and medium-sized cyclotrons are in ion back scattering work. However, the𝛼𝛼 back-scattered commercially available. Occasionally intermediate energy 40 MeV

Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production | 603 spectra then become very complex, and powerful com- gies to . Due to the much lower range of -particles puter programs are needed to unfold them. in matter than that of protons, PIXE-alpha spectrometers The elastic recoil detection analysis (ERDA) involves are occasionally1 5 MeV used in analysis of very thin𝛼𝛼 upper sur- quantitative detection of a recoiling nucleus, released faces (cf. [3]). from its environment, subsequent to the interaction of The particle-induced gamma ray emission (PIGE) tech- a charged particle projectile with a light nucleus. By de- nique involves quantitative determination of prompt - termining the energy of the recoiling nucleus, its depth- rays emitted in a nuclear reaction or Coulomb excitation of profile is measured. This technique is particularly suit- the nucleus. This technique finds only limited specific𝛾𝛾 ap- able for the assay of hydrogen and helium isotopes in sur- plication in the analysis of light mass elements for which face layers. By a suitable choice of the incident projec- RBS and PIXE are not very successful. Using -particles of tile, the technique can be extended also to lithium and about , for example, the reactions ( , ) and beryllium. If the host substrate is thin compared with the ( , ) allow a rather easy determination7 𝛼𝛼 󸀠󸀠 of7 the two range of the projectile, a considerable improvement in de- target19 5 elements󸀠󸀠 MeV19 lithium and fluorine by on-lineLi 𝛼𝛼 𝛼𝛼 𝛾𝛾determina-Li tection sensitivity is achieved by the use of the kinematic tionF 𝛼𝛼 of𝛼𝛼 the𝛾𝛾 -raysF ( and , respectively). coincidence technique (KCT), which involves detection of Charged particle activation analysis (CPAA) involves both the recoil light nucleus and the scattered projectile in quantitative𝛾𝛾 determination478 keV of197 a keV radioactive product coincidence. formed in the interaction of a nucleus with a charged Analysis by ERDA is generally done using low or inter- particle as projectile. Due to the Coulomb barrier effect mediate energy projectiles. In the case of -particles the the technique is applied only in the region of light el- energies used are either below or around . ements, especially for surface analysis using protons With -particles, the limit of detection𝛼𝛼 of concen- and -particles. The use of -particles has also been tration of hydrogen and deuterium5 MeV within a depth25 of MeV demonstrated3 in the analysis of several metals like , , of the5 substrate MeV 𝛼𝛼 consisting of light elements is about , He, etc. (cf. [4]). 𝛼𝛼 ( ). By using -particles, the depth which1 μm In summary, elemental analysis of materials isV veryCr can be examined is in the range of to , depend-0.5% successfullyMn Fe carried out using -particle beams utilizing ing5000 on ppm the substrate. Thus25 MeV the 𝛼𝛼 detection of hydrogen, he- the RBS and ERDA techniques, the former for heavy ele- lium (and lithium) in a matrix of heavy100 elements300 μm also be- ments and the latter for very light𝛼𝛼 elements. A few light el- comes possible (at a concentration limit of about ). ements can also be analysed using PIGE in combination When KCT is used with -particles on a thin sub- with -particles. PIXE, on the other hand, commonly uti- strate, the limit of detection of those three light elements,0.1% lizes a proton beam, and activation analysis using neu- especially in heavy substrates,25 MeV is𝛼𝛼 considerably improved trons𝛼𝛼 has been applied for decades more successfully than and lies in the range of . Thus, ERDA and its exten- charged particle activation. sion KCT provide powerful, accurate and fast methods of determination of very light100 ng elements (hydrogen, helium, lithium) in various host matrices, especially polymer sur- 2.2 Materials properties faces and interfaces. In fact this technique has contributed significantly to polymer science. In recent years, the ion beam, especially the -particle The particle induced X-ray emission (PIXE) technique beam or heavier mass beam at an intermediate energy involves quantitative determination of X-rays emitted in up to about , has been finding increasing𝛼𝛼 applica- interactions of an ion-beam with materials. The ionisa- tion in implantation studies related to development of new tion or excitation of an inner atomic shell by the projectile materials. In40 general, MeV the main research direction here is leads to a vacancy which is filled by an electron from the the fabrication and characterisation of micro- and nano- outer shell, the process being accompanied by emission of structured substances, which are of high interest in ma- X-rays. As the energy of the X-ray is a signature of the of terials, environmental and bio-medicinal sciences, micro- the element, a quantitative determination of the element is and nanotechnology, electronics, optics and laser technol- possible via characterisation of the intensity of the X-ray.𝑍𝑍 ogy. The doses administered to achieve the desired effects It is an analytical technique of high sensitivity, especially are deduced from the -particle energy as well as its per- in the medium and heavy mass regions where detection missible intensity. This is a very fast developing field and limits lie in the ng range. The technique is, however, more its importance is expected𝛼𝛼 to increase further in the future. suitable for analysis of trace elements on or near surface Another aspect of -particle implantation studies is re- layers. In general, the PIXE makes use of protons of ener- lated to the investigation of radiation damage in structural 𝛼𝛼

Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 604 | S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production materials of nuclear technology. As it is well known, radia- 3.2 Nuclear reaction data tion damage in nuclear reactors is caused by displacement of atoms from their lattice positions, mainly due to scatter- As regards nuclear reaction studies using -particles, ing effects of neutrons. In fast reactors, especially in future some on-line measurements on the spectra of emitted neu- fusion reactors, the (n,x ) processes will also occur and trons and charged particles have been performed𝛼𝛼 with will lead to the formation of considerable quantities of a view to investigating angular and energy distributions of gas, whose damage effects𝛼𝛼 are relatively unknown. The im- the emitted particles. The data lead to very useful informa- plantation and simulation studies using -particle beamsHe tion on the mechanism of emission of those particles. The allow investigation of the damage effects, e.g. brittleness, technique is, however, very demanding and cumbersome. change in elasticity, formation of voids, etc.𝛼𝛼 Most of the work has therefore been done using the acti- A yet another special application of the -particle vation technique in which the residual radioactive prod- beam is to produce a profile of radioactivity in a mate- uct of a nuclear reaction is determined. This method leads rial whose wear and tear in an industrial process𝛼𝛼 or its to very little information on the route and mechanism of erosion and corrosion under various environmental condi- formation of the product. However, if the result could be tions are to be studied. This so called “thin layer activation compared with nuclear model calculations, developed ex- technique” generally makes use of activation with protons tensively in recent years, it may be possible to discern the or deuterons, but occasionally -particle activation is also contributions of various nuclear processes involved. Such employed (cf. [5–8]), for example, production of and investigations are of direct relevance to accelerator pro- via the ( ,d) and𝛼𝛼 ( ,p) reactions,58 duction of radionuclides as well and involve total and iso- respectively,95 in56 the surface58 layers.92 Due to the95 shorterCo range meric cross sections. They are therefore discussed below ofNb the -particleFe in𝛼𝛼 the matterCo as comparedZr 𝛼𝛼 Nb to the proton in some detail. or the deuteron, the profile of the generated radioactivity in -particle𝛼𝛼 irradiation is shorter. The study of removal of the radioactivity from the generated profile under sim- 3.2.1 Excitation function ulated𝛼𝛼 conditions leads to an understanding of the phe- nomenon involved (wear, corrosion, etc.). Measurement of the total cross section of a reaction chan- nel as a function of the -particle energy is a standard approach. A typical case is discussed here. The irradi- 3 Nuclear reaction studies ation of an target with𝛼𝛼 -particles of energies up to leads123 to ( ,n) , ( ,2n) and Nuclear reaction studies using -particle beams deal both ( ,3n) Sbreactions.123 Many𝛼𝛼126 groups123 reported125 data for with nuclear structure analysis and nuclear reaction cross 123those50MeV reactions124 [9–17] andSb 𝛼𝛼 a criticalI evaluationSb 𝛼𝛼 [18I] pro- sections. A brief discussion of the𝛼𝛼 two aspects is given be- videdSb 𝛼𝛼 a set ofI reliable results. The more consistent set of low. The emphasis is, however, on cross section data. experimental data [12, 13, 19] are shown in Figure 1, to- gether with the calculated results [19] from a modern nu- clear model calculational code TALYS, which is primarily 3.1 Nuclear structure data based on the statistical model but takes into account pre- compound and direct interactions as well as the nuclear Studies related to nuclear structure generally involve in- structures of the nuclei involved. The agreement between beam -ray spectroscopy, i.e. measurement of -ray spec- the experiment and theory is excellent, both in terms of tra during the irradiation of a sample with -particles. It shapes and magnitudes of the three excitation functions. may involve𝛾𝛾 Coulomb excitation, if the -particle𝛾𝛾 energy From these results it is inferred that multi-neutron emis- cannot surmount the Coulomb threshold, or𝛼𝛼 may lead to sion in the interaction of a medium mass nucleus with high-lying levels of an ( ,x) reaction product,𝛼𝛼 which sub- -particles can be described well by the existing theory. sequently deexcite via -ray transitions. Thus, some in- Interesting is a comparison of the three curves: the ( ,n) teresting nuclear structure𝛼𝛼 results may be obtained, es- cross𝛼𝛼 section has a low value of at the maximum pecially if direct reactions𝛾𝛾 like ( ,d) or ( ,t) are involved, of the excitation function, the whole curve is rather𝛼𝛼 nar- because of the possibility of population of high-spin lev- row, but the tail is long, suggesting380 a mb high contribution of els which may be difficult to reach𝛼𝛼 via𝛼𝛼 an (n, ) or a (d,p) the compound nucleus mechanism in the early part but process. more non-equilibrium contributions at higher energies. 𝛾𝛾 The curves for the ( ,2n) and ( ,3n) reactions, on the other

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34]), (cf. [35–37]) and -particles(cf. [32, 33, 35, 37, 38]) to elucidate3 some important aspects of isomer distribu- tion. InHe general, it appears𝛼𝛼 that low-spin levels are better formed in low-energy reactions induced by neutrons and protons whereas higher spin levels are preferentially pop- ulated in -particle induced reactions. This is illustrated below through a consideration of three typical isomeric pairs, namely𝛼𝛼 m,g , m,g and m,g , which belong to three different58 mass94 regions of194 the Chart of Nuclides. The radionuclideCo pair Tc consistsIr of a metastable state ( ) having58m a,g spin of and the ground state ( ) with a spinCo of . The+ separation en- 1/2 ergy between𝑇𝑇 = 9.1 the h two isomeric levels+ 5 is only and 1/2 the metastable𝑇𝑇 = 71 state d decays completely2 to the ground state. The isomeric cross section ratio ( ) was measured25 k eV in Figure 1: Excitation functions of ( ,xn) reactions. The three different charged-particle induced𝜎𝜎𝜎𝜎 reactions, namely experimental data are reproduced123 well by nuclear126,125,124 model ,n), ,n) and ( 𝜎𝜎𝜎𝜎,n)�𝜎𝜎𝜎𝜎 [32, 33], and the re- calculations using the code TALYS (diagramSb 𝛼𝛼 adaptedI from Uddin 58 57 55 et al. [19]). sults are shown in Figure 2(a). Evidently, the ratio in- creasesFe(p in allFe(d reactions withMn the𝛼𝛼 increasing projectile en- ergy. Conspicuous, however, is the higher formation prob- hand, are much broader and have much higher maximum ability of the high-spin isomer in the -particle induced values of about . This suggests occurrence of more reaction. precompound interactions. These results show trends sim- The radionuclide pair consists𝛼𝛼 of a metastable ilar to those in1400 (p,xn) mb and (n,xn) processes. The (p,n) ex- state ( ) having94m a,g spin of and the ground citation function is rather narrow and the (p,xn) curves state ( ) with a spinTc of . The+ separation en- 1/2 are broad (cf. [20, 21]). The (n,n ) reaction, on the other ergy between𝑇𝑇 = 52 the min two states is + .2 The two states de- 1/2 hand, is an exception but the (n,xn)󸀠󸀠 excitation functions cay independently𝑇𝑇 = 4.9 h to . The isomeric7 cross section ra- are rather broad (cf. [22, 23]). From this comparison it may tio ( ) was measured94 in three different75 k eV reactions, namely be inferred that ( ,xn) reactions are similar to multineu- 𝜎𝜎𝜎𝜎 ,n), ( ,2n)Mo and ( ,d pn) [39–42], and 𝜎𝜎𝜎𝜎 tron emission reactions induced by single particles (n or p) the94 results are93 depicted3 in Figure94 2(b). Two conspicuous which proceed predominantly𝛼𝛼 via compound and precom- trendsMo(p are observed:Nb He (i) the ratioMo decreases𝛼𝛼 + in the (p,n) pound processes. The same may not apply to excitation reaction with the increasing projectile energy, indicating functions of reactions like ( ,d), ( ,t) etc., where strong thereby the increasing population of the higher spin iso- contributions from direct interactions may be expected. mer with the increasing projectile energy; (ii) the ratio is In order to understand the mechanism𝛼𝛼 𝛼𝛼 of those reactions, low in - and -particle induced reactions which leads spectral measurements dealing with angular and energy to the conclusion3 that the higher spin isomer is preferen- distributions are essential. tially populatedHe in𝛼𝛼 the latter two reactions. Since m is a low-spin isomer, it is preferably produced via the94 (p,n) reaction (cf. [39, 40]). Tc 3.2.2 Isomeric cross section The radionuclide pair consists of a metastable state ( ) having194m a, highg spin of or and Whereas the total cross section for the formation of a reac- the ground state ( Ir)withalowspinof . 1/2 tion product (i.e. integral cross section) can be described The separation𝑇𝑇 = 171 energy d between the two isomeric10 11 levels− 1/2 relatively well by the nuclear model calculation, there is . Both𝑇𝑇 of them= 19.3 decay h independently to 1 , are considerable difficulties in the prediction of formation emitting particles and several -rays. The isomeric194 cross section of an isomer (i.e. partial cross section) be- cross< 440 section keV− ratio was reported as ( ) for two reactions,Pt cause it depends on a large number of parameters, such namely 𝛽𝛽 ( ,d pn) m,g and 𝜎𝜎𝜎𝜎𝛾𝛾 ,p) m,g [38, 𝜎𝜎𝜎𝜎 as excitation energy, spin of the level concerned, type of 43] and192 the results are194 shown in194 Figure 2(c).194 Whereas projectile used, reaction channel, etc. (cf. [24–26]). Exten- the ratio forOs the𝛼𝛼 (n,p)+ reactionIr is veryPt(n low, that forIr the sive studies have been performed over the years using neu- -particle induced reaction is relatively high. trons (cf. [27–30]), protons (cf. [31–36]), deuterons (cf. [32– 𝛼𝛼 Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 606 | S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production

Figure 2: Isomeric cross section ratio as a function of projectile energy for three isomeric pairs: (a) m,g , (b) 94m,g , (c) 194m,g . In each case experimental data reported in the literature [32, 33, 38–43] are given. The -particle irradiation58 leads to a preferential population of the higher spin isomer. Co Tc Ir 𝛼𝛼

From the above discussed three examples it is qual- demands a special type of radionuclide. For in vivo diag- itatively concluded that, besides other factors, high spin nostic investigations involving organ imaging, for exam- isomers are preferentially populated in -particle induced ple, radionuclides are required that can be efficiently de- reactions, irrespective of the separation energy of the two tected from outside of the body. To this end, short-lived states concerned. This observation is of𝛼𝛼 considerable sig- -ray emitters, like m and , and positron emitters, nificance in the production of a few isomeric states (see like and , are99 commonly123 used, the former finding below). 𝛾𝛾application11 in18 Single PhotonTc EmissionI Computed Tomog- raphyC (SPECT) andF the latter in Positron Emission Tomog- raphy (PET). The underlying principle in diagnostic nu- 4 Medical radionuclide production clear medicine is that the radiation dose to the patient is as low as possible, compatible with the required qual- 4.1 General ity of imaging and the diagnostic advantage in compari- son to non-radioactive methods. The internal radionuclide Radioactivity is unique in the sense that, in spite of its haz- therapy, on the other hand, stipulates that a localised, ardous nature, it finds application in medicine both in di- well-defined radiation dose is deposited in a malignant agnosis and therapy (cf. [44]). Each application, however, or inflammatory tissue. Therefore, radionuclides emitting

Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production | 607 low-range highly-ionising radiation, i.e. - or particles, conversion and/or Auger electrons, are of great− interest. Many radionuclides are produced𝛼𝛼 using𝛽𝛽 neutron- induced reactions in nuclear reactors. However, in recent years considerable progress has been achieved in produc- tion of radionuclides using charged particle induced reac- tions, and the relevant technology is developing rapidly (cf. [45–47]). In principle, all four light charged particles, namely p, d, and could be utilized. The emphasis is, however, on3 protons4 which are more commonly avail- able and canHe be acceleratedHe to deliver both and beams. In particular, for production of the commonly+ used− PET radionuclides ( and , commerciallyH availableH single or two particle11 (p and18 d) small cyclotrons are now routinely used. Many ofC those cyclotronsF) are being utilized also for production of several non-standard positron emit- Figure 3: Excitation functions for the reactions (p,3n) , ters (cf. [46]). On the other hand, for production of some (d,4n) , ( ,2n) and ( ,n)75 drawn73 using the common SPECT-radionuclides, like and , or ther- 75data in References73 72 [483 –53]. 73 70 73As Se As Se Ge He Se Ge 𝛼𝛼 Se apeutic radionuclides, like and123 201, a medium- sized cyclotron is required. Furthermore,103 I 186 for productionTl of several other important radionuclides,Pd suchRe as , , ( , ( , etc., proton beams of energies52 67 up 68to 68 are82 desired82 (cf. [45]). In contrast to protons,Fe Cu the chargedGe Ga) particlesSr d, Rb) and have found only limited application,100 MeV though there3 are4 cases where the use of one of those particles may beHe advantageousHe as compared to the others. Yet such applications constitute special cases. The case of -particles is interesting. It is discussed below in some detail. The𝛼𝛼 cross sections of some of the -particle induced re- actions, for example ( ,xn) (see above), ( ,p), ( ,d), ( ,t) etc. are fairly high, especially for the𝛼𝛼 light and medium mass target nuclei. As𝛼𝛼 an example, the𝛼𝛼 excitation𝛼𝛼 func-𝛼𝛼 tions of the four investigated reactions for the production Figure 4: Thick target yields of calculated from the excitation of , namely (p,3n), (d,4n), ( ,2n) and functions of (p,3n) , 73 (d,4n) , ( ,2n) and Se 73 ( ,n), (cf. [7548–53]) are75 shown in Figure72 3 . The cross ( ,n) 75reactions73 shown75 in Figure733. 72 3 73 70 73 As As As Se Ge He Se 70sectionSe for the ( As,n) reactionAs is the highest.Ge He Thus, from Ge 𝛼𝛼 Se theGe viewpoint𝛼𝛼 of nuclear data, it is feasible to use the of irradiation. The calculated yield ( ) value (in ) rep- -particle induced𝛼𝛼 reaction for production purposes. The resents the maximum yield which can be expected from major disadvantage, however, comes to light while calcu- a given nuclear process. 𝑌𝑌 Bq lating𝛼𝛼 the thick target yield for a certain energy range ( Since the absorption of an -particle in a target ma- to ) which makes use of the following equation (cf. [54]): terial is much stronger than that of a proton, deuteron 1 𝐸𝐸 or -particle, the total range𝛼𝛼 of the -particle is much 2 𝐸𝐸 d shorter3 than that of any of the other three particles; cor- 𝐸𝐸2 d d −1 respondinglyHe the number of target nuclei𝛼𝛼 involved in the 𝐿𝐿 −𝜆𝜆𝜆𝜆 𝑁𝑁 ⋅𝐻𝐻 𝐸𝐸 -particle induced reaction is the lowest. Thus even if the 𝑌𝑌푌 𝐼𝐼퐼� 퐼 𝐼𝐼 ) ∫1 ( ) 𝜎𝜎𝜎𝜎𝜎 𝐸𝐸 where L is the𝑀𝑀 Avogadro number,𝐸𝐸 (𝜌𝜌𝜌𝜌�the enrichment (or cross sections of all reactions would be almost equal, the isotopic abundance) of the target nuclide, the mass yield𝛼𝛼 of the radioactive product in the -particle induced number𝑁𝑁 of the target element, the𝐻𝐻 projectile current, reaction would be much lower than in other reactions. d ( d ) the stopping power, the cross section𝑀𝑀 at en- The integral yields of calculated𝛼𝛼 for the above ergy𝐸𝐸 , the decay constant of the𝐼𝐼 product and the time mentioned four reactions are73 shown in Figure 4. Evidently, (𝜌𝜌𝜌𝜌휌 𝜎𝜎𝜎𝜎𝜎 Se

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Table 1: Radionuclides commonly produced using the -particle beam.

𝛼𝛼 Radio- Radiation Nuclear Energy Yielda) Purity References Other investigated nuclide emitted reaction range ( )() to reactionse) 1/2 𝑇𝑇 ( )() production [Reference] MBq/μAh % %( ) ( ,3p) MeV [56, 57] (t,p) (cf. [56, 57]) 28 − 27 28 26 28 b) Mg 21.1 h 𝛽𝛽 (100) Al(𝛼𝛼,n) Mg 140 → 30ca. 1.5 > 99 [60, 61] Mg(n,t) Mg[61] 30 + 27 30 32 30 b) P 2.5 min 𝛽𝛽 (100) Al(𝛼𝛼,n) P 24 → 10 ca.1000 > 99.9 [62–67] S (p,n)P [68] 38 + 35 38 38 (p,3n)38 [69, 70] K 7.6 min 𝛽𝛽 100 Cl 𝛼𝛼 K 22 → 7 400 > 99.8 40Ar 38K ( ) ( ,p) [74–76] Ar( ,p) K[77, 78] 43 − 40 43 44 (n,p)43 [79] K 22.2 h 𝛽𝛽 100 Ar 𝛼𝛼 K 21 → 10 7.0 97.5 43Ca 𝛾𝛾 43K EC ( ) ( ,2n) [84–87] Ca(p,n) K [88, 89] 77 ( ) 75 77 77 (p,2n)77 [89, 90] Br 57.0 h + 99.3 As 𝛼𝛼 Br 28 → 16 16.6 > 99.9 78Se(p,3n)77Br [91, 92] 𝛽𝛽 0.7 79Se(d,4n)77Br 77 [93] 79Br 77Kr → 77Br c) nat EC ( ) ( ,n) [97, 98] Br ( ,xn)Kr → Br[97, 98] 95 ( ) 92 95 3 95 Ru 1.65 h + 85.0 Mo 𝛼𝛼 Ru 28 → 14 240 > 99 Mo He Ru nat d) nat 𝛽𝛽EC (15.0) ( ,xn) [97–99] ( ,xn) [97, 98] 97 97 3 97 Ru 2.9 d EC ( 100) Mo(𝛼𝛼,n) Ru 28 → 16 1.8 > 99.8 [100, 101] Mo( He,3n) Ru [100, 101] 147 ( ) 144 147 147 3 147 Gd 38.1 h + 99.7 Sm 𝛼𝛼 Gd 27 → 12 4.8 > 99.8 Sm He Gd 𝛽𝛽EC (0.3) ( ,2n) [81, 104–110] , (p,spall) [112] 211 ( ) 209 211 232 ( 238 ,xn) 211 [113, 114] At 7.3 h 58 Bi 𝛼𝛼 At 28 → 10 17.5 > 99 209Th6,7 U 211 At211 a) Calculated from excitation𝛼𝛼 42 function. Bi Li Rn → At b) This is saturation yield. c) Value extrapolated to enrichment of . d) At after EOB. 92 e) For comments on these100% reactions, see text. Mo 15 h

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Figure 5: Schematic representation of a remotely controlled target and processing system for the production of via the ( ,n)-reaction (taken from Blessing and Qaim [66]). 38 35 K Cl 𝛼𝛼

The radionuclide ( ) was produced emitted from a source. In later years the same nu- for about two decades28 via the ( ,3p) reaction clear reaction was210 used to produce large amounts of by 1/2 using intermediate energyMg 𝑇𝑇-particles27= 21.1 [56 h,2857]. The yield employing higher energyPo -particles from a cyclotron30 [60, is rather low but in a irradiationAl 𝛼𝛼 withMg 61]. This short-lived non-standard positron emitterP has -particles at a beam current𝛼𝛼 of , about found some application in𝛼𝛼 biological studies both in an- of in no-carrier-added6h form were obtained140 for stud- MeV imals and humans using PET. The other investigated reac- ies𝛼𝛼 28 on plant physiology as well as20-scintigraphy μA 100 of MBq chil- tion, namely (n,t) , does not lead to satisfactory re- drenMg suffering from magnesium deficiency. The other re- sult since the32 yield is30 low [60]. In three other cases, viz. action rather commonly employed was𝛾𝛾 the (t,p) ( ,d) , S ( P,p) and (d, ) reactions, whereby either a tritium beam was used26 or a sequen-28 only28 cross30 section28 measurements3 30 were32 performed30 [61]. The tial reaction in a nuclear reactor was employedMg (forMg re- methodSi 𝛼𝛼 ofP choiceSi forHe productionP hasS therefore𝛼𝛼 P been the view cf. [56, 57]). The latter involved irradiating a mix- ( ,n) process. Typical batch yields of of ture of and whereby tritons released in the in- 27 and30 of were achieved [61]. teraction of neutrons with reacted with to yield 30AlThe𝛼𝛼 radionuclideP 30 ( 3− ) is also740MBq a short- 3 4 . TheLi productMg obtained after extensive26 chemical pro- livedPH non-standard300 MBq positron38 PO emitter and has been applied 1/2 cessing28 was not carrier-free.Li The ( ,3p)Mg reac- in myocardial blood flowK studies𝑇𝑇 = 7.6 using min PET. It is produced tionMg therefore became the method27 of choice28 for produc- using the ( ,n) reaction [62–67] and the technol- tion of . Several other reactionsAl 𝛼𝛼 with intermedi-Mg ogy is well35 developed38 to be able to obtain this radionuclide ate energy28 protons, e.g. (p,3p) , (p,4p) , in a pure formCl 𝛼𝛼 in quantitiesK of about (cf. [66]). nat nat (p,5p) Mg , (p,6pxn)30 28, 31(p,7pxn)28 A typical automated production system, taken from Ref- nat and32 (p,8pxn)28 , wereSi also28 investigatedMg P [58, 5928]Mg but erence [66], is shown in Figure 5.A 700 MBqpellet is irra- theS yields wereMg found28 Cl to be low [Mg59]. Ar Mg diated with -particles. Thereafter it is removed from the TheK radionuclideMg ( ) was historically target holder and is simply dissolvedNaCl in water. After fil- the first artificial transmutation30 product to be identified. tering through𝛼𝛼 a millipore filter, the solution is ready for 1/2 It was produced via theP 𝑇𝑇 nuclear= 2.5 reaction min ( ,n) application. which was induced by the low-energy ( 27) -particle30 Al 𝛼𝛼 P

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The other investigated processes for the production tracer development work. A few other reports dealing with of include the (p,n) reaction on highly en- cross section measurements of proton induced reactions riched38 [68] and38 the 38(p,3n) reaction with in- on isotopes of selenium, leading to the formation of termediateK 38 energy protonsAr 40 [69, 70K]. The38 former reaction is several bromine radionuclides, have also been published very promisingAr though the costAr of the highlyK enriched tar- in recent years (cf. [94–96]). For application oriented get material is rather high and the handling of enriched production of , however, the -particle induced is more difficult than that of an enriched isotope of reaction has hitherto77 been most successfully applied. 38 or . In the second case, i.e. the (p,3n)-reaction, The radionuclideBr ( 𝛼𝛼 ) is a non- a separationAr of from the accompanying40 impurity standard positron emitter95 potentially useful for preparing 1/2 Kr( Xe 38) was found to be very cumbersome.Ar A38 few ruthenocomplexes for diagnosticRu 𝑇𝑇 studies= 1.65 using h PET. It has other investigationsK report only low yields of (cf. [71Cl– been produced using nuclear reactions induced by both 1/2 nat 73𝑇𝑇]). The= 37.2 method min of choice to date for producing38 sufficient - and -particles on [97, 98] but due to rare quantities of in a radionuclidically pure formK is there- 3availability of the -particle beam and in view of the ra- fore the -particle38 induced reaction on . The level of dionuclidicHe 𝛼𝛼 purity3 of the product,Mo the -particle induced m the impurityK ( ) in 35 is reduced to reaction on enrichedHe is to be preferred, whereby 34 by𝛼𝛼 keeping the incident -particle38Cl energy on the a batch yield of up to 92 is expected.𝛼𝛼 1/2 target belowCl 𝑇𝑇. = 32.0 min K The radionuclide Mo ( ) is suitable for < 0.2% 𝛼𝛼 preparing ruthenocomplexes197 GBq for diagnostic studies using 1/2 [Correction added22 MeV after online publication June 08, 2016: SPECT. It has been producedRu via𝑇𝑇 nuclear= 2.9 reactionsd induced On page 10, line 2, “ (p,3p)-reaction” was changed to by both - and -particles [97–99]. However, in gen- “ (p,3n)-reaction”.]40 eral the 3 -particle induced production is preferred be- 40 Ar cause it isHe more economical.𝛼𝛼 The radioruthenium chemi- ArThe radionuclide ( ) is a longer lived cally separated𝛼𝛼 from the irradiated nat target contains isotope of potassium. It43 is used in plant physiological stud- three radionuclides, namely ( ) 1/2 ies and to some extent inK cardiology,𝑇𝑇 = 22.2 though h due to the rel- and . Nonetheless, if the94 productMo is allowed to decay95 1/2 atively high radiation dose caused by it, the emphasis has for about97 , radionuclidicallyRu pure𝑇𝑇 = 51.8is min obtained.Ru shifted over to the emitter discussed above as well Batch yieldsRu of up to have been97 achieved for this as to the analogue (SPECT)-isotope+ 38 . For the produc- radionuclide15 h(cf. [97, 98]). Ru tion of the most𝛽𝛽 useful reactionK 201 is the ( ,p) The radionuclide200 MBq( ) is suitable for process43 on a gas target (cf. [74–76]) andTl batch40 yields43 of SPECT studies, especially147 in combination with Magnetic 1/2 about K were achieved [76]. The level ofAr the𝛼𝛼 impu-K Resonance Imaging (MRI)Gd because𝑇𝑇 = 38.1 Gd his the most im- rity ( ) at EOB is about which can, portant contrast agent used in MRI. It has been pro- however,42 300 be MBq almost completely eliminated if the incident duced with high radionuclidic and chemical purity via the 1/2 -particleK 𝑇𝑇 energy= 12.3 is kept h below 2.5%[76]. Three other ( ,n) reaction on enriched investigated reactions, namely ( ,p) with target;144 a batch147 yield of about was achieved144 [100, 2 3 𝛼𝛼bremsstrahlung (cf. [77, 78]), 4417 MeV(n,p)43 with reactor 101Sm]. Another𝛼𝛼 Gd important production86.6% reaction investigatedSm O neutrons (cf. [79]) and (d,x)43 Ca[80𝛾𝛾 ] with43K intermediate20 MeV was ( ,3n) on400 MBqenriched energy deuterons need51 either highly43Ca expensiveK enriched target,147 whereby3 the147 yield of was about 147 higher 2 3 targets or the yield is low.V K but theSm productHe containedGd 14796.5% ( Sm O) The radionuclide ( ) has been as impurity [101]. The enrichedGd 149 is more80% expen- 1/2 used in labelling of molecules77 for SPECT studies. It sive than the enriched 0.3%. Nonetheless,144 Gd 𝑇𝑇 due= to 9.3 the d 1/2 is also potentially usefulBr for𝑇𝑇 Auger= 57.0 electron h therapy. impurity and due147 to the rareSm availability of the For its production a large number of nuclear reactions 149 beam, the -particleSm induced reaction on have been suggested (for early reviews cf. [81, 82] and appears3 Gd to be more interesting. Some additional144 reac- for a recent evaluation cf. [83]). Most successfully the tionsHe like nat (p,xn)𝛼𝛼 at [102] andSm nat ( ,2n) reaction was utilized [84–87] and the (d,xn) 146,147,148at [103] have also been product75 was77 achieved in amount. The other in- investigated.147,149,151,153Eu However, no mediumGd to100 large MeV scale produc- vestigatedAs 𝛼𝛼 reactionsBr include (p,n) [88, 89], tionEu of has hithertoGd been60 reported. MeV (p,2n) [89, 90], GBq(p,3n)77 77 [91, 92] The147 radionuclide ( ) is an -emitting and78 (d,4n)77 79[93]. TheSe77 amountBr77 of the prod- heavy halogenGd nuclide211 and thus it is of great potential 1/2 uctSe obtained79 Br in77 each case,77 however,Br wasKr sufficient → Br only for interest in -targeted internalAt 𝑇𝑇 radiotherapy.= 7.3 h It𝛼𝛼 has been Br Kr → Br

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Table 2: Radioactive high-spin isomeric states advantageously produced using the -particle beam.

𝛼𝛼 Isomeric Spin Mode of Preferential production Thick target Reference Other reactions used state and decay ( ) method yield c) 1/2 parity 𝑇𝑇 ( ) % Nuclear reaction Energy range ( ) MBq/μAh

a) m m IT (100) ( ,3n) MeV60 30 8.4 [119–123] (n,n ) [116] m 117m − 116 117 117 (p,2p3n)󸀠󸀠 117 [117, 118] nat m Sn 11/2 13.6 d Cd 𝛼𝛼 Sn → 121Sn( ,pxn)𝛾𝛾 117Sn [119] nat m Sb ( ,xn) 117 Sn[119, 120] In 𝛼𝛼 117 Sn b) m d) IT ( ) ( ,3n) 10 [124–126] Cd(n,𝛼𝛼 ) Sn (cf. [127, 128]) 193m + 192 193𝑚𝑚 192 193 b) m d) Pt 13/2 4.33 d IT (100) Os(𝛼𝛼,n) Pt 40 → 30 0.25 [124–126] Pt(n,𝛾𝛾) Pt (cf. [127]) m 195m + 192 195𝑚𝑚 194 (n,n 195) [116] Pt 13/2 4.02 d 100 Os 𝛼𝛼 Pt 24 → 18 195Pt 𝛾𝛾󸀠󸀠 195Pt a) Highly converted; energy of conversion electrons ~ . Pt 𝛾𝛾 Pt b) Highly converted; . c) Calculated from the excitation function for a highly150 enriched keV target. d) Using enriched target> 30 material. Auger electrons emitted per decay

produced for the last in high radionuclidic pu- produced using an -particle beam because they have rity via the ( ,2n) reaction in GBq quantities (for rather high spins (see Section 3.2.2). They are listed in Ta- early works209 cf. [104–10621140], years and for early review cf. [81]). ble 2. The decay characteristics𝛼𝛼 of each state, its major pro- In recent yearsBi more𝛼𝛼 optimisationAt work has been done duction method, the suitable energy range and the thick (see for example [107, 108]) and the separation methods target yield calculated from the excitation function are have been reviewed (cf. [109, 110]). Some new cross sec- given. In the last column other investigated reactions are tion measurements have also been done and the data have enumerated. Some more production details for each state been evaluated (for a review cf. [111]), but no substan- are given below. tial change has occurred. The spallation reaction (cf. [112]) The radioactive ( ) having a spin of g gives much lower yield of and the level of impurity lies above117m the ground state which is 1/2 is high. Also the reactions211 ( ,xn) stable.− The emitted conversionSn 𝑇𝑇 electrons= 13.6 d of117 energy about (cf. [113, 114]) have been investigated.209At 6,7 Worth211 emphasizing211 11/2 are315 ideally keV suited for some internalSn therapeutic is, however, that no reaction otherBi thanLi theRn ( ,2n) → pro-At studies, e.g. in the form of m -labelled porphyrin con- cess mentioned above has so far delivered with the jugates150 keV (cf. [115]). The radionuclide117 has been under consid- required quality and in quantities sufficient211 𝛼𝛼 for medical eration for more than three decadesSn and its small quanti- applications. At ties were hitherto produced via four routes: (1) (n,n ) m , (2) (p, n 2p3n) m , nat m nat m (3) 117( ,xn) 󸀠󸀠 117, (4) 121( ,pxn) (cf.117 [116– 4.3 Advantageous production of radioactive 119]). The (Sn,3n)117 reaction𝛾𝛾 Sn on a highlySb enriched𝛼𝛼117+ targetSn isomeric states using -particles (cf. [119Cd–122𝛼𝛼]) was foundSn to be moreIn 𝛼𝛼 interestingSn116 and an effi- cient chemical𝛼𝛼 separation method for m wasCd worked Radioactive isomeric states of a𝛼𝛼 few nuclides have very out [119]. Very recently, in an effort by117 Clear Vascular Inc. it suitable decay properties for therapeutic applications. In has been shown that only this reaction canSn lead to a prod- general, they are low-lying states having high nuclear uct of specific activity and chemical purity high enough to spins. They decay mostly to their respective ground states meet the requirement for medical application [123]. So this by a highly converted internal transition. The low-energy reaction has now become the method of choice for the pro- conversion electrons, or an avalanche of emitted Auger duction of m . electrons, can lead to precise localised internal therapy ef- The two117 radionuclides ( ) and fect, if the radioactive species is properly attached to an ( Sn ) are pure193m Auger electron emitters with 1/2 appropriate chemical carrier. Several such isomeric states 195mtheir energies distributed betweenPt and𝑇𝑇 = 4.33 d. Since 1/2 have been identified. Some of them are advantageously platinum-complexesPt 𝑇𝑇 = 4.02 d (like cis-di-chlorodiaminplatinum) 10 130 keV

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are two other shorter lived isomeric states whose forma- tion through -particle induced reactions appears to be preferable. The first one is ( ; spin ) g which decays 𝛼𝛼 by IT to44m the ground state ( + 1/2 ; spin ) and by ECSc to stable𝑇𝑇 = 2.444 d. Its forma-6 m m 1/2 tion in the +98.6%(p,n) and (d,2n)44 Screactions𝑇𝑇 = 3.9has h been investigated442 1.4%44 [129–131]44 and the latter44Ca reaction is more suitable.Ca Cross sectionSc measurementsCa onSc the reac- tion ( ,n) m,g show a still higher ratio for the forma- m tion41 of 44[132–136]. Thus this reaction could be more m suitableK44 for𝛼𝛼 the productionSc of . Its practical applica- tion, however,Sc has not been demonstrated.44 The isomeric Figure 6: Thick target yields of the radionuclides m and m , state m itself is not very usefulSc for diagnostic or ther- 193 195 calculated from the measured excitation functions, shown as apeutic44 studies, but it could serve as an in-vivo generator a function of the -particle energy (taken from UddinPt et al. [125]).Pt of g (cf.Sc [129]) which is a useful positron emitter, espe- 𝛼𝛼 cially44 in combination with its theranostic counterpart have been in use in chemotherapy as potent anti-tumour (cf. [137Sc]). An alternative way of its production could be47 via agents for a long time, both m and m have the / generator system (cf. [138, 139]). Sc a great potential in Auger electron193 therapy.195 So far the 44The second44 interesting shorter lived isomeric state is major drawback in their widespreadPt use has beenPt their Ti( Sc ; spin ) which decays by g non-availability with a high specific activity. Due to the IT197m to the ground state ( + ; spin ½ ) and m m 1/2 very high spin ( ) of both and , it Hgby𝑇𝑇 EC to= the23.8 stable h 197 13/2. The ratio ( ) was93.5%− mea- 1/2 𝑚𝑚 was considered more fruitful+ to investigate193 the 195-particle sured in the (p,n) Hg197m,g 𝑇𝑇 and= 64.1 h(d,2n)𝜎𝜎 m,g 𝜎𝜎𝑔𝑔 induced reactions13/2 on highly enrichedPt . In recentPt processes6.5% [140197–142] and197 foundAu to be197 at 197 for studies [124–126] the excitation functions192 of𝛼𝛼 the reac- protons and Au at Hgfor deuterons.Au The practi-Hg m m tions ( ,n) and ( ,3n) Os were mea- cal use of both the reactions for production0.88 19 has MeV been sured192 [124, 125]195 and thick target192 yields193 were calculated demonstrated1.35 [143, 14421]. MeV Very recently the advantageous which areOs shown𝛼𝛼 inPt Figure 6.Os In small𝛼𝛼 scalePt production production of m via the proton-induced reaction runs it could also be demonstrated that both the ra- has been reported197 and the medical application has also dionuclides can be produced with high specific activity; been discussed [145Hg]. On the other hand, the ( ) ratio m the achieved yield of is rather low but that of nat m,g𝜎𝜎𝑚𝑚 m increased to about in the ( ,xn) 𝑔𝑔 pro- over the energy range195 amounts 𝜎𝜎 cess [142] at . We therefore predict197 that the reac- to193 about [126Pt]. Thus this radionuclide can m,g 𝛼𝛼 tion ( ,2n) 2.2 on highlyPt enriched𝛼𝛼 targetHg mate- be producedPt in quantities sufficient𝐸𝐸 = 40 → for 30 therapeutic MeV appli- rial would195 lead27197 MeV to relatively high yields of the isomeric cations. 10 MBq/μA ⋅ h state. Pt 𝛼𝛼 Hg The other reactions used for the produc- tion of the two radionuclides are (n, ) m m (cf. [127]), (n, ) (cf. [127192, 128]),193 and m 4.4 Limited scale production of (n,n ) 194 [116]195 but even whilePt using𝛾𝛾 highlyPt enriched195 󸀠󸀠 isotopes195 Pt as target𝛾𝛾 materials,Pt the specific activity radionuclides using -particles achievedPt is𝛾𝛾 notPt high enough for therapeutic application. Table 3 lists some medically related radionuclides which The idea to produce via double neutron capture by 𝛼𝛼 m are either commonly used or are of potential use. They are and its subsequent195 decay to (i.e. via the route generally obtained via one of the three production routes: 193 m,gIr m195 (n, ) (n, ) − ) is interesting but (a) intermediate energy proton ( ) induced reac- Ir 𝛽𝛽 Pt 193has not been194 really195 attempted.195 Thus for the production of tion, (b) low-energy (p,n) reaction on highly enriched tar- theseIr two𝛾𝛾 radionuclides,Ir 𝛾𝛾 Ir the󳨀󳨀� -particlePt induced reactions get material, (c) (n, ) process. In> 30all MeV those cases limited are most promising. scale production could also be achieved through -particle In addition to the above mentioned𝛼𝛼 three longer lived induced reactions, as𝛾𝛾 discussed below. high-spin isomeric states whose advantageous production The radionuclides , , ( ), 𝛼𝛼 ( ), using -particles has been practically demonstrated, there , , , ( 52 ) and57 68 are68 positron72 emitters72 72 73 77 82 82 Fe Ni83 Ge Ga Se As 𝛼𝛼 As Se Kr Sr Rb Sr Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production | 613 176 ] 153 ] 200 ] 160 ] 170 ] 195 ] 173 ] 187 ] 185 ] 147 ] 155 ] 50 ] 50 ] 174 – 50 ] 92 ] 148 – 49 , 48 – 169 , 194 , 171 , 172 ] 94 , 198 – 158 – 186 , 49 , 91 , 149 , 146 , 154 , [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ ) 3 8 d) d) 15 22 93 8 a) 2.8 MBq/μAh ) yield 8 → 3 252 16 → 320 → 8 3900 1049 12 → 913 → 8 647 433 15 → 8 360 18 → 8 range target Energy Thick Reference 40 → 24 18 → 11 288 60 → 15 45 → 35 45 → 35 40 → 30 1.4 × 10 40 → 3027 → 19 1500 1776 MeV 100 → 60 ( Major production routes c) c) Ga) As) 68 ( c) c) 72 b) b) c) c) c) ( b) b) b) b) Fe b) Ge As Ni Cl Se Se Se Rb Kr b) 52 Cu 68 72 Ga Cl 57 Cu Br 72 72 73 81 77 F 61 66 34 m 61 76 ) ) 18 reaction Nuclear 34 m 𝛼𝛼 𝛼𝛼 (p,xn) (p,xn) (p,4n) (p,3n) (p, (p,n) (d, (p,4n) (p,4n) (p,3n) (p,2n) (p,n) (p,3n) (p,n) (p,n) (p,n) Ga Ge O S Ar Mn Co Ni Zn Ge As As As Se Br Kr 79 18 34 36 55 61 64 66 nat 75 75 76 82 75 nat 59 55 ] 166 ] 204 ] 192 ] 197 ] 206 ] ] ] – – ] ] , , – 207 ] 51 , , , 168 49 49 168 164 201 208 193 196 205 188 [ [ [ [ [ [ [ [ [ [ [ )( 33 40 90 a) -particles 𝛼𝛼 MBq/μAh ( -particle beam in comparison to their large scale production via other nuclear processes. 𝛼𝛼 ) yield MeV range target ( Energy Thick Reference 20 → 10 450 37 → 2028 → 13 115 126 55 → 25 260 b) b) b) b) b) b) b) Ga 20 → 10 Fe 30 → 20 0.11 Cu 33 → 23 185 Se Br Rb 27 → 13 Production method using 66 Ga As As Se Cl52 40 → 10 450 Cl 50 → 20 1608 61 Cu 18 → 10 72 Ni Kr 76 81 F 68 72 72 73 61 57 77 18 34 m 34 m ,xn) ,2n) ,2n) ,n) ,n) ,n) ,n) ,2n) ,3n) ,p) ,2n) ,n) ,n) 𝛼𝛼 ,d) 𝛼𝛼 𝛼𝛼 𝛼𝛼 ( 𝛼𝛼 𝛼𝛼 𝛼𝛼 𝛼𝛼 ,n) ,d) 𝛼𝛼 ( 𝛼𝛼 𝛼𝛼 𝛼𝛼 𝛼𝛼 ( ( ( ( ( ( 𝛼𝛼 ( ( ( ( ( reaction Nuclear 𝛼𝛼 𝛼𝛼 ( ( ( Cr Cu O S P Fe Co Ni Cu Ga Ga Ge Ge As Se Br 16 32 31 nat 54 59 58 nat 65 69 69 70 70 75 74 79 ) ) 3 % 97 ) 54 ) 40 ) 62 ) 89 ) 88 ) 66 ) 58 ) 87 ) 31 ) 46 ) 60 ) 11 ) 12 ) 42 ) 13 ) 69 ) 38 ) 34 ) ( ( ( ( ( ( ( ( ( ( 100 ) ) 56.5 ) 56.5 ) 43.5 ) 43.5 + + ( + + ( + + + + + + EC ( EC ( EC ( EC ( EC ( EC ( EC ( EC ( EC ( EC ( 𝛽𝛽 𝛽𝛽 𝛽𝛽 𝛽𝛽 𝛽𝛽 𝛽𝛽 𝛽𝛽 𝛽𝛽 𝛽𝛽 𝛽𝛽 + + EC ( EC ( EC ( 𝛽𝛽 𝛽𝛽 Mode of 1/2 1.5 d 8.5 d 8.3 h 3.4 h 9.4 h 7.1 h 𝑇𝑇 1.13 h 26.0 h 16.0 h 1.24 h 4.58 h 110 min 32.2 min Radionuclides produced in limited amounts using the Cl F Fe Ni Cu Ga Ga As Se Se Br Kr Rb Radio- Table 3: nuclide decay ( 18 34m 52 57 61 66 68 72 72 73 76 77 81

Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 614 | S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production ] 217 156 ] 221 ] 184 ] 163 ] 149 , 219 ] 219 ] 219 , 178 , 212 – 157 ] 161 ] 162 , 177 ] [ [ [ [ [ [ [ [ [ [ ) e) e) e) d) 16 a) 14 amounts amounts amounts MBq/μAh GBq GBq GBq ) yield : 3.1 b 12 → 8 18 → 5 4.8 : 206 b range target Energy Thick Reference 70 → 30 37 → 30 160 45 → 30 ∼ 100 80 → 30 ∼ 50 th MeV : 2100 b th ( 𝜎𝜎 14.5 → 10 370 𝜎𝜎 th 𝜎𝜎 Major production routes ) Lu b) c) 177𝑚𝑚푚𝑚𝑚 b) e) ( Lu b) c) b) b,c) Yb W b) Sm Sr Yb Sr Re I Rb 166 82 178 83 153 177 177𝑚𝑚푚𝑚𝑚 186 124 ) ) ) 82 m 𝛾𝛾 𝛾𝛾 reaction 𝛾𝛾 (p,4n) (n, (n, (p,xn) (n, (p,4n) (p,n) (p,n) (p,3n) (p,n) Te Sm Tm Lu Yb Ta W Rb Kr Rb 181 169 82 nat 124 152 176 176 85 186 211 ] 225 ] 211 ] , ] , , 210 220 224 210 [ [ [ [ )( a) -particles 𝛼𝛼 MBq/μAh ( ) yield MeV range target ( Energy Thick Reference Nuclear 22 → 1325 → 13 2.1 1.1 45 → 32 6.7 b) b) b,f) b) Lu b) W Yb b) b) Sm Sr 120 → 20 1.9 I Re Rb 178 166 82 Sr Production method using 153 177𝑚𝑚푚𝑚𝑚 124 186 83 82 m ,n) ,p) ,2n) ,n) ,xn) ,d) ,2n) ,xn) ,n) 𝛼𝛼 ,n) 𝛼𝛼 𝛼𝛼 𝛼𝛼 𝛼𝛼 𝛼𝛼 ( 𝛼𝛼 𝛼𝛼 ( ( ( 𝛼𝛼 ( ( ( ( 𝛼𝛼 ( ( Nuclear reaction . Sb Nd Er Yb Hf W Kr Sb Br Kr Ta 79 nat 80 121 nat 150 164 174 176 184 178 ) ) % 23 ) 24 ) 22 ) 77 ) 78 ) 76 ) 7.8 ( ( ( 100 ) 100 ) 100 ) 100 ) 100 ) ) 92.2 ( ( ( + + + 9.3 min − − EC ( EC ( EC ( 𝛽𝛽 𝛽𝛽 𝛽𝛽 − EC ( EC ( EC ( EC ( 𝛽𝛽 Mode of 1/2 2.3 d 6.7 d 𝛽𝛽 3.8 d 6.3 h 𝑇𝑇 4.15 d 1.93 d 𝛽𝛽 22.0 d 25.5 d 32.2 h Continued. Rb I Sm Yb Lu W Re Using highly enriched target material. Yield of parent. Calculated from excitation function. Using highly enriched target for irradiation in a medium-flux reactor. Using intermediate energy protons. Sr Sr For use as parent of Radio- Table 3: nuclide decay ( 82m 82 83 124 153 166 177 178 186 a) b) c) d) e) f)

Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production | 615 and useful for PET studies, is a emitter and so of potential therapeutic use,166 and has− found applica- tion in ( ) generator systemYb178 for𝛽𝛽 SPECT. They are all produced178 178 using intermediate energyW protons (cf. [48– 50, 146–163W]). TheTa suitable energy ranges for those reac- tions and the thick target yields calculated from the respec- tive excitation functions are given in Table 3. However, due to non-availability of intermediate energy protons, in a few laboratories the practical production of , , and using -particles has been demonstrated52 68 (cf.72 [46, 49, 5573, 164–166, 207]). The yields are, however,Fe muchGa lowerSe (cf. TableSe 3) than𝛼𝛼 via the major production route, but are sufficient for local tracer applications. In order to substan- tiate the possibility of developing an alternate production route, we considered the reaction ( ,n) to gen- erate . A thin layer of electrodeposited70 73 alloy on a wedged73 Cu-backing was irradiatedGe in𝛼𝛼 the internalSe70 tar- Figure 7: (Lower part) Schematic representation of the thermochro- 3 get systemSe of the compact cyclotron CV28 atCu anGe angle of matographic system used for the separation of no-carrier-added from a wedged target irradiated with with -particles at a beam current of about 73-particles. Radiogallium70 released from the target was deposited on 3 ∘ [55]. After the end of the irradiation the radiosele- theSe inner wall of theCu quartzGe tube immediately above28 theMeV target while nium6.2 was28 separated MeV 𝛼𝛼 by thermochromatography [55]. The radioselenium𝛼𝛼 was carried away to the zone outside the quartz tube profile100 μA of activity deposited in a quartz tube outside where it was collected in a small amount of warm . (Upper part) Radioactivity profile after separation. The activity of the the oven is73 shown in Figure 7. A clean separation of 2 2 side-product has been increased by a factor ofH O (taken from could be realizedSe and its batch yield amounted to 73 . Blessing et al.66 [55]). This quantity of should be sufficient for manySe appli- Ga 10 cations. For 73, , , , and 2, GBq how- ever, the application57 72Se of the77 -particle83 166 route for178 production (p,n)-process (cf. [212–217]), and the -production has so far notNi beenAs reported,Kr mainlySr dueYb to the highW cost route186 has so far not been investigated. of the required enriched target.𝛼𝛼 The cross sections on nat- WAs regards the (n, ) process, many of the𝛼𝛼 reactor ra- ural targets have, however, been measured in relation to dionuclides are produced via this route. The resulting the production of and [167, 234]. specific activity, however,𝛾𝛾 is often low. One such case is The radionuclides57 , 178 , , , , , . It is extensively used in radiotherapy [218] but and areNi also18 positron34mW 61 emitters66 and76 81 is no153 suitable alternative to (n, ) reaction has been found a82m emitter124 of interest inF therapy.Cl MostCu ofGa themBr186 are pro-Rb (cf.Sm [219]). In our laboratory the excitation function of the ducedRb− via theI (p,n) or (p,2n) reaction on the respectiveRe ( ,n) reaction was𝛾𝛾 investigated [220] and the highly𝛽𝛽 enriched target isotope (cf. [46, 94, 169–185]). For 140result is promising.153 It could be used for production of production, the low-energy (p, ) reaction no-carrierNd 𝛼𝛼 addedSm ; however, the cost will be rather has61 also been utilized [186, 187].64 The practical61 feasibil- high. A second case153 is . It is broadly used for tu- ityCu of the -particle induced reactionZn for𝛼𝛼 productionCu has mour treatment: in theSm form177 of bisphosphonates for bone been shown in cases of , m , , , and metastases, and with peptidesLu and monoclonal antibod- . The 𝛼𝛼-particle induced18 reactions34 61 to produce66 81 those ra- ies for soft tissue tumours, e.g. in neuroendocrine and 124dionuclides make use ofF eitherCl targetCu materialsGa ofRb natu- prostate diseases. It should, however, be pointed out that ralI isotopic𝛼𝛼 composition or if enriched material, then its besides the , there exists a longer lived iso- m cost is much lower (cf. [16–19, 188–211]). However, as ex- meric state 177( ) which is undesirable. pected, the yield of the product in -particle induced re- The direct production1776.7 d Lu via the (n, )-reaction leads to 1/2 action is lower than in the commonly used reaction. For a mixture of theLu two𝑇𝑇 isomers= 160176 and d since the abundance only the ( ,3n) reaction𝛼𝛼 cross sections have of the target isotope in natLu 𝛾𝛾is only , de- m been76 measured75 [174, 20976]. Similarly for only the spite its high capture176 cross section, the specific activ- m Br( ,n) Asreaction𝛼𝛼 crossBr sections have82 been reported ity of the product LuachievedLu is not high.2.59% Generally (cf.79 [237–82239]) which are, however, very discrepant.Rb Re- enriched target177 is used [219]. An alternative indi- gardingBr 𝛼𝛼 Rb, the practical method of production is the rect production route,Lu namely (n, ) , 186 > 70% 176 177 177

Re Bereitgestellt von | ForschungszentrumYb 𝛾𝛾 Yb Juelich → Lu Angemeldet Heruntergeladen am | 05.12.16 16:17 616 | S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production not only gives in the n.c.a. form but also the content reactions. In many other cases, however, production us- m of is lower177 [221]. An -particle induced reaction, ing an -particle beam is only done when intermediate en- m,g namely177 ( ,p)Lu , could also prove to be an in- ergy protons are not available or when a commonly used terestingLu174 alternative177 production𝛼𝛼 route, but so far it has not method𝛼𝛼 involving a highly enriched target isotope cannot been investigated.Yb 𝛼𝛼 The formationLu cross section of g be employed due to its high cost. nat using , however, has been measured [228]. 177 In our institute a new cyclotron (IBA Cyclone 30 XP) In addition to the radionuclides listed in Table 3 theLu has been recently installed and will soon go in opera- possibilityYb of production of several other radionuclides tion. Besides protons and deuterons, an -particle beam using -particle induced reactions has also been inves- of maximum energy will also be available. In ad- tigated, e.g. , , and in ( ,xn) reactions dition to routine production of a few standard𝛼𝛼 radionu- nat nat on 𝛼𝛼 and86 87[22288, 223] or 89 via ( ,xn) reactions clides, it is intended30 to MeV perform fundamental nuclear re- nat on and Y [Y224, 225Y ]. Besides82Zr cross𝛼𝛼 section mea- action studies as well as technologically oriented research surements,Rb chemical82 Sr separations andSr radionuclidic𝛼𝛼 qual- in support of our radionuclide development program. The ity controlKr checksKr were carried out. The yields of the prod- -particle beam is expected to broaden the scope of nu- ucts, however, were found to be very low. Furthermore, clear chemistry research related to development of both excitation functions of -particle induced reactions on non-standard𝛼𝛼 positron emitters and radionuclides of inter- a large number of target elements have been measured in est in internal radiotherapy. recent years in several laboratories𝛼𝛼 (cf. [226–236]). Some of those studies are of confirmatory character, dealing with the radionuclides , , m , etc. but a few de- References m scribe newer routes52 for 97 ,117 , , , and . Some of theFe reported99 Ru 99 dataSn 111 on targets131 of177 natu- 1. Alfassi, Z. B., Peisach, M. (Editors): Elemental Analysis by Par- ticle Accelerators. CRC Press, Inc., Boca Raton, Florida, USA, ral isotopic178 composition mayTc be potentiallyMo In usefulCs for de-Lu 1991; especially see contributions by Rauhala, E. (pp. 180– veloping production routes of a few radionuclides. How- W 241),England,J.B.A.(pp.243–278),Pineda,C.A.(pp.280– ever, further studies related to practical production using 305), Peisach, M. and Gihwala, D. (pp. 307–349). highly-enriched targets are needed. 2. Composto, R. J., Walters, R. M., Genzer, J.: Application of ion scattering techniques to characterize polymer surfaces and interfaces. Materials Science and Engineering R38, 107–180 (2002). 5 Concluding remarks 3. Pappalardo, L., Alberti, R., Cali, C., Garraffo, S., Litrico, P., Pappalardo, G., Rizzo, F., Romano, F. P.: The new PIXE-alpha The above discussion shows that the -particle beam has spectrometer for the analysis of Roman nummi surfaces. X- great advantages. It allows on one hand elemental analy- Ray Spectrometry 42, 33 (2013). sis of various materials and, on the other,𝛼𝛼 helps improve 4. Raghunatha Rao, V., Khathing, D. T., Chowdhury, D. P., Gan- their physical properties. The activation of materials in ir- gadharan, S.: An external-beam charged-particle (alpha) activation system for direct trace element analysis in liquids. radiations with -particles, i.e. the formation of radioac- Meas. Sci. Technol. 2, 610 (1991). tive products, is an interesting topic of study both from 5. Ditrói, F., Fehsenfeld, P., Khanna, A. S., Konstantinov, I., fundamental and𝛼𝛼 applied points of views. A comparison Mahunka, I., Racolta, P. M., Sauvage, T., Thereska, J.: The of experimental data with results of nuclear model calcu- thin layer activation method and its applications in industry, lations sheds some light on the reaction mechanism. In IAEA-TECDOC-924, Vienna, 1997, pp. 1–143. 6. Abbas, K., Gilliland, D., Stroosnijder, M. F.: Radioactivity mea- particular the formation of nuclear isomeric states, i.e. the surements for the thin layer activation technique. Appl. Ra- partial formation cross section, is difficult to reproduce by diat. Isot. 53, 179 (2000). theory. This topic thus still poses a challenge to both exper- 7. Chowdhury, D. P., Datta, J., Reddy, A. V. R.: Applications of imentalists and theorists. The cross section data obtained thin layer activation technique for the measurement of sur- as a function of -particle energy, on the other hand, are of face loss of materials: An Indian perspective. Radiochim. Acta great practical significance in the production of some med- 100, 139 (2012). 8. Ditrói, F., Tárkányi, F., Takács, S.: Wear measurement using ically related radionuclides,𝛼𝛼 though their yields are gener- radioactive tracer technique based on proton, deuteron and ally much lower than in proton or deuteron induced reac- -particle induced nuclear reactions on molybdenum. Nucl. tions. Nonetheless, there are several radionuclides which Instr. Meth. B 290, 30 (2012). are exclusively produced through the use of -particles, 9. Watson,𝛼𝛼 I. A., Waters, S. L., Silvester, D. J.: Excitation func- and there are a few low-lying high-spin isomeric states tions for the reactions producing , and from irra- 121 123 124 which are preferentially populated in -particle𝛼𝛼 induced I I I

𝛼𝛼 Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production | 617

diation of natural antimony with and particles with Technology, Gatlinburg, Tennessee, USA, May 1994, American energies up to . J. Inorg. Nucl.3 Chem.4 35, 3047 (1973). Nuclear Society, La Grange Park, Illinois, p. 186 (1994). 10. Homma, Y., Murakami, Y.: ProductionHe of Heby bombard- 26. Qaim S. M., Sudár, S., Fessler, A.: Influence of reaction chan- ing antimony target30 MeV with and particles.123 Radioisotopes nel on the isomeric cross-section ratio. Radiochim. Acta 93, (Tokyo) 25, 315 (1976). 3 I 503 (2005). 11. Prasad, R., Bhardwaj, H. D.:𝛼𝛼 ExcitationHe functions for 27. Qaim, S. M.: Activation cross sections, isomeric cross-section ( ,xn), (x – ), reactions in – range. Re- ratios and systematics of (n,2n) reactions at – . Nucl. 121,123port No. IC/86/41, ICTP, Trieste, Italy (1986). Phys. A185, 614 (1972). 12. Ismail,Sb M.:𝛼𝛼 Measurement=1 4 and analysis10 of40 the MeV excitation func- 28. Qaim, S. M., Ibn Majah, M., Wölfle, R., Strohmaier,14 15 B.:MeV Ex- tions for alpha-induced reactions on Ga and Sb isotopes. citation functions and isomeric cross-section ratios for the Phys. Rev. C 41, 87 (1990). (n,p) m,g and (n,p) m,g processes. Phys. Rev. 13. Singh, B. P., Bhardwaj, H. D., Prasad, R.: A study of pre- 90C42, 36390 (1990). 91 91 equilibrium emission in -induced reactions on . 29. Nesaraja,Zr C. D.,Y Sudár,Zr S., Qaim, S.Y M.: Cross sections for the m,g m,g Can. J. Phys. 69, 1376 (1991). 121,123 formation of and in neutron induced reac- 14. Bhardwaj, M. K., Rizvi, I.𝛼𝛼 A. Chaubey, A. K.: Alpha inducedSb tions near their69 thresholds:71 Effect of reaction channel on the reactions in antimony. Int. J. Mod. Phys. E3, 239 (1994). isomeric cross-sectionZn ratio. Phys.Zn Rev. C68, 024603 (2003). 15. Singh, B. P., Sharma, M., Musthafa, M. M., Bhardwaj, H. D., 30. Al-Abyad, M., Sudár, S., Comsan, M. N., Qaim, S. M.: Cross Prasad, R.: A study of pre-equilibrium emission in some sections and isomeric cross-section ratios in the interactions proton- and alpha-induced reactions. Nucl. Instr. Meth. A 562, of fast neutrons with isotopes of mercury. Phys. Rev. C73, 717 (2006). 064608 (2006). 16. Hassan, K. F., Qaim, S. M., Saleh, Z. A., Coenen, H. H.: Alpha- 31. Sudár, S. Szelecsényi, F., Qaim, S. M.: Excitation function and particle induced reactions on nat and with particular isomeric cross-section ratio for the (p, ) m,g process. reference to the production of the medically121 interesting ra- Phys. Rev. C48, 3115 (1993). 61 58 dionuclide . Appl. Radiat. Isot.Sb64, 101 (2006).Sb 32. Sudár, S., Qaim, S. M.: Excitation functionsNi 𝛼𝛼 of protonCo and 17. Tárkányi, F.,124 Takács, S., Király, B., Szelecsényi, F., Andó, L., deuteron induced reactions on iron and -particle induced Bergman, J., Heselius,I S. J., Solin, O., Hermanne, A., Shu- reactions on manganese in the energy region up to . bin, Yu.N., Ignatyuk, A. V.: Excitation functions of - and Phys. Rev. C50, 2408 (1994). 𝛼𝛼 nat -particle induced nuclear reactions on for production3 33. Sudár, S., Qaim, S. M.: Isomeric cross-section ratio25 for MeV of medically relevant and radioisotopes. Appl.He Radiat. the formation of m,g in neutron, proton, deuteron and Isot.𝛼𝛼 67, 1001 (2009).123 124 Sb -particle induced58 reactions in the energy region up to 18. Aslam, M. N., Sudár, S.,I Hussain,I M., Malik, A. A., Qaim, . Phys. Rev. C53Co, 2885 (1996). S. M.: Evaluation of excitation functions of - and -particle 34.𝛼𝛼 Sudár, S., Hohn, A., Qaim, S. M.: Nuclear model calculations induced reactions on antimony isotopes with3 special rele- on25 MeV proton and deuteron induced reactions on and vance to the production of iodine- . Appl.He Radiat. Isot.𝛼𝛼 69, with particular reference to the formation of the122 isomeric120 94 (2011). states m,g . Appl. Radiat. Isot. 52, 937 (2000). Te Te 19. Uddin, M. S., Hermanne, A., Sudár,124 S., Aslam, M. M., 35. Strohmaier,120 B., Faßbender, M., Qaim, S. M.: Production cross Scholten, B., Coenen, H. H., Qaim, S. M.: Excitation functions sections of groundI and isomeric states in the reaction sys- of -particle induced reactions on enriched and nat for tems , and p. Phys. Rev. C56, production of . Appl. Radiat. Isot. 69, 699123 (2011). 265493 (1997).3 92 94,95 20. Hohn,A.,Nortier,F.M.,Scholten,B.,vanderWalt,T.N.,Co-𝛼𝛼 124 Sb Sb 36. Hilgers,Nb K., + Sudár,He S.,Mo+𝛼𝛼 Qaim, S. M.:Mo+ Formation of the isomeric enen, H. H., Qaim,I S. M.: Excitation functions of (p,xn) pairs m,g and m,g in proton and -particle in- reactions from their respective thresholds up to 125 with duced139 nuclear reactions.141 Phys. Rev. C76, 0646013 (2007). special reference to the production of . Appl. Radiat.Te Isot. 37. Sudár, S., Qaim,Nd S. M.: CrossNd sections for theHe formation of m,g m,g m,g 55, 149 (2001). 124 100 MeV , and in alpha and -particle 21. Kastleiner, S., Shubin, Yu.N., Nortier, F. M.,I van der Walt, 195induced reactions197 on Pt:196 Effect of level density3 parameter on T. N., Qaim, S. M.: Experimental studies and nuclear model the calculatedHg isomericHg cross-sectionAu ratio. Phys.He Rev. C73, calculations on (p,xn) and (p,pxn) reactions on from their 034613 (2006). thresholds up to . Radiochim. Acta 92,85 449 (2004). 38. Uddin, M. S., Sudár, S., Qaim, S. M.: Formation of the iso- 22. Bayhurst B. P., Gilmore, J. S., Prestwood, R. J., Wilhelmy,Rb J. B., meric pair m,g in interactions of -particles with . Jarmie, N., Erkkila,100 B. MeV H., Hardekopf, R. A.: Cross sections for Phys. Rev. 194C84, 024605 (2011). 192 (n,xn) reactions between and , Phys. Rev. C12, 451 39. Rösch, F., Qaim,Ir S. M.: Nuclear data𝛼𝛼 relevant to the produc-Os (1975). tion of the positron emitting technetium isotope m via the 23. Rahman, M. M., Qaim, S.7.5 M.: Excitation28 MeV functions of some (p,n)-reaction. Radiochim. Acta 62, 115 (1993);94 Erratum neutron threshold reactions on isotopes of molybdenum. 9475, 227 (1996). Tc Nucl. Phys. A435,43(1985). 40. Rösch,Mo F., Novgorodov, A. F., Qaim, S. M.: Thermochromato- 24. Qaim, S. M., Mushtaq, A., Uhl, M.: Isomeric cross-section graphic separation of m from enriched molybdenum tar- m,g ratio for the formation of in various nuclear reactions. gets and its large scale94 production for medical application. Phys. Rev. C38, 645 (1988).73 Radiochim. Acta 64, 113 (1994).Tc 25. Qaim, S. M.: Recent developmentsSe in the study of isomeric 41. Faßbender, M., Novgorodov, A. F., Rösch, F., Qaim, S. M.: Ex- cross sections. Proc. Int. Conf. Nuclear Data for Science and citation functions of ( ,xn) processes 93 3 93𝑚𝑚�𝑚𝑚𝑚�𝑚𝑚�𝑚𝑚𝑚�𝑚𝑚�𝑚𝑚 Nb He Tc Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 618 | S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production

from threshold up to : possibility of production of 60. Sahakundu, S. M., Qaim, S. M., Stöcklin, G.: Cyclotron pro- m in high radiochemical purity using a thermochromato- duction of short-lived . Int. J. Appl. Radiat. Isot. 30,3 94graphic separation technique.35 MeV Radiochim. Acta 65, 215 (1994). (1979). 30 42. Denzler,Tc F.-O., Rösch, F., Qaim, S. M.: Excitation functions 61. Qaim, S. M., Ollig, H., Blessing,P G.: A comparative inves- of -particle induced nuclear reactions on highly enriched tigation of nuclear reactions leading to the formation of : comparative evaluation of production routes for m . short-lived and optimization of its production via the 92Radiochim.𝛼𝛼 Acta 68, 13 (1995); Erratum 75, 227 (1996). 94 ( ,n) 30process at a compact cyclotron. Int. J. Appl. Ra- 43. Filatenkov,Mo A. A., Chuvaev, S. V.: Experimental determinationTc 27diat. Isot.3033,P 271 (1982). of cross sections of a set of badly known neutron induced 62. Tilbury,Al 𝛼𝛼 R. S.,P Myers, W. G., Chandra, R., Dahl, J. R., Lee, reactions for heavy elements ( – ). Leningrad Report R. J.: Production of potassium- for medical use. No. 259, Khlopin Radium Institute, St. Petersburg, 2003. J. Nucl. Med. 21, 867 (1980). 44. Stöcklin, G., Qaim, S. M., Rösch,𝑍𝑍 F.: The 푍푍푍 79 impact of radioactiv- 63. Vandecasteele, C.,7 Vanderwalle,.6 minute T., Slegers,38 G.: Production of ity on medicine. Radiochim. Acta 70/71, 249 (1995). using the ( ,n) reaction. Radiochim. Acta 29, 71 45. Qaim, S. M.: The present and future of medical radionuclide 38(1981). 35 38 production. Radiochim. Acta 100, 635 (2012). 64. Qaim,K S. M., Sutisna,Cl 𝛼𝛼 M.K S., Ollig, H.: Production of via the 46. Qaim, S. M.: Development of novel positron emitters for med- ( ,n)-process at a compact cyclotron. Appl. Radiat.38 Isot. ical applications: Nuclear and radiochemical aspects. Ra- 3539, 479 (1988). K diochim. Acta 99, 611 (2011). 65. Guillaume,Cl 𝛼𝛼 M., De Landsheere, C., Rigo, P., Czichosz, R.: Auto- 47. Qaim, S. M.: Nuclear data relevant to the production and mated production of potassium- for the study of myocardial application of diagnostic radionuclides. Radiochim. Acta 89, perfusion using positron emission tomography. Appl. Radiat. 223 (2001). Isot. 39, 97 (1988). 38 48. Guillaume, M., Lambrecht, R. M., Wolf, A. P.: Cyclotron iso- 66. Blessing, G., Qaim, S. M.: A remotely controlled target and topes and radiopharmaceuticals – XXVII, . Int. J. Appl. processing system for routine production of via the Radiat. Isot. 29, 411 (1978). 73 ( ,n)-reaction. Appl. Radiat. Isot. 41, 122938 (1990). 49. Nozaki, T., Itoh, Y., Ogawa, K.: Yield of forSe various reac- 67.35 Tárkányi, F., Kovács, Z., Mahunka, I., Solin, O.,K Bergman, J.: tions and its chemical processing. Int.73 J. Appl. Radiat. Isot. ExcitationCl 𝛼𝛼 function of the ( ,n) reaction using gas 30, 595 (1979). Se targets. Radiochim. Acta 5435 , 165 (1991).38 50. Mushtaq, A., Qaim, S. M., Stöcklin, G.: Production of via 68. Tárkányi, F., Kovács, Z., Qaim,Cl S.𝛼𝛼 M.,K Stöcklin, G.: Production (p,3n) and (d,4n) reaction son arsenic. Appl. Radiat. Isot.73 39, of via the (p,n)-process at a small cyclotron. Appl. 1085 (1988). Se Radiat.38 Isot. 4338, 503 (1992). 51. Mushtaq, A., Qaim, S. M.: Excitation functions of - and - 69. Lambrecht,K R. M.,Ar Hara, T., Gallagher, B. M., Wolf, A. P., particle induced nuclear reaction son natural germanium:3 Ansari, A., Atkins, H.: Cyclotron isotopes and radiophar- Evaluation of production routes for . Radiochim.𝛼𝛼 ActaHe50, maceuticals – XXVIII. Production of potassium- for my- 27 (1990). 73 ocardial perfusion studies. Int. J. Appl. Radiat. Isot. 29, 52. Brodovitch, J. C., Hogan, J. J., Burns, K.Se I.: The pre-equilibrium 667 (1978). 38 statistical model: Comparison of calculation with two (p,xn) 70. Nagatsu, K., Kubodera, A., Suzuki, K.: Excitation func- reactions. J. Inorg. Nucl. Chem. 38, 1581 (1976). tion measurements of (p,3n) , (p,2pn) , 53. Calboreanu, A., Salagean, O., Pencea, C., Zimmer, K. W., Cio- (p,2p) reactions.40 Appl. Radiat.38 40 Isot. 50, 38938 (1999). canel, A.: Formation and decay of the compound nucleus in 71. Helus,40 F., Gasper,39 H., Maier-Borst,Ar W.:K RoutineAr productionCl of alpha induced reaction on . Rev. Roum. Phys. 32, 725 Arfor medicalCl use. J. Radioanal. Chem. 55, 191 (1980). (1987). 70 72. Yagi,38 H., Amano, R.: Production of carrier-free by means 54. Qaim, S. M.: Nuclear data forGe medical applications: An ofK photonuclear reactions. Int. J. Appl. Radiat.38 Isot. 32, 225 overview. Radiochim. Acta 89, 189 (2001). (1981). K 55. Blessing, G., Lavi, N., Qaim, S. M.: Production of via the 73. Daube, M. E., Nickles, R. J.: Development of myocardial per- ( ,n)-process using high current target materials.73 Appl. fusion tracers for positron emission tomography. Int. J. Nucl. 70Radiat. Isot. 43, 455 (1992). Se Med. Biol. 12, 303 (1985). 56. Probst,Ge 𝛼𝛼 H. J., Qaim, S. M., Weinreich, R.: Excitation functions 74. Clark, J. C., Thakur, M. L., Watson, I. A.: The production of of high-energy -particle induced nuclear reactions on alu- potassium- for medical use. Int. J. Appl. Radiat. Isot. 23, minium and magnesium: Production of . Int. J. Appl. 329 (1972). Radiat. Isot. 27,𝛼𝛼 431 (1976). 28 75. Guillaume,4 M.:3 Production en routine par cyclotron de fluor- 57. Weinreich, R., Qaim, S. M., Michael, H., Stöcklin,Mg G.: Pro- et potassium- á usage medical au moyen d’une cible duction of and by high-energy nuclear reactions gazeuse télécommandée. Nucl. Instr. Meth. 36, 185 (1976). for applications123 in life28 science. J. Radioanalyt. Chem. 30, 53 76.18 Fenyvesi, A., Tárkányi,43 F., Szelecsényi, F., Takács, S., (1976). I Mg Szücs, Z., Molnár, T., Sudár, S.: Excitation function and thick 58. Morrison, D. L., Caretto, Jr., A. A.: Excitation functions of target yield of the ( ,p) reaction: Production of . (p,xp) reactions. Phys. Rev. 127, 1731 (1962). Appl. Radiat. Isot. 4046, 1413 (1995).43 43 59. Lundqvist, H., Malmberg, P.: Production of carrier-free 77. Oka, Y., Kato, T., Namura,Ar 𝛼𝛼 K.: AK study on the yield of ( ,p)K reac- and by – protons on , , , , and28 : tions with bremsstrahlung. Bull. Chem. Soc. Jap. 41, excitation24 functions and chemical separation. Int. J. Appl.Mg 380 (1968). 𝛾𝛾 Radiat.Na Isot. 5030,180 33 (1979). MeV Si P S Cl Ar K 20 MeV

Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production | 619

78. Gray, F. C., Cole, C. M., Meaburn, G. M., Bruhhart, G.: Electron with particular reference to the production of medically inter- linear accelerator production of .J.Nucl.Med.14, 931 esting radionuclides and . Appl. Radiat. Isot. 60, 899 (1973). 43 (2004). 76 77 79. Poggenburg, J. K.: : the reactorK production, physical prop- 95. El-Azony, K. M., Suzuki,Br K., Fukumura,Br T., Szelecsényi, F., erties and potential43 availability of a useful radioisotope. Kovács, Z.: Excitation functions of proton induced reactions J. Nucl. Med. 12, 457K (1971). on natural selenium up to . Radiochim. Acta 97, 71 80. Qaim, S. M., Probst, H. J.: Excitation functions of deuteron (2009). induced nuclear reactions on vanadium with special reference 96. Spahn, I., Steyn, G. F., Vermeulen,62 MeV C., Kovács, Z., Szelec- to the production of : systematics of (d,xn) reaction cross sényi, F., Shehata, M. M., Spellerberg, S., Scholten, B., Co- sections relevant to the43 formation of highly neutron deficient enen, H. H., Qaim, S. M.: New cross section measurements for radioisotopes. Radiochim.K Acta 35, 11 (1984). the production of the Auger electron emitters and m . 81. Qaim, S. M., Stöcklin, G.: Production of some medically im- Radiochim. Acta 98, 749 (2010). 77 80 portant short-lived neutron-deficient radioisotopes of halo- 97. Comar, D., Crouzel, C.: Ruthenium- preparationBr with a com-Br gens. Radiochim. Acta 34, 25 (1983). pact cyclotron. Radiochem. Radioanalyt. Letters 27, 307 82. Qaim, S. M.: Recent developments in the production of , (1976). 97 and . Int. J. Appl. Radiat. Isot. 37, 803 (1986).18 98. Comparetto, G., Qaim, S. M.: A comparative study of the pro- 83. Hassan,75,76,77 H. E.,123 Qaim, S. M.: A critical survey of experimentalF duction of short-lived neutron deficient isotopes crossBr section data,I comparison with nuclear model calcula- in - and -particle induced nuclear reactions on94,95,97 natural tions and estimation of production yields of and in molybdenum.3 Radiochim. Acta 27, 177 (1980). Ru no-carrier-added form via various nuclear processes.77 77 Nucl. 99. Gessner,𝛼𝛼 M.,He Music, S., Babarovic, B., Vlatkovic, M.: Investi- Instr. Meth. B 269, 1121 (2011). Br Kr gation of the preparation of . Int. J. Appl. Radiat. Isot. 30, 84. Helus, F.: Preparation of carrier-free bromine- for medical 578 (1979). 97 use. Radiochem. Radioanal. Lett. 3, 45 (1970). 100. Denzler, F.-O., Rösch, F., Qaim,Ru S. M.: Excitation functions of 85. Nunn, A. D., Waters, S. L.: Target materials for77 the cyclotron - and -particle induced nuclear reactions on highly en- production of carrier-free . Int. J. Appl. Radiat. Isot. 26, riched 3 and : comparative evaluation of production 731 (1975). 77 routes𝛼𝛼 144 forHe . Radiochim.147 Acta 69, 209 (1995). 86. Blessing, G., Weinreich, R.,Br Qaim, S. M., Stöcklin, G.: Pro- 101. Denzler, F.-O.,Sm147 Lebedev,Sm N. A., Novgorodov, A. F., Rösch, F., duction of and via the ( ,3n) and Qaim, S. M.:Gd Production and radiochemical separation of ( ,2n) 75 reactions77 using 75 3-alloy as75 a high-current . Appl. Radiat. Isot. 48, 319 (1997). 75target material.77 Br Int. J.Br Appl. Radiat.As Isot.He33, 333Br (1982). 102. Lebedev,147 N. A., Novgorodov, A. F., Slovak, J., Khalkin, V. A., 3 87. Blessing,As 𝛼𝛼 G.,Br Qaim, S. M.: An improvedCu As internal -alloy Ekhu,Gd L.: preparations prepared from europium cyclotron target for the production of and and sep- irradiated146,147,149 by protons. Radioisotopy 29, 240 (1988). 3 aration of the by-product from the75 matrix activity.77Cu As Int. J. 103. Buchholz, M., Spahn,Gd I., Coenen, H. H.: Cross section mea- Appl. Radiat. Isot. 35, 92767 (1984). Br Br surements of100 proton MeV and deuteron induced reactions on nat- 88. Norton, E. F., Kondo, K., Karlstrom,Ga K., Lambrecht, R. M., Wolf. ural europium and yields of SPECT-relevant radioisotopes of A. P., Treves, S.: Cyclotron isotopes and radiopharmaceuticals gadolinium. Appl. Radiat. Isot. 91,8(2014). XXVI. A carrier-free separation of from . J. Radioanal. 104. Meyer, G.-J., Rössler, K.: Preparation of inorganic forms and Chem. 44, 207 (1978). 77 interhalogen compounds of via distillation techniques. 89. Janssen, A. G. M., van den Bosch, R.Br L. P., DeSe Goeij, J. J. M., Radiochem. Radioanal. Lett.21125, 377 (1976). Theelen, H. M. J.: The reactions (p,n) and (p,2n) as 105. Beyer, G.-J., Dreyer, R., Odrich,At H., Rösch, F.: Production of production routes for . Int. J.77 Appl. Radiat.78 Isot. 31, 405 at the Rossendorf cyclotron. Radiochem. Radioanal. (1980). 77 Se Se 211Lett. 47, 63 (1981). 90. Madhusudhan, C. P., Treves,Br S., Wolf, A. P., Lambrecht, R. M.: 106. Doberenz,At V., Nhan, D. D., Dreyer, R., Milanov, M., Khalkin, Cyclotron isotopes and radiopharmaceuticals XXXI. Improve- V. A.: Preparation of astatine of high specific activity in solu- ments in production and radiochemical separation from tions of a given composition. Radiochem. Radioanal. Lett. 52, enriched 77 . J. Radioanal. Chem. 53, 299 (1979). 119 (1982). 91. Diksic, M.,78Br Galinier, J.-L., Marshall, H., Yaffe, L.: Preparation 107. Henriksen, G., Messelt, S., Olsen, E., Larsen, R. H.: Op- of carrier-freeSe by (p,xn) reactions on natural bromine. Int. J. timisation of cyclotron production parameters for the Appl. Radiat. Isot. 28, 885 (1977). ( ,2n) reaction related to biomedical use of . 92. De Jong, D., Kooiman,Kr H.; Veenboer, J.Th.: and from 209Appl. Radiat.211 Isot. 54, 839 (2001). 211 decay of cyclotron produced and 76. Int. J. Appl.77 Ra- 108. Lindegren,Bi 𝛼𝛼 S.,At Bäck, T., Jensen, H. J.: Dry distillation of At diat. Isot. 30, 786 (1979) 76 77 Br Br from irradiated bismuth targets: A time-saving procedure211 with 93. Qaim, S. M., Stöcklin, G., Weinreich,Kr R.:Kr Excitation functions high recovery yields. Appl. Radiat. Isot. 55, 157 (2001). At for the formation of neutron deficient isotopes of bromine 109. Lahiri, S., Maiti, M.: Recent developments in nuclear data and krypton via high-energy deuteron induced reactions measurements and chemical separation methods in accel- on bromine: Production of , and . Int. J. Appl. erator production of astatine and technetium radionuclides. Radiat. Isot. 28, 947 (1977).77 76 79 Radiochim. Acta 100, 85 (2012). 94. Hassan, H. E., Qaim, S. M., Shubin,Br Br Y., Azzam,Kr A., Morsy, M., 110. Zalutsky, M., Pruszynski, M.: Astatine- : production and Coenen, H. H.: Experimental studies and nuclear model cal- availability. Curr. Radiopharm. 4, 177 (2011). culations on proton-induced reactions on nat , and 211 76 77 Se Se Se Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 620 | S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production

111. Qaim, S. M., Tárkányi, F., Capote, R. (Editors): Nuclear Data 128. Tóth, G.: A novel target for reactor-produced m . Int. J. for the Production of Therapeutic Radionuclides. Technical Appl. Radiat. Isot. 31, 411 (1980). 193 Reports Series No. 473, IAEA, Vienna, 2011, pp. 1–377. 129. Huclier-Markai, S., Kerdjoudj, R., Alliot, C., Bonraisin,Pt A., 112. Vachtel, V. M., Vinel, G. V., Vylov, C., Gromova, I. I., Nov- Michel, N., Haddad, F., Barbet, J.: Optimization of reaction gorodov, A. F., Norseev, Yu.V., Khalkin, V. A., Tschumin, V. G.: conditions for the radiolabeling of DOTA and DOTA-peptide Gasthermochromatographic method for astatine extraction. with m,g and experimental evidence of the feasibility of an Radiokhimiya 18, 886 (1976). in-vivo44 PET generator. Nucl. Med. Biol. 41, 36 (2014). 113. Meyer, G.-J., Lambrecht, R. M.: Excitation function for the 130. Alliot, C.,Sc Kerdjoudj, R., Michel, N., Haddad, F., Huclier- ( ,5n) nuclear reaction. Int. J. Appl. Radiat. Isot. Markai, S.: Cyclotron production of high purity m,g with 20931, 3517 (1980).211 deuterons from targets. Nucl. Med. Biol.44 42, 524 114. Greene,Bi Li J. P.: Nolen,Rn J., Baker, S.: Nickel-backed targets for (2015). 44 Sc 3 the production of . J. Radioanal. Nucl. Chem. 305, 943 131. Duchemin, C., Guertin,CaCO A., Haddad, F., Michel, N., Métivier, V.: m g (2015). 211 Bi Production of and with deuterons on : Cross 115. Jia, Z., Pu, M., Yang,At Y., Luo, S., Deng, H.: Synthesis and char- section measurements44 and44 production yield calculations.44 acterization of novel water-soluble m labeled porphyrin Phys. Med. Biol. 60Sc, 6847 (2015).Sc Ca m,g conjugates. J. Radioanal. Nucl. Chem.117 305, 681 (2015). 132. Bailey, S.: Yield ratios for the isomeric pair formed in 116. Mirzadeh, S., Knapp Jr., F. F., Alexander,Sn C. W., Mausner, L. F.: ( , n) and ( ,n) reactions. Phys. Rev. 123, 57944 (1961). Evaluation of neutron inelastic scattering for radioisotope 133. Riley, C., Ueno, K., Linder, B.: Cross sections andSc isomer ra- production. Appl. Radiat. Isot. 48, 441 (1997). tios𝛼𝛼 𝛼𝛼 for the 𝛼𝛼 ( ,n) m,g reaction. Phys. Rev. 135,B1340 117. Mausner, L. F., Mirzadeh, S., Ward, T. E.: Nuclear data for (1964). 41 44 production of m for biomedical application. Radiation 134. Keedy, C. R., Haskin,K 𝛼𝛼 L., Wing,Sc J., Huizenga, J. R.: Isomer ratios m,g m,g Effects 94, 59117 (1986). for the ( ,n) and ( ,n) reactions. Nucl. 118. Ermolaev, S. V., Zhuikov,Sn B. L., Kokhanyuk, V. M., Abramov, Phys. 8241, 1 (1966).44 55 58 A. A., Togaeva, N. R., Khamianov, S. V., Srivastava, S. C.: Pro- 135. Matsuo, T.,K 𝛼𝛼 Matuszek,Sc Jr. J. M.,Mn Dudey,𝛼𝛼 N. D.,Co Sugihara, duction of no-carrier added m from proton irradiated T. T.: Cross section ratios of isomeric nuclides produced antimony. J. Radioanalyt. Nucl.117 Chem. 280, 319 (2009). in medium-energy ( ,xn) reactions. Phys. Rev. 139, B 886 119. Qaim, S. M., Döhler, H.: ProductionSn of carrier-free m . (1968). Int. J. Appl. Radiat. Isot. 35, 645 (1984). 117 136. Zheltonozhsky, V. A.,𝛼𝛼 Mazur, V. M.: Investigation of the iso- 120. Fukushima, S., Hayashi, S., Kume, S., Okamura, H., Otozai,Sn K., meric ratio for m,g . Physics of Atomic Nuclei 63, 323 Sakamoto, K., Tsujino, R., Yoshizawa, Y.: The production of (2000), translated44 from Yadernaya Fizika 63, 389 (2000). high specific activities of tin. Bull. Chem. Soc. Jpn. 36, 1225 137. Rösch, F., Baum, R.Sc P.: Generator-based PET radiopharma- (1963). ceuticals for molecular imaging of tumours: On the way to 121. Montgomery, D. M. Porile, N. T.: Reactions of with in- theranostics. Dalton Transactions 40, 6104 (2011) termediate energy and ions. Nucl. Phys.116 A130, 65 138. Pruszyński, M., Loktionova, N. S., Filosofov, D. V., Rösch, F.: (1969). 3 4 Cd Post-elution processing of / generator-derived 122. Adam Rebeles, R., Hermanne,He He A., van den Winkel, P., for clinical application. Appl44 Radiat44 Isot. 68, 1636 (2010)44 Tárkányi, F., Takács, S., Daraban, L.: Alpha induced reactions 139. Filosofov, D. V., Loktionova, N.Ti S.,Sc Rösch, F.: A / ra-Sc on and : an experimental study of excitation func- dionuclide generator for potential application44 of 44-based tions.114 Nucl. Instr.116 Meth. B 266, 4731 (2008). PET-radiopharmaceuticals. Radiochim. Acta 98,Ti 14944 (2010)Sc 123. Stevenson,Cd N. R.,Cd George, G. S., Simón, J., Srivastava, S. C., 140. Vandenbosch, R., Huizenga, J. R.: Isomeric cross sectionSc ra- Mueller, D. W., Gonzales, G. R., Roger, J. A., Frank, R. K., Horn, tios for reactions producing the isomeric pair m,g . Phys. I. M.: Methods of producing high specific activity Rev. 120, 1313 (1960). 197 with commercial cyclotrons. J. Radioanalyt. Nucl. Chem. 305, 141. Tilbury, R. S., Yaffe, L.: Nuclear isomers m,g , Hgm,g m,g 99 (2015). Sn − 117m and formed by bombardment of197 gold with195 protons of 124. Hilgers, K., Coenen, H. H., Qaim, S. M.: Production of the energies196 from 8 to . Can. J. Chem. 41, 2634Hg (1963).Hg therapeutic radionuclides m and m with high spe- 142. Sudár, S.,Au Qaim, S. M.: Cross sections for the formation of m,g m,g m,g cific activity via -particle induced193 reactions195 on . Appl. , and60 MeV in - and -particle induced Radiat. Isot. 66, 545 (2008). Pt Pt 192 195reactions197 on : Effect196 of the level density3 parameters on 125. Uddin, M. S., Scholten,𝛼𝛼 B., Hermanne, A., Sudár, S.,Os Coenen, the calculatedHg isomericHg cross-sectionAu 𝛼𝛼 ratio.He Phys. Rev. C73, H. H., Qaim, S. M.: Radiochemical determination of cross sec- 034613 (2006).Pt tions of alpha particle induced reactions on for the pro- 143. Wilkniss, P. E., Beach, L. A., Marlow, K. W.: Production of m m,g duction of the therapeutic radionuclide 192. Appl. Radiat. carrier-free with a cyclotron. Radiochim. Acta 17, Isot. 68, 2001 (2010). 193 Os 110 (1972). 197 126. Uddin, M. S., Hermanne, A., Scholten, B., Spellerberg,Pt S., 144. Paans, A. M. J., Vaalburg,Hg W., Reiffers, S., de Graaf, E. J., Coenen, H. H., Qaim, S. M.: Small scale production of high Beerling-van der Molen, H. D., Wiegman, T., Rijskamp, A., purity m by the ( ,3n)-process. Radiochim. Acta 99, Woldring, M. G.: The production of radionuclides for medical th 131 (2011).193 192 applications with the cyclotron in Groningen. Proc. 8 127. Lange, R. C.,Pt Spencer,Os R. P.,𝛼𝛼 Harder, H. C.: The antitumor agent Int. Conf. on Cyclotrons and their Applications, Bloomington, cis- : distribution studies and dose calculations Indiana, USA, IEEE, p.280 2271 cm (1979). for m and m . J. Nucl. Med. 14, 191 (1973). 3 2 2 193Pt(NH ) Cl195 Pt Pt Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production | 621

145. Walther, M., Preusche, S., Bartel, S., Wunderlich, G., Freuden- 160. Ditrói, F., Tárkányi, F., Takács, S., Hermanne, A., Yamazaki, H., berg, R., Steinbach, J., Pietzsch, H.-J.: Theranostic mercury: Baba, M., Mohammadi, A.: Activation cross sections of longer m with high specific activity for imaging and therapy. lived products of proton induced nuclear reactions on cobalt 197Appl. Radiat. Isot. 97, 177 (2015). up to . J. Radioanal. Nucl. Chem. 298, 853 (2013). 146. Stang,Hg L. G.: The Brookhaven Linac Isotope Producer. Prog. 161. Tárkányi, F., Hermanne, A., Takács, S., Ditrói, F., Spahn, I., Nucl. Med. 4, 34 (1978). Ignatyuk,70 MeV A. V.: Activation cross sections of proton induced 147. Steyn, G. F., Mills, S. J., Nortier, F. M., Simpson, B. R. S., nuclear reactions on thulium in the – energy range. Meyer, B. R.: Production of via proton induced reactions Appl. Radiat. Isot. 70, 309 (2012). on manganese and nickel. Appl.52 Radiat. Isot. 41, 312 (1990). 162. Neirinckx, R. D., Ku, T. H., Holman, B.20 L.,45 Jones, MeV A. G., 148. Loc´h, C., Maziére, B., Comar,Fe D., Knipper, R.: A new prepara- Richards, P.: Production and purification of . Int. J. tion of . Int. J. Appl. Radiat. Isot. 33, 267 (1982). Appl. Radiat. Isot. 30, 341 (1979). 149. Qaim, S. M., Tárkányi, F., Takács, S., Hermanne, A., 163. Dmitriev, S. N., Zaitseva, N. G., Starodub, G.Ya.,W − 178Maslov, O. D., Nortier,Ge M., − Oblozinsky,68 P., Scholten, B., Shubin, Yu.N., Youxi- Shishkin, S. V., Shishkina, T. V., Buklanov, G. V., Sabelnikov, ang, Z.: Positron emitters, In: Charged Particle Cross-Section A. V.: High-purity radionuclide production: Material construc- Database for Medical Radioisotope Production: Diagnostic tion target chemistry for , , , , . Radioisotopes and Monitor Reactions. IAEA-TECDOC-1211, Nucl. Instr. Meth. A 397, 12526 (1997).97 178 235 236,237 Vienna, Austria, pp. 234–280 (2001). 164. Yano, Y., Anger, H. O.: ProductionAl Ru and chemicalW Np processingPu of 150. Adam-Rebeles, R., Hermanne, A., van den Winkel, P., De for medical use. Int. J. Appl. Radiat. Isot. 16, 153 (1965). Vis, L., Waegeneer, R., Tárkányi, F., Takács, S., Takács, M. P.: 165.52 Thakur, M. L., Nunn, A. D., Waters, S. L.: : improving its / production revisited: New excitation curves, target recoveryFe from cyclotron targets. Int. J. Appl.52 Radiat. Isot. 22, 68preparation68 and chemical separation-purification. Radiochim. 481 (1971). Fe ActaGe 101Ga, 481 (2013). 166. Akiha, F., Aburai, T., Nozaki, T., Murakami, Y.: Yield of for 151. Fitzsimmons, J. M., Mausner, L. F.: Determination of germa- the reactions of and on chromium. Radiochim. Acta52 18, nium isotope abundances and specific activity in accelerator 108 (1972). 3 Fe produced . J. Radioanal. Nucl. Chem. 305, 283 (2015). 167. Wanet, P. M., Cogneau,He M.𝛼𝛼 A., Apers, D. J.: Excitation functions 152. Rösch, F., Filosofov, D. V.: Production, radiochemical process- of – alpha induced reactions on iron: Production of ing and qualityGe−68 evaluation of , In: IAEA Radioisotopes . Radiochem. Radioanalyt. Letters 43, 1 (1980). and Radiopharmaceuticals Series No. 2: Production of long 168.57 Szelecsényi,25 50 MeV F., Kovács, Z., Nagatsu, K., Fukumara, K., lived parent radionuclides forGe−68 generators: , , and Suzuki,Ni K., Mukai, K.: Investigations of direct production of . STI/PUB/1436, IAEA, Vienna, 2010. 68 82 90 with low energy multiparticle accelerator. Radiochim. 153. Velikyan,188 I.: -based radiopharmaceuticals:Ge ProductionSr Sr 68Acta 100, 5 (2012). andW application68 relationship. Molecules 20, 12913 (2015). 169. Ruth,Ga T. J., Wolf, A. P.: Absolute cross sections for the produc- 154. Spahn, I., Steyn,Ga G., Nortier, F. M., Coenen, H. H., Qaim, S. M.: tion of via the (p,n) reaction. Radiochim. Acta 26, nat Excitation functions of (p,xn) reactions up to 21 (1979).18 18 18 with a focus on the production71,72,73,74 of for medical 170. Hess, E.,F Takács, S.,O Scholten,F B., Tárkányi, F., Coenen, H. H., and for environmentalGe studies. Appl.As Radiat.72 Isot. 65, Qaim, S. M.: Excitation function of the (p,n) nuclear 1057100 MeV73 (2007). As reaction from threshold up to . Radiochim.18 18 Acta 89, 155. Jennewein,As M., Schmidt, A., Novgorodov, A. F., Qaim, S. M., 352 (2001). O F Rösch, F.: A no-carrier-added / radionuclide genera- 171. Szelecsényi, F., Blessing, G., Qaim,30 MeV S. M.: Excitation functions tor based on distillation. Radiochim.72 72 Acta 92, 245 (2004). of proton induced nuclear reactions on enriched and 156. Qaim, S. M., Steyn, G. F., Spahn,Se I., Spellerberg,As S., van der : possibility of production of no-carrier-added61 and Walt, T. N., Coenen, H. H.: Yield and purity of produced 64 at a small cyclotron. Appl. Radiat. Isot. 44, 575Ni61 (1993). nat via the (p,xn) process. Appl. Radiat.82 Isot. 65, 247 172. Szelecsényi,64Ni F., Boothe, T. E., Tavano, E., Plitnikas, M.Cu E., (2007). 82 Sr Tárkányi,Cu F.: Compilation of cross sections/thick target yields 157. Kastleiner,Rb S., Qaim,Sr S. M., Nortier, F. M., Blessing, G., for , and production using targets up to van der Walt, T. N., Coenen, H. H.: Excitation functions of 66 proton67 energy.68 Appl. Radiat. Isot. 45, 473 (1994). (p,xn) reactions up to : integral 173. McCarthy,Ga D.Ga W., Bass,Ga L. A., Cutler, P. D., Shefer,Zn R. E., 85test of cross85𝑚𝑚 section�𝑚𝑚𝑚𝑚𝑚𝑚� data, comparison of production routes of Klinkowstein,30 MeV R. E., Herrero, P., Lewis, J. S., Cutler, C. S., An- Rband thick target yieldSr of . Appl.100 Radiat. MeV Isot. 56, 685 derson, C. J., Welch, M. J.: High purity production and poten- 83(2002). 82 tial applications of copper- and copper- . Nucl. Med. Biol. 158. Haasbroek,Sr F. J., Steyn, J., Neirinckx,Sr R. D., Burdzik, G. F., 26, 351 (1999). Cogneau, M., Wanet, P.: Excitation functions and thick target 174. Paans, A. J. M., Welleweerd,60 J., Vaalburg, W.,61 Reiffers, S., yields for radioisotopes induced in natural , , and Woldring, M. G.: Excitation function for the production of by medium energy protons. CSIR Research Report, FIS 89, bromine- : a potential nuclide for the labelling of radiophar- Pretoria, South Africa, 1976. Mg Co Ni maceuticals. Int. J. Appl. Radiat. Isot. 31, 267 (1980). 159. Johnson,Ta P. C., Lagunas-Solar, M. C., Avila, M. J.: The 175. Kovács, Z.,75 Blessing, G., Qaim, S. M., Stöcklin, G.: Production indirect production of no-carrier-added via the of via the (p,2n) reaction at a compact cyclotron. (p,3n) reaction. Int. J. Appl.57 Radiat. Isot. 35, Int.75 J. Appl. Radiat.76 Isot. 3675 , 635 (1985). 59371 (1984).57 57 Co Br Se Br Co Ni → Co

Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 622 | S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production

176. Tolmachev, V., Lövqvist, A., Einarsson, L., Schultz, J., 191. Lindner, L., Suér, T. H. G. A., Brinkman, G. A., Veenboer, J. T.: Lundqvist, H.: Production of at a low-energy cyclotron. A dynamic loop target for the in-cyclotron production of Appl. Radiat. Isot. 49, 1537 (1998).76 by ( ,d) reaction on water. Int. J. Appl. Radiat. Isot.18 24, 177. Kovács, Z. Tárkányi, F., Qaim, S.Br M., Stöcklin, G.: Production 12416 (1973). 18 F of m via the (p,n)-process at a low-energy cy- 192. Bakker,O 𝛼𝛼 C. N.F M., Kaspersen, F. M.: Production of by clotron82 – a potential substitute82 for . Appl. Radiat. Isot 42, -particle bombardment of . Int. J. Appl. Radiat.18 Isot. 8316.5 (1991). h Rb Kr 82 30, 61 (1979). F 2 178. Scholten, B., Kovács, Z., Tárkányi, F.,Rb Qaim, S. M.: Excitation 193. Zatolokin,𝛼𝛼 B. V., Konstantinov,SiO I. O., Krasnov, N. N.: Thick functions of (p,xn) reactions from to target yields of m and produced by various charged with special124 reference to124,123 the production of at a small particles on phosphorus,34 sulphur38 and chlorine targets. Int. J. cyclotron. Appl.Te Radiat. Isot.I46, 255 (1995).1246 31 MeV Appl. Radiat. Isot. 27Cl, 159 (1976).Cl 179. Sheh, Y., Koziorowski, J., Balatoni, J., Lom, C.,I Dahl, J. R., Finn, 194. Abrams, D. M., Knaus, E. E., Wiebe, L. I., Helus, F., Maier- R. D.: Low energy cyclotron production and chemical sepa- Borst, W.: Production of m from a gaseous target. Int. J. ration of no carrier added iodine- from usable, enriched Appl. Radiat. Isot. 35, 104534 (1984). tellurium- oxide/aluminium oxide solid solution target. 195. Helus, F., Gasper, H., Rettig,Cl G., Maier-Borst, W.: Cyclotron Radiochim. Acta 88, 169 (2000). 124 production of m for biomedical use. J. Radioanal. Nucl. 180. Qaim, S. M.,124 Hohn, A., Bastian, Th., El-Azoney, K. M., Bless- Chem. Lett. 9434, 149 (1985). ing, G., Spellerberg, S., Scholten, B., Coenen, H. H.: Some 196. Takei, M., Nagatsu,Cl K., Fukumura, T. Suzuki, K.: Remote con- optimisation studies relevant to the production of high-purity trol production of an aqueous solution of no-carrier-added and g at a small-sized cyclotron. Appl. Radiat. Isot. 58, m via the ( ,pn) nuclear reaction. Appl. Radiat. Isot. 65, 12469 (2003).120 34981 (2007). 32 181. Glaser,I M., Mackay,I D. B., Ranicar, A. S. O., Waters, S. L., 197. Nagatsu,Cl K., Fukumura,S 𝛼𝛼 T., Takei, M., Szelecsényi, F., Brady, F., Luthra, S. K.: Improved targetry and production of Kovács, Z., Suzuki, K.: Measurement of thick target yields for PET studies. Radiochim. Acta 92, 951 (2004). of the nat ( ,x) m nuclear reaction and estimation of its 182. Sajjad,124 M., Bars, E., Nabi, H. A.: Optimisation of produc- excitation function34 up to . Nucl. Instr. Meth. B 266, 709 tionI via (p,n) reaction. Appl. Radiat. Isot.12464, 965 (2008). S 𝛼𝛼 Cl (2006). 124 124 I 198. Engle, J., Barnhart, T. E., DeJesus,70 MeV O. T., Nickles, R. J.: Produc- 183. Nye, J. A., Avila-Rodriguez,Te I M. A., Nickles, R. J.: Production of tion of m and via the (d, ) reaction on and nat [ ]-iodine on an cyclotron. Radiochim. Acta 94, 213 gas at 34 . Appl.38 Radiat. Isot. 69, 75 (2011).36 (2006).124 199. Engle, J. W.,Cl Severin,Cl G. W., Barnhart,𝛼𝛼 T. E., Knutson,Ar Ar 184. Aslam,I M. N., Sudár,11 S., MeV Hussain, M., Malik, A. A., Shah, H. A., L. D., Nickles,8.4 MeV R. J.: Cross sections of the (d, ) m , Qaim, S. M.: Evaluation of excitation functions of proton and (d, ) and (d,p) nuclear reactions36 34 below deuteron induced reactions on enriched tellurium isotopes 40 . Appl.38 Radiat.40 Isot. 4170, 355 (2012). Ar 𝛼𝛼 Cl with special relevance to the production of iodine- . Appl. 200. Engle,Ar J.𝛼𝛼 W.,Cl Barnhart,Ar T. E., Severin,Ar G. W., Nickles, R. J.: The Radiat. Isot. 68, 1760 (2010). unrealized8.4 MeV potential of m for radiopharmaceutical re- 185. Kovács, Z., Tárkányi, F., Qaim, S. M., Stöcklin, G.: Excitation124 search with PET. Current34 Radiopharmaceuticals 4, 102 (2011). functions for the formation of some radioisotopes of rubid- 201. Homma, Y., Murakami, Y.: ProductionCl of by - and nat ium in proton induced nuclear reactions on , and bombardments on cobalt. Chem. Lett. Chem.61 Soc. Jpn.,3 397 m with special reference to the production of 82 ( (1976). Cu 𝛼𝛼 He 83generator radionuclide. Appl. Radiat. IsotopesKr4281, 329Kr81 (1991). 202. Fukumura, T. Okada, K., Szelecsényi, F., Kovács, Z., 186. Szelecsényi,Kr F., Kovács, Z., Suzuki, K., Okada, K., vanRb derKr) Suzuki, K.: Practical production of using natural Co Walt, T. N., Steyn, G. F., Mukherjee, S.: Production of us- target and its simple purification61 with a chelating resin for ing proton induced nuclear reactions on zinc for PET studies.61 -ATSM. Radiochim. Acta 92, 209Cu (2004). J. Radioanal. Nucl. Chem. 263, 539 (2005). Cu 203.61 Das, S. S., Chattopadhyay, S., Barua, L., Das, M. K.: Produc- 187. Thieme, S., Walther, M., Preusche, S., Rajander, J., Pietzsch, tionCu of using natural cobalt target and its separation H. J., Lill, J. O., Kaden, M., Solin, O., Steinbach, J.: High spe- using ascorbic61 acid and common anion exchange resin. Appl. cific activity via (p, ) reaction at low proton Radiat. Isot.Cu 70, 365 (2012). energies. Appl.61 Radiat.64 Isot. 7261, 169 (2013). 204. Aslam, M. N., Qaim, S. M.: Nuclear model analysis of exci- 188. Furukawa, M.,Cu Tanaka, S.:Zn Excitation𝛼𝛼 Cu function for the reaction tation functions of proton and deuteron induced reactions ( ,d) . J. Phys. Soc. Jpn., 16, 129 (1961). on and - and -particle induced reactions on 189.16 Clark, J. C.,18 Silvester, D. J.: A cyclotron method for the produc- leading64 to the3 formation of copper- : comparison of major59 tionO 𝛼𝛼 of .F J. Appl. Radiat. Isot. 17, 151 (1966). productionZn routes.He Appl.𝛼𝛼 Radiat. Isot. 94, 131 (2014). Co 190. Krasnov,18 N. N., Dimitriyev, P. P., Dimitriyeva, S. P., Konstanti- 205. Szelecsényi, F., Suzuki, K., Kovács,61 Z., Takei, M., Okada, K.: nov, I. O.,F Molin, G. A.: Experimental data on the yields of Production possibility of radioisotopes by alpha , , isotopes used for the detection of carbon, ni- induced reactions on cobalt60,61,62 for PET studies. Nucl. Instr. Meth- 11trogen,13 oxygen18 and neighbouring light element impurities by ods Phys. Res B 187, 153 (2002).Cu meansC N of activationF analysis with different charged particles 206. Aslam, M. N., Qaim, S. M.: Nuclear model analysis of exci- (p, d, , ). Proc. Conf. “The Use of Cyclotrons in Chemistry, tation functions of proton, deuteron and -particle induced Metallurgy3 and Biology” Oxford, September 1969 (ed. C. B. reactions on nickel isotopes for production of the medically Amphlett),He 𝛼𝛼 Butterworths, London, 1970, p. 341. interesting copper- . Appl. Radiat. Isot.𝛼𝛼89, 65 (2014).

61 Bereitgestellt von | Forschungszentrum Juelich Angemeldet Heruntergeladen am | 05.12.16 16:17 S. M. Qaim et al., Uses of alpha particles, especially in medical radionuclide production | 623

207. Jennewein, M., Qaim, S. M., Kulkarni, P. V., Mason, R. P., Her- 222. Kandil, S. A., Spahn, I., Scholten. B., Saleh, Z. A., Saad, manne, A., Rösch, F.: A no-carrier-added / radionu- S. M. M., Coenen, H. H., Qaim, S. M.: Excitation functions nat nat clide generator based on solid phase extraction.72 72 Radiochim. of ( ,xn) reactions on and from threshold up to Acta 93, 579 (2005). Se As : Possibility of production of , and . Appl. 208. Clark, J. C., Horlock, P. L., Watson, I. A.: generators. Radiat.𝛼𝛼 Isot. 65, 561 (2007).Rb Sr87 88 89 Radiochem. Radioanalyt. Lett. 25, 245 (1976). 223.26 Kandil, MeV S. A., Scholten, B., Hassan, K.Y F., Hanafi,Y H.Zr A., Qaim, 209. Alfassi, Z. B., Weinreich, R.: The productionKr − of 81m positron emit- S. M.: A comparative study on the separation of radioyttrium ters and : Excitation functions and yields for and from - and -targets via ion-exchange and solvent extrac- -particle75 induced76 nuclear reactions on arsenic. Radiochim.3 tion techniques, with special reference to the production of Acta 30Br, 67 (1982).Br He no-carrier-addedSr Rb , and using a cyclotron. J. Radio- 210.𝛼𝛼 Hassan, K. F., Spellerberg, S., Scholten, B., Saleh, Z. A., Qaim, analyt. Nucl. Chem.86 27987 , 823 (2009).88 S. M.: Development of an ion-exchange method for separation 224. Tárkányi, F., Qaim, S.Y M.,Y Stöcklin,Y G.: Excitation functions of radioiodine from tellurium and antimony and its appli- of - and -particle induced nuclear reactions on natural cation to the production of via the ( ,n)-process. krypton:3 Production of at a compact cyclotron. Appl. J. Radioanalyt. Nucl. Chem.124302, 689 (2014).121 Radiat.He Isot.𝛼𝛼39, 135 (1988).82 211. Uddin, M. S., Qaim, S. M., Hermanne,I A.,Sb Spahn,𝛼𝛼 I., Speller- 225. Tárkányi, F., Qaim, S. M.,Sr Stöcklin, G.: Excitation functions of berg, S., Scholten, B., Hossain, S. M., Coenen, H. H.: Ion ex- high-energy - and -particle induced nuclear reactions change separation and its application to production of by on natural krypton3 with special reference to the production of alpha induced reactions on antimony. Radiochim. Acta 124103, . Appl. Radiat.He Isot.𝛼𝛼41, 91 (1990). 587 (2015). I 226. Fenyvesi,82 A., Merchel, S., Takács, S., Szelecsényi, F., 212. Tárkányi, F., Takács, S., Szelecsényi, F., Ditrói, F., Her- Tárkányi,Sr F., Qaim, S. M.: Excitation functions of manne, A., Sonck, M.: Excitation functions of proton induced nat ( ,x) and nat (alpha,x) processes: In- nuclear reactions on natural tungsten up to . Nucl. vestigation3 of22,24 production of and 22,24 at a medium sized Instr. Meth. B 252, 160 (2006). cyclotron.Ne He Radiochim.Na ActaNe7922, 207 (1997).24 Na 213. Lapi, S., Mills, W. J., Wilson, J., McQuarrie, S.,34 Publicover, MeV J., 227. Hermanne, A., Tárkányi, F., Takács,Na S., Shubin,Na Yu.N., Kovalev, Schueller, M., Schleyer, D., Ressler, J. J., Ruth, T. J.: Produc- S. F.: Experimental determination of activation cross section tion cross sections of isotopes from proton bom- of alpha-induced nuclear reactions on nat . Nucl. Instr. Meth. bardment of natural tungsten.181−186 Appl. Radiat. Isot. 65, 345 B 251, 333 (2006). (2007). Re 228. Király, B., Tárkányi, F., Takács, S., Hermanne,Pt A., Kovalev, 214. Khandaker, M. U., Uddin, M. S., Kim, K., Lee, M. W., Kim, K. S., S. F., Ignatyuk, A. V.: Excitation functions of alpha-particle Lee, Y. S., Kim, G. N., Cho, Y. S., Lee, Y. O.: Excitation functions induced nuclear reactions on natural ytterbium. Nucl. Instr. of proton induced nuclear reactions on nat up to . Meth. B 266, 3919 (2008). Nucl. Instr. Meth. B 266, 1021 (2008). 229. Tárkányi, F., Hermanne, A., Király, B., Takács, S., Ditrói, F., 215. Hussain, M., Sudár, S., Aslam, M. N., Malik,W A. A., Ahmad,40 MeV R., Sonck, M., Kovalev, S. F., Ignatyuk, A. V.: Investigation of Qaim, S. M.: Evaluation of charged particle induced reaction excitation functions of alpha-induced reactions on nat : cross section data for production of the important therapeutic Production of the therapeutic radioisotope . Nucl. Instr. radionuclide . Radiochim. Acta 98, 385 (2010). Meth. B 267, 742 (2009). 131 Xe 216. Bonardi, M. L.,186 Groppi, F. Manenti, S., Persico, E., Gini, L., Ab- 230. Hermanne, A., Daraban, L., Adam-Rebeles, R.,Cs Ignatyuk, A., bas, K., Holzwarth,Re U., Simonelli, F., Alfassi, Z. B.: Production Tárkányi, F., Takács, S.: Alpha induced reactions on nat study of high specific activity NCA by proton and up to : Experimental and theoretical studies of the deuteron cyclotron irradiation. Appl. Radiat. Isot. 68, 1595 excitation functions. Nucl. Instr. Meth. B 268, 1376 (2010).Cd (2010). Re − 186g 231. Takács,38.5 S., MeV Hermanne, A., Tárkányi, F., Ignatyuk, A.: Cross- 217. Fassbender, M. E., Ballard, B., Birnbaum, E. R., Engle, J. W., sections for alpha-particle produced radionuclides on natural John, K. D., Maassen, J. R., Nortier, F. M., Lenz, J. W., Cutler, silver. Nucl. Instr. Meth. B 268, 2 (2010). C. S., Ketring, A. R., Jurisson, S. S., Wilbur, D. S.: Proton irra- 232. Tárkányi, F., Hermanne, A., Király, B., Takács, S., Ignatyuk, diation parameters and chemical separation procedure for A. V.: Study of excitation functions of alpha-particle induced the bulk production of high-specific-activity g using nuclear reactions on holmium for production. Appl. targets. Radiochim. Acta 101, 339 (2013). 186 Radiat. Isot. 68, 404 (2010). 167 3 218. Therapeutic Applications of Radiopharmaceuticals,Re TEC-DOC-WO 233. Ditrói, F., Hermanne, A., Tárkányi, F.,Tm Takács, S., Ignatyuk, 1228, IAEA, Vienna, 2001. A. V.: Investigation of the alpha-particle induced nuclear re- 219. Manual for Reactor Production of Radioisotopes, TEC-DOC- actions on natural molybdenum. Nucl. Instr. Meth. B 285, 125 1340, IAEA, Vienna, 2003. (2012). 220. Qaim, S. M., Spahn, I., Kandil, S. A., Coenen, H. H.: Nuclear 234. Tárkányi, F., Takács, S., Ditrói, F., Hermanne, A., Ignatyuk, data for production of , , and via novel A. V., Uddin, M. S.: Activation cross sections of alpha-particle routes. Radiochim. Acta88 95,140 313 (2007).153 169 induced nuclear reactions on hafnium and deuteron induced 221. Lebedev, N. A., Novgorodov,Y A.NdF., Misiak,Sm R., Brockmann,Yb J., nuclear reaction on tantalum: Production of / m Rösch, F.: Radiochemical separation of no-carrier-added generator. Appl. Radiat. Isot. 91, 114 (2014). 178 178 as produced via the (n, ) process. Appl.177 235. Hermanne, A., Adam-Rebeles, R., Tárkányi, F., Takács,W Ta S.: nat Radiat. Isot. 53, 421176 (2000). 177 177 Lu Alpha particle induced reactions on up to : Ex- Yb 𝛾𝛾 Yb → Lu perimental cross-sections, comparison with theoretical cal- Cr 39 MeV

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culations and thick target yields for medically relevant g 238. Homma, Y., Kurata, K.: Excitation functions for the production m production. Nucl. Instr. Meth. B 356, 28 (2015). 52 of - via the ( ,2n) and the ( ,3n) 236. Pupillo, G., Esposito, J., Gambaccini, M., Haddad, F., Fe reactions.81 81 Int. J. Appl.79 Radiat. Isot.81 30, 345 (1979).81 3 81 Michel, N.: Experimental cross section evaluation for inno- 239. Levkovskii,Rb Kr V. N.: MiddleBr mass𝛼𝛼 nuclidesRb ( Br– He) activa-Rb vative production via the ( ,n) reaction on target. tion cross sections by medium energy ( – ) pro- J. Radioanalyt.99 Nucl. Chem. 302, 911 (2014). 96 tons and -particles (experiment and systematics).𝐴𝐴 퐴 𝐴 100 Inter-Vesi, 237. Gilly, L. J.,Mo Henriet, P., Alves, P., Capron,𝛼𝛼 P. C.: AbsoluteZr cross- Moscow (1991), 215 pp. 𝐸𝐸 𝐸𝐸 50 MeV sections and excitation functions for particles induced reac- 𝛼𝛼 tions on bromine between and . Nucl. Phys. 55, 375 (1964). 𝛼𝛼 10 24 MeV

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