A new generation of medical grade Cf-252 sources was developed in 2002 at the Oak Ridge National Laboratory (ORNL). The combination of small size and large activity of these Cf-252 sources makes them suitable to be used with the conventional high-dose-rate (HDR) remote afterloading systems for interstitial brachytherapy. A recent in-water calibration experiment showed that the measured gamma dose rates near the new source are slightly greater than the neutron dose rates; contradicting the well established neutron-to-gamma dose ratio of approximately 2:1 at locations near a Cf-252 brachytherapy source. Specifically, the MCNP-predicted gamma dose rate is a factor of two higher than the measured gamma dose rate at the distance of 1 cm, and the differences between the two results gradually diminish at distances farther away from the source. To resolve this discrepancy, we updated the source gamma spectrum by including in the ORIGEN-S data library the experimentally measured Cf-252 prompt gamma spectrum as well as the true Cf-252 spontaneous fission yield data to explicitly model delayed gamma emissions from fission products. We also investigated the bremsstrahlung x-rays produced by the beta particles emitted from fission-product decays. The results show that the discrepancy of gamma dose rates is mainly caused by the omission of the bremsstrahlung x-rays in the MCNP runs. By including the bremsstrahlung x-rays, the MCNP results show that the gamma dose rates near a new Cf-252 source agree well with the measured results and that the gamma dose rates are indeed greater than the neutron dose rates. The calibration experiment also showed discrepancies between the experimental and computational neutron dose profiles obtained. Specifically the MCNP-predicted neutron dose rates were ~25% higher than the measured neutron dose rates at all distances. In attempting to resolve this discrepancy the neutron emission rate was verified by the National Institute of Standards and Technology (NIST) and an experiment was performed to explore the effects of bias voltage on ion chamber charge collection. So far the discrepancies between the computational and experimental neutron dose profiles have not been resolved. Further study is needed to completely resolve this issue and some suggestions on how to move forward are given.

Galveston Bay is the second largest estuary in the Gulf of Mexico. The bay’s watershed and shoreline contains one of the largest concentrations of petroleum and chemical industries in the world, with the greatest concentration within the lower 15 km of the San Jacinto River/Houston Ship Channel (SJR/HSC). Extensive groundwater has been withdrawn to support these industries and an expanding population has resulted elevated land subsidence, with the highest land subsidence in the lower SJR/HSC, of over 3 m (3 cm yr^-1) and has decreased seaward throughout the bay to 0.6 cm yr^-1 near Galveston Island. Mercury (Hg) contamination is well documented throughout the bay’s sediments. Sediment vibra-cores were collected throughout the bay systems. 210Pb and 137Cs geochronologies from these cores was used to determine sedimentation rates and correlated to Hg profiles to estimate input histories. Relative Sea Level Rise (RSLR) is the sum of eustatic sea level rise and land subsidence. The results show sedimentation rates are high in areas with high rates of RSLR and the rates are of the same order of magnitude, however, in general, sedimentation rates are as much as 50% of RSLR, indicating that sedimentation has not kept pace with land subsidence, although they have the same relative order. Hg core profiles were correlated with radioisotope geochronologies and show significant input of Hg beginning around 1940, with a peak around 1971, and a dramatic drop off in concentration afterwards, demonstrating it to be a valuable geochronology tool. Hg concentrations were found to be dramatically higher proximal to the SJR/HSC and progressively decreasing seaward and to distal parts of the bay.

Introduction The embrace of PET by medical clinicians has been reluctant (ΔT ≈ 20 yr) primarily due to the scale of the infrastructure that is needed. The capital cost of a cyclotron (≈ 106 USD) is now dwarfed by the demand for compliance to recent regulatory standards. This is a recurring expense, not only imposing an order-of-magnitude increase in staffing and operating costs, but damping the enthusiasm of researchers recalling the brisk pace of research in earlier days. Now an academic site, with little interest or opportunity to scale up production for wider distribution, is burdened by the new regulatory terrain of good manufacturing practice (GMP), mandated for translational studies that will reach only a few subjects. With our production resources held within a basic science department, the Medical Physics cyclotron facility at the University of Wisconsin has sought a sustainable pathway. We now anchor the operating budget by providing high-value, long-lived radionuclides to off-site users, to buffer the fluctuations of local demand for conventional PET synthons. Material and Methods: The tools of the trade The radioisotopes discussed here belong to the 3-d and 4-d sub shell, but are now moving into the rare-earths, with applications ranging from - targeted molecular imaging agents, - internal radionuclide therapy using to Auger electron-emitters, - to basic physics experiments using 163Ho (t1/2 ≈ 4500 yr) to determine the mass of the neutrino. Rather than focusing on the dozens of radionuclides produced, a number of tools deserve mention, as they support a variety of targets, reactions and products. These will be listed in order (A-G) from cyclotron to extraction to analysis. A. Two cyclotrons are used, a legacy RDS 112 (#1; 1985) and a GE PETtrace (2009). Neutron and gamma detectors are monitored during the long irradia-tions, signaling any subtle changes in the running conditions. (1). The PET-trace is fitted with a quick-change variable degrader target (2), as well as a beam-line with a 5-port (0 o, ±15 o, ±30 o) vertical switching magnet (3). The downward directed beam ports provide support for solid targets (e.g. Ga, S, Se, Te) that melt at low temperature. The irradiation of gas targets employs a generalized manifold to handle inert gases such as 36Ar for the production of 34mCl, as well as natural Kr and Xe for making Rb and Cs isotopes to act as fission product surrogates. These products are captured on a stainless steel target chamber liner, and rinsed off with warm water. The alkali metals are convenient tracers to study the ion exchange trapping process, pivotal in future 99Mo production from solution reactors (4). B. The preparation of malleable solid targets employs a 10-ton hydraulic bench press, and a jeweler’s mill to roll out foils from pellets, pressed between Nb foils to avoid contamination. C. Binary alloys are smelted in a programmable 1600o tube furnace under argon flow (eg. NiGa4). Alternatively, an induction furnace now permits highly localized heating of the binary metal charge, while allowing mechanical agitation during the smelting process. D. Electroplating onto gold discs is used for various enriched target material or the alloys above where quantitative recovery is essential, or where heat transfer from high beam current is demanding. E. The separation chemistry, prior to che-lation to targeted molecular imaging agents, is performed in LabView-driven, home-built “black boxes” resident in mini-cells (Radiation Shielding Inc.). F. Analysis of the targets after irradiation makes use of HPGe spectroscopy for gammas and characteristic X-rays of decay (e.g. rare earths). The elemental constitution of target alloys is deter-mined prior to irradiation by X-ray fluorescence analysis, excited by 109Cd and 241Am sources. G. Finally, broad-band elemental analysis at the ppb level now makes use of a microwave plasma atomic emission spectrometer (Agilent 4200), to be de-scribed elsewhere in this meeting. Results and Conclusions The tools above (A-G) are employed in the pro-duction of the expanded list of radionuclides offered by our cyclotron group to both local and off-site colleagues. The list below is ordered in terms of decreasing use, from regular production for national distribution (64Cu, 89Zr), to weekly inhouse use (44Sc, 66,68Ga, 68,69,71Ge, 72As, 61Cu, 86Y), to infrequent production for multi-site collaborations (163Ho, 95mTc, 206Bi): Radionuclide Target Employs 64Cu 64Ni/Au A, D, G 89Zr natY A, E, G 44Sc natCa A, B, E, F, G 66, 68Ga Zn/Ag A, B, D, E, F, G 68, 69, 71Ge Ga, GaO2 A, B, C, E,F 72As GeO2 A, B, E, F 52Mn natCr A, E, F, G 76, 81mBr SeO A, E, F 34mCl, Rb, Cs noble gas A, E, F 95mTc,163Ho Mo, Dy A, E, F TABLE 1. Target materials and processes. The production of long-lived radionuclides lends itself to crowd-sourcing, with distributed irradia-tion at virtually any site with a suitable accelera-tor and a relaxed beam schedule. A number of unique challenges do arise that don’t appear in the usual production of conventional cyclotron products such as 11C or 18F. Contamination by stable metals, inadvertently introduced by target pressing or beam-induced sputtering from degraders, can cause serious interference downstream limiting effective specific activity. Long-lived manganese isotopes are ubiquitous. And some very high value products are simply not within the reach of small cyclotrons, such as 52Fe and 67Cu, being too far off the line of beta stability. In conclusion, the research leading to a doctoral degree necessarily must focus on the physics and chemistry of novel radionuclides and tracers. On the other hand, clinical and translational research needs established imaging agents, with little room for innovation within the regulatory constraints. Our experience at Wisconsin has led us to a balancing act, with our routine production of clinical doses countered with our research program to provide high-value radionu-clides for our collaborative work with our basic science colleagues.

Thesis (doctoral)--University of Göteborg, 1998. / Added t.p. with thesis statement inserted.

Thesis (doctoral)--University of Göteborg, 1997. / Added t.p. with thesis statement inserted.

Thesis (doctoral)--University of Göteborg, 1998. / Added t.p. with thesis statement inserted.

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