Cross sections of proton-induced reactions on 152Gd, 155Gd and 159Tb with emphasis on the production of selected Tb radionuclides

Cross sections are presented for various Dy, Tb and Gd radionuclides produced in the proton bombardment of 159Tb as well as for the reactions 152Gd(p,4n)149Tb and 155Gd(p,4n)152Tb up to 66 MeV. The experimental excitation functions are compared with theoretical predictions by means of the geometrydependent hybrid (GDH) model as implemented in the code ALICE/ASH, as well as with values from the TENDL-2012 library and previous literature experimental data, where available. Physical yields have been derived for the production of some of the medically important radioterbiums, namely 149Tb (radionuclide therapy), 152Tb (PET) and 155Tb (SPECT). The indirect production of high-purity 155Tb via the decay of its precursor 155Dy is reported. The possibility of a large-scale production facility based on a commercial 70 MeV cyclotron is also discussed

Neutron activation as an independent indicator of expected total yield in the production of 82Sr and 68Ge with 66 MeV protons

Introduction A method based on neutron activation is being developed to assist in resolving discrepancies between the expected yield and actual yield of radionuclides produced with the vertical-beam target station (VBTS) at iThemba LABS. The VBTS is routinely employed for multi-Ci batch productions of the radionuclide pairs 22Na/68Ga and 82Sr/68Ga using standardized natMg/natGa and natRb/natGa tandem targets, respectively [1]. The metal-clad target discs are bombarded with a primary beam of 66 MeV protons at an intensity of nominally 250 µA. The encapsulation materials are either Nb (for Mg and Ga) or stainless steel (for Rb) which serve to contain the molten target materials during bombardment and act as a barrier to the high-velocity cooling water which surrounds the targets in a 4π geometry. The natRb/natGa targets are typically bombarded according to a two-week cycle while natMg/natGa targets are bombarded on an ad-hoc basis, depending on a somewhat unpredictable 22Na demand. A too-large deviation between expected yield and actual yield has at times plagued this programme. These deviations can manifest both as an apparent loss or an apparent gain (relative to the expected yield) by up to about 15% in either direction. The resulting uncertainty of up to 30% (in the worst case) from one production batch to another can be costly and is unacceptable in a large-scale production regimen. This phenomenon is believed to be brought about by two types of problems: (1) Production losses, e.g. during the radio-chemical separation process or incomplete recovery of activated target material during the decapsulation step. (2) Incorrect values obtained for the accumulated proton charge. A problem of type (1) will always result in a loss of yield. A problem of type (2) can manifest as an apparent loss or gain. In an effort to get a handle on this second type of problem, neutron activation of suitable material samples, embedded in a target holder, is being investigated as an independent indicator of the total yield. For this purpose, samples of Co, Mn, Ni and Zn were activated during production runs and Co was found to be the most appropriate. Preliminary results will be presented after first discussing why the determination of the accumulated pro-ton charge is a problem with the VBTS. Materials and Methods The VBTS consists of a central region in which a target holder is located during bombardment as well as two half-cylindrical radiation shields which completely surround the target. The shields can be moved away from the central region on dedicated rails, e.g. when repairs or maintenance is required. FIGURE 1 shows the VBTS with the shields moved to the “open” position. As some components of the station are located below the vault floor, with the target position near floor level, it proved difficult to electrically isolate the VBTS as was done for the two horizontal-beam target stations at iThemba LABS [1]. The VBTS does not act as a Faraday cup like the other target stations. Instead, the beam current and accumulated charge is measured by means of a calibrated capacitive probe [1,2]. There appears to be a variation in the response of the capacitive probe, sensitive to the beam microstructure, in particular a dependence on the beam packet length. This problem is not yet fully resolved. FIGURE 2 (a) shows the beamstop of a VBTS target holder with several Co samples mounted on the outside as well as one each of Ni, Mn and Zn. The samples are small “tablets” with a 10 mm diameter and 1 mm thickness. The reactions of interest are 59Co(n,γ)60Co, 59Co(n,3n)57Co, nat-Ni(n,X)60Co, natNi(n,X)57Co, natZn(n,X)65Zn and 55Mn(n,2n)54Mn. The relevant half-lives are 60Co(5.271 a), 57Co(271.8 d), 65Zn(244.3 d) and 54Mn(312.2 d). The half-life should be long compared to the two-week cycle in order to reduce the dependence on the exact beam history, which is very fragmented over any production period. In this respect, 60Co is considered to be particularly attractive as its long half-life of more than 5 years leads to a negligible effect by the beam history. Note that the tandem targets, shown in FIGURE 2 (b), are mounted just upstream of the beamstop – in fact, the targets and beamstop form a single unit before being fitted into the target holder. At the end of bombardment, all samples were assayed for their characteristic γ-emissions using standard off-line γ-ray spectrometry with an HPGe detector connected to a Genie 2000 MCA. Calculations of the neutron fluence density in the central sample volume on the beamstop were also performed using the Monte Carlo radiation transport code MCNPX. For these calculations, the entire VBTS, a Rb/Ga target and the vault walls were included in the model. Results and Conclusion All samples activated significantly – copious amounts of 60Co were detected in the Co discs after a two-week run. The neutron fluence density for the case of a 250 µA, 66 MeV proton beam on a natRb/natGa tandem target is shown in FIGURE 3. The dominance of low-energy neutrons is evident, which is in part due to the large amount of paraffin-wax shielding material in close proximity to the target. While reactions such as the (n,2n) and (n,3n) would be sensitive to the more energetic part of the neutron spectrum, the (n,γ) capture reaction benefits from the large low-energy component. This explains the copious amounts of 60Co formed. It was therefore decided to only retain the central Co sample for subsequent bombardments, as shown in FIGURE 4. The first results are shown in TABLE 1. The accumulated charge as obtained from the capacitive probe (Q), the specific 60Co activity (A) at the end of bombardment (EOB), and their ratio (A/Q) are presented in the table, together with the deviation of individual ratios relative to their average for the case of the Mg/Ga tandem tar-gets only. Note that all samples were counted until the statistical uncertainties were negligible. Any systematic uncertainties are ignored at this stage as they are considered to remain the same from one batch production to another. For the sake of argument, the average value of the ratio is taken as the expected value. A positive deviation of the A/Q value is then indicative of a too-small value of the accumulated charge obtained from the capacitive probe, leading to a corresponding overproduction. Likewise, a negative value is indicative of a too-large value of the accumulated charge, leading to a corresponding underproduction. It is certainly true that the data in TABLE 1 are currently very limited. It is envisaged, however, that with time the growing database of values will assist in reducing the uncertainty in determining the accumulated charge and reduce the discrepancies between predicted and actual yields significantly. TABLE 1 illuminates the underlying problem satisfactorily. The four Mg/Ga tandem target bombardments, on identical targetry, were performed successively. The neutron activation correlates well the with actual yields, pointing directly to the current integration as the main source of error. The method already proves to be useful. An indication of an over or underprediction can be obtained prior to the target processing by recovering and measuring the Co disc. This in-formation can be used to make a decision concerning the present batch production and/or the subsequent one. One can either add beam to the present production target and/or in-crease/reduce the total beam on the subsequent production target to compensate for an expected overproduction or shortfall. In conclusion, we would like to stress that the capacitive probes show great promise and that better understanding and/or possibly some development of their signal processing algorithm may improve their ability to measure the accumulated charge to the desired accuracy. Segmented capacitive probes used at iThemba LABS and elsewhere for beam position measurement [1,3] are not affected by beam microstructure as only the ratios of the signal strengths on the different sectors are important. In this case, changes in response affect all sec-tors equally and the ratios are unaffected

Saturation conditions in elongated single-cavity boiling water targets

Introduction It is shown that a very simple model reproduces the pressure versus beam current characteristics of elongated single-cavity boiling water targets for 18F production surprisingly well. By fitting the model calculations to measured data, values for a single free parameter, namely an overall heat-transfer coefficient, have been extracted for several IBA Nirta H218O targets. IBA recently released details on their new Nirta targets that have a conical shape, which constitutes an improvement over the original Nirta targets that have a cylindrical shape [1,2]. These shapes are shown schematically in FIGURE 1. A study by Alvord et al. [3] pointed out that elevated pressures and temperatures in excess of the saturation conditions may exist in a water target during bombardment. However, as long as the rate of condensation matches the rate of vaporization, the bulk of the system should remain at saturation conditions. Superheated regions are therefore likely to form but also likely to disappear rapidly, typically on the scale of a few milliseconds. Even though the boiling process is generally quite complex, enhanced by radiation-induced nucleation, the presence of fast mixing mechanisms in the water volume justifies some simplifications to be made. Materials and Methods The simplified model assumes that the bulk of the target water has a constant temperature, which is the same as the inner wall temperature of the cavity, Tw. A second simplification is to neglect the temperature difference across the target chamber wall, which is only justified if the wall is thin. The boiling is not explicitly taken into consideration, including the rather complex boiling behaviour at the Havar window, except to acknowledge that it is the main mixing mechanism. Large temperature gradients can briefly exist in the water medium but they also rapidly disappear. A further assumption is that a single, overall convective heat-transfer coefficient can be applied, which is constant over the entire water-cooled surface. As the wall thickness is neglected, the heat-transfer surface is assumed to be the inner surface of the cavity, excluding the surface of the Havar window. One can then write down an energy balance between the beam heating and the convection cooling (Newton’s law of cooling), where Ib is the beam intensity, ΔE is the energy windows of the target (taken as 18 MeV), h is the convective heat-transfer coefficient, A is the inner cavity surface through which the heat has to be transferred from the target-water volume to the cooling water, and T0 is the cooling-water temperature. The saturated vapour pressure of water versus temperature is a characteristic curve, given by the steam tables [4]. Assuming the bulk of the system at saturation conditions, one gets from (1) and (2). The function f is represented by a polynomial. The only unknown in Equation (3) is the overall convective heat-transfer coefficient h. Our approach was to adjust h until a good fit with a set of measured data was obtained. It also has to be mentioned that subtle differences in the physical properties between 18O-water and natural water have been neglected. All in all, quite a few assumptions and simplifications are made in deriving Equation (3) and the system is, admittedly, much more complex. Nevertheless, the results obtained by applying Equation (3) are rather interesting. Results and Conclusion Measured data and corresponding calculations are shown in FIGURE 2 for three different conical targets and one cylindrical target. The extracted convective heat-transfer coefficients are pre-sented in TABLE 1 for the four cavities. As can be seen in FIGURE 2, while there are some differences between the data and calculated curves, especially towards lower beam currents, the overall agreement is remarkably good. It is possible that the better agreement towards higher beam intensities is related to more ebullient boiling and more rapid mixing, i.e. closer to the conditions that the model assumes. The values obtained for the overall convective heat-transfer coefficient are also remarkably similar. This tells us that, by and large, all the cavities perform in a similar way and the performance in terms of maximum operational beam current depends largely on the available surface to effectively remove the heat from. The values of h increase marginally if a smaller value is adopted for the cooling water. Note that the choice of T0 = 30 ᵒC used to obtain the results in TABLE 1 is typical for the room temperature closed-loop cooling system used at iThemba LABS, once it has stabilized under operational conditions. A study by Buckley [5] on a quite different target design reports a value of h = 0.49 W cm−2 ᵒC−1, which is reassuringly similar. That study describes a cylindrical target cavity with a volume of 0.9 cm3, 8 mm deep, cooled with 25 ᵒC water from the back, operated with a 15 MeV proton beam with an intensity of 30 µA. The Nb Nirta targets are typically filled with 18O-water to about 60% of the cavity volume (see refs. [1,2] for the recommended values). The elongated shape, in combination with the ebullient properties of the boiling water, prevents burn-through. All the targets deliver the expected saturation yield. The targets are self-regulating ─ no external gas pressure is required. While the thermosyphon targets seemingly take advantage of a superior concept, we are now questioning whether this is really so in practice? It is not clear to us that the much more complex thermosyphon targets deliver any operational and/or performance advantages compared to the simple elegance of these elongated, single-cavity boiling target designs

Isotopic Production Cross Sections in Proton-Nucleus Collisions at 200 MeV

Intermediate mass fragments (IMF) from the interaction of $^{27}$Al, $^{59}$Co and $^{197}$Au with 200 MeV protons were measured in an angular range from 20 degree to 120 degree in the laboratory system. The fragments, ranging from isotopes of helium up to isotopes of carbon, were isotopically resolved. Double differential cross sections, energy differential cross sections and total cross sections were extracted.Comment: accepted by Phys. Rev.

No evidence of an 11.16 MeV 2+ state in 12C

An experiment using the 11B(3He,d)12C reaction was performed at iThemba LABS at an incident energy of 44 MeV and analyzed with a high energy-resolution magnetic spectrometer, to re-investigate states in 12C published in 1971. The original investigation reported the existence of an 11.16 MeV state in 12C that displays a 2+ nature. In the present experiment data were acquired at laboratory angles of 25-, 30- and 35- degrees, to be as close to the c.m. angles of the original measurements where the clearest signature of such a state was observed. These new low background measurements revealed no evidence of the previously reported state at 11.16 MeV in 12C

Tufa stromatolite ecosystems on the South African south coast

Following the first description of living marine stromatolites along the South African east coast, new investigations along the south coast have revealed the occurrence of extensive fields of actively calcifying stromatolites. These stromatolites have been recorded at regular distances along a 200-km stretch of coastline, from Cape Recife in the east to the Storms River mouth in the west, with the highest density found between Schoenmakerskop and the Maitland River mouth. All active stromatolites are associated with freshwater seepage streams flowing from the dune cordon, which form rimstone dams and other accretions capable of retaining water in the supratidal platform. Resulting pools can reach a maximum depth of about 1 m and constitute a unique ecosystem in which freshwater and marine organisms alternate their dominance in response to vertical mixing and the balance between freshwater versus marine inflow. Although the factors controlling stromatolite growth are yet to be determined, nitrogen appears to be supplied mainly via the dune seeps. The epibenthic algal community within stromatolite pools is generally co-dominated by cyanobacteria and chlorophytes, with minimal diatom contribution

Second T = 3/2 state in 9^9B and the isobaric multiplet mass equation

Recent high-precision mass measurements and shell model calculations~[Phys. Rev. Lett. {\bf 108}, 212501 (2012)] have challenged a longstanding explanation for the requirement of a cubic isobaric multiplet mass equation for the lowest $A = 9$ isospin quartet. The conclusions relied upon the choice of the excitation energy for the second $T = 3/2$ state in $^9$B, which had two conflicting measurements prior to this work. We remeasured the energy of the state using the $^9{\rm Be}(^3{\rm He},t)$ reaction and significantly disagree with the most recent measurement. Our result supports the contention that continuum coupling in the most proton-rich member of the quartet is not the predominant reason for the large cubic term required for $A = 9$ nuclei

Wavelet signatures of KK-splitting of the Isoscalar Giant Quadrupole Resonance in deformed nuclei from high-resolution (p,p′') scattering off 146,148,150^{146,148,150}Nd

The phenomenon of fine structure of the Isoscalar Giant Quadrupole Resonance (ISGQR) has been studied with high energy-resolution proton inelastic scattering at iThemba LABS in the chain of stable even-mass Nd isotopes covering the transition from spherical to deformed ground states. A wavelet analysis of the background-subtracted spectra in the deformed 146,148,150Nd isotopes reveals characteristic scales in correspondence with scales obtained from a Skyrme RPA calculation using the SVmas10 parameterization. A semblance analysis shows that these scales arise from the energy shift between the main fragments of the K = 0, 1 and K = 2 components.Comment: 7 pages, 6 figure

Binary projectile fragmentation of 12C at an incident energy of 33.3 MeV/nucleon

Direct binary projectile fragmentation is being investigated for the case where a 400 MeV 12C projectile breaks up into an particle and a 8Be fragment in the interaction with a thin 93Nb and 197Au target. While the 8Be fragments were measured at 9 , the correlated particles were detected in an angular range between 16 and 30 on the opposite side of the beam. From the preliminary results presented here one may obtain information on the amount of quasi-elastic fragmentation (both fragments do not suffer any further interactions after they are produced). These experimental results indicate that the quasi-elastic break-up process is the dominant contribution to the measured correlation spectra. As was also observed in earlier work, the most forward quasi-elastically emitted particles have energies exceeding the beam velocity