Beyond Californium-A Neutron Generator Alternative for Dosimetry and Instrument Calibration in the U.S.

Evaluations of neutron survey instruments, area monitors, and personal dosimeters rely on reference neutron radiations, which have evolved from the heavy reliance on (α,n) sources to a shared reliance on (α,n) and the spontaneous fission neutrons of californium-252 (Cf). Capable of producing high dose equivalent rates from an almost point source geometry, the characteristics of Cf are generally more favorable when compared to the use of (α,n) and (γ,n) sources or reactor-produced reference neutron radiations. Californium-252 is typically used in two standardized configurations: unmoderated, to yield a fission energy spectrum; or with the capsule placed within a heavy-water moderating sphere to produce a softened spectrum that is generally considered more appropriate for evaluating devices used in nuclear power plant work environments. The U.S. Department of Energy Cf Loan/Lease Program, a longtime origin of affordable Cf sources for research, testing and calibration, was terminated in 2009. Since then, high-activity sources have become increasingly cost-prohibitive for laboratories that formerly benefited from that program. Neutron generators, based on the D-T and D-D fusion reactions, have become economically competitive with Cf and are recognized internationally as important calibration and test standards. Researchers from the National Institute of Standards and Technology and the Pacific Northwest National Laboratory are jointly considering the practicality and technical challenges of implementing neutron generators as calibration standards in the U.S. This article reviews the characteristics of isotope-based neutron sources, possible isotope alternatives to Cf, and the rationale behind the increasing favor of electronically generated neutron options. The evaluation of a D-T system at PNNL has revealed characteristics that must be considered in adapting generators to the task of calibration and testing where accurate determination of a dosimetric quantity is necessary. Finally, concepts are presented for modifying the generated neutron spectra to achieve particular targeted spectra, simulating Cf or workplace environments.

Neutron metrology laboratory facility simulation.

The Neutron Low Scattering Laboratory in Brazil has been completely rebuilt. Evaluation of air attenuation parameters and neutron component scattering in the room was done using Monte Carlo simulation code. Neutron fields produced by referenced neutron source were used to calculate neutron scattering and air attenuation.

The analysis of complex mixed-radiation fields using near real-time imaging.

A new mixed-field imaging system has been constructed at Lancaster University using the principles of collimation and back projection to passively locate and assess sources of neutron and gamma-ray radiation. The system was set up at the University of Manchester where three radiation sources: (252)Cf, a lead-shielded (241)Am/Be and a (22)Na source were imaged. Real-time discrimination was used to find the respective components of the neutron and gamma-ray fields detected by a single EJ-301 liquid scintillator, allowing separate images of neutron and gamma-ray emitters to be formed. (252)Cf and (22)Na were successfully observed and located in the gamma-ray image; however, the (241)Am/Be was not seen owing to surrounding lead shielding. The (252)Cf and (241)Am/Be neutron sources were seen clearly in the neutron image, demonstrating the advantage of this mixed-field technique over a gamma-ray-only image where the (241)Am/Be source would have gone undetected.

Unusual structure, bonding and properties in a californium borate.

The participation of the valence orbitals of actinides in bonding has been debated for decades. Recent experimental and computational investigations demonstrated the involvement of 6p, 6d and/or 5f orbitals in bonding. However, structural and spectroscopic data, as well as theory, indicate a decrease in covalency across the actinide series, and the evidence points to highly ionic, lanthanide-like bonding for late actinides. Here we show that chemical differentiation between californium and lanthanides can be achieved by using ligands that are both highly polarizable and substantially rearrange on complexation. A ligand that suits both of these desired properties is polyborate. We demonstrate that the 5f, 6d and 7p orbitals are all involved in bonding in a Cf(III) borate, and that large crystal-field effects are present. Synthetic, structural and spectroscopic data are complemented by quantum mechanical calculations to support these observations.

TEPC performance for a reference standard.

A portable tissue-equivalent proportional counter (TEPC)-based system was developed, which will be used as a reference standard in the neutron mixed field for radiation protection. In this paper, microdosimetry of the TEPC system was studied both in neutron ((252)Cf and (241)Am-Be sources) and gamma ((137)Cs and (60)Co sources) reference radiation fields. The measured neutron and gamma-dose equivalent rates were, respectively, compared with those of the reference ambient dose equivalent rate H(*)(10). And the measured microdosimetric spectra were compared with the Monte Carlo code FLUKA simulated results. All of the comparisons primarily agreed well.

Evaluation of H*(10) using the developed spherical type neutron dose monitor.

An instrument for evaluating the neutron ambient dose equivalent has been developed. It has the characteristic of uniform response to wide energy of neutrons. The monitor is four-layered spherically shaped, based on moderation and absorption of neutrons. Neutron dose can be evaluated from the linear combination of three specific responses of thermoluminescent dosimeters (TLDs), which are located at three depths in the moderator. TLDs were arranged between layers of two consecutive depths on 12 radial axes at even intervals so that the monitor is equally sensitive to all directions of neutrons. In order to verify the usefulness of dose evaluation by the monitor, irradiation experiments were conducted at the FRS, JAEA. The D2O-moderated 252Cf was used for the calibration of the monitor. Experiments were also conducted by using two neutron sources of 252Cf bare and 241Am-Be. As a result, the evaluated dose for each irradiation was obtained close to the actual irradiated dose. It was confirmed that the method of dose evaluation by the developed monitor can be applied to practical neutron fields where the distance of neutron source is unknown.

On the effect of an error in a standard D2O-moderated 252Cf energy spectrum.

There appears to be an error in the neutron fluence for neutrons with energies between 9 and 10 MeV for the tabulated D2O-moderated Cf source in ISO 8529-1. If the referenced spectrum is used as tabulated, the error contributes a total error to neutron dose values from this source of approximately 3%.

Evaluation of the characteristics of the neutron reference field using D2O-moderated 252Cf source.

The ambient/personal dose equivalent per fluence for D(2)O moderated (252)Cf neutron source was determined by measurement. An appropriate subtraction of the scattered neutrons is required for the accurate measurement of direct neutrons. A cubic shadow object was used for the subtraction of the scattered neutrons from the surroundings. The scattered neutrons to be subtracted vary with the position of the shadow object due to the large volume of the source. Using the Monte Carlo code MCNP-4C, the optimum positions of the shadow object were surveyed for subtracting the scattered neutrons. The energy spectra of direct neutrons were measured in the optimum position. The dosimetric parameters for the D(2)O moderated (252)Cf neutron source were reasonable, taking into account the uncertainties of the parameters.

Fast neutron spectrometry and dosimetry using a spherical moderator with position-sensitive detectors.

A neutron spectrometry and dosimetry measurement system has been developed based on a different design of the divided regions for a sphere, with three position-sensitive counters. The characteristics of the measurement system have been investigated in the reference radiation fields of Am-Be and (252)Cf sources. When realistic input spectra are used for the unfolding, the overall deviations of the calculated results for four dosimetric quantities are less than +/-10%. The results of other input spectra are also discussed in this report.

Development of a thermal neutron sensor for Humanitarian Demining.

A thermal neutron sensor prototype for Humanitarian Demining has been developed, trying to minimize cost and complexity of the system as required in such application. A (252)Cf source or a sealed-tube neutron generator is employed to produce primary fast neutrons that are thermalized in a moderator designed to optimize the neutron capture reaction yield in buried samples. A description of the sensor, including the performances of the acquisition system based on a Flash ADC card and final tests with explosive simulants are reported. A comparison of the sensor performance when using a radioactive source to that when employing a sealed-tube neutron generator is presented. Limitations and possible applications of this technique are discussed.

Shielding design studies for a neutron irradiator system based on a 252Cf source.

This study aims to investigate a shielding design against neutrons and gamma rays from a source of 252Cf, using Monte Carlo simulation. The shielding materials studied were borated polyethylene, borated-lead polyethylene and stainless steel. The Monte Carlo code MCNP4B was used to design shielding for 252Cf based neutron irradiator systems. By normalising the dose equivalent rate values presented to the neutron production rate of the source, the resulting calculations are independent of the intensity of the actual 252Cf source. The results show that the total dose equivalent rates were reduced significantly by the shielding system optimisation.

Enhancement of a 252Cf-based neutron beam via subcritical multiplication for neutron capture therapy.

Previous studies indicated that an epithermal-neutron beam based on bare 252Cf is not feasible for neutron capture therapy (NCT). It was reported that a clinically useful epithermal-neutron beam requires a minimum of 1.0 g of 252Cf, which is more than twice the US current annual supply. However, it was reasoned that the required quantity of 252Cf could be dramatically reduced when used with a subcritical multiplying assembly (SMA). This reasoning is based on the assumption that the epithermal-neutron beam intensity for NCT is directly proportional to the fission neutron population, and that the neutron multiplying factor of the SMA can be estimated by 1/(1 - k(eff)). We have performed detailed Monte Carlo calculations to investigate the validity of the above reasoning. Our results show that 1/(1 - k(eff)) grossly overestimates the beam enhancement factor for NCT. For example, Monte Carlo calculations predict a beam enhancement factor of 6.0 for an optimized SMA geometry with k(eff) = 0.968. This factor is much less than 31 predicted by 1/(1 - k(eff)). The overestimation is due to the fact that most of the neutrons produced in the SMA are self-shielded, whereas self-shielding is negligible in a bare 252Cf source. Since the beam intensity of a 0.1 g 252Cf with the optimized SMA enhancement is still more than an order of magnitude too low compared to the existing reactor beams, we conclude that the enhancement via an SMA for a 252Cf-based epithermal-neutron beam is inadequate for NCT.

Development of high-activity 252Cf sources for neutron brachytherapy.

The Gershenson Radiation Oncology Center of Wayne State University (WSU), Detroit, Michigan, is using 252Cf medical sources for neutron brachytherapy. These sources are based on a 20-year-old design containing < or = 30 micrograms 252Cf in the form of a cermet wire of Cf2O3 in a palladium matrix. The Radiochemical Engineering Development Center (REDC) of Oak Ridge National Laboratory has been asked to develop very compact, high-activity 252Cf neutron sources for use with remote afterloading equipment in order to reduce treatment times and dose to clinical personnel and to expedite treatment of brain and other tumors. To date, the REDC has demonstrated that 252Cf loadings can be greatly increased in cermet wires and with much smaller diameters. Equipment designed for hot cell fabrication of these wires is being tested. A parallel program is under way to relicense the existing source design for fabrication at the REDC.

Distinct difference in relative biological effectiveness of 252Cf neutrons for the induction of mitotic crossing over and intragenic reversion of the white-ivory allele in Drosophila melanogaster.

The relative biological effectiveness (RBE) of 252Cf neutrons was determined for two different types of somatic mutations, i.e., loss heterozygosity for wing-hair mutations and reversion of the mutant white-ivory eye-color, in Drosophila melanogaster. Loss of heterozygosity for wing-hair mutations results predominantly from mitotic crossing over induced in wing anlage cells of larvae, while the reverse mutation of eye color is due to an intragenic structural change in the white locus on the X-chromosome. For a quantitative comparison of RBE values for these events, we have constructed a combined mutation assay system so that induced mutant wing-hair clones as well as revertant eye-color clones can be detected simultaneously in the same individuals. Larvae were irradiated at the age of 80 +/- 4 h post-oviposition with 252Cf neutrons or 137Cs gamma-rays, and male adult flies were examined under the microscope for the presence of the two types of clonal mosaic spots appearing. The induction of wing-hair spots per dose unit was much greater for 252Cf neutrons than for 137Cs gamma-rays, whereas the frequencies of eye-color reversion were similar for neutrons and gamma-rays. The estimated RBE values of neutrons were 8.5 and 1.2 for the induction of mutant wing-hair spots and revertant eye-color spots, respectively. These results indicate that the RBE of neutrons is much greater for mitotic crossing over in comparison to the intragenic white-ivory reversion events. Possible causes for the difference in RBE are discussed.

252Cf-plasma desorption mass spectrometry analysis of lipids A obtained by an elimination reaction under mild conditions.

Lipids A are the hydrophobic domains of bacterial endotoxic lipopolysaccharides. Since they are responsible for most of the biological activities (both pathogenic and beneficial) of endotoxins, the characterization of their structure is crucial to the understanding of their mode of action. However, the inadequacy of existing methods for preparing certain lipids A has prompted us to devise a new, mild procedure which gives intact products. Use was made of the special features of 252Cf-plasma desorption mass spectrometry for forming molecular ions from these species and giving qualitative and quantitative information from the primary mass spectrum.

[Use of time-of-flight mass spectrometry with ionization division fragments of californium-252 for studying the mechanisms of action of drugs on DNA and its components]. / Primenenie vremia proletnoi mass-spektrometrii s ionizatsiei oskolkami deleniia kaliforniia-252 k izucheniiu mekhanizmov deistviia lekarstvennykh preparatov na DNK i ee komponenty.

Using soft-ionization mass spectrometry (252-Cf particle desorption mass spectrometry, PDMS) a minor adduct of anticancer drug prospidine and deoxyguanosine-5-phosphate (pdG) has been found. It has been shown experimentally that PDMS is very useful for study of biological mixtures as well as mechanisms of interactions between drugs and biomolecules.

Clinical evaluation of 252Cf neutron intracavitary therapy for primary endometrial adenocarcinoma.

BACKGROUND: A pilot feasibility study of the neutron-emitting radioisotope 252Cf was done on patients with uterine adenocarcinoma and medically inoperable disease or unfavorable G3 histologic findings. METHODS: 252Cf intracavitary therapy was combined with 40-45 Gy of fractionated whole-pelvis photon therapy. In select patients, hysterectomy was performed. RESULTS: Thirty-one patients with Stage I-III adenocarcinoma of the corpus uteri were treated with 252Cf neutron brachytherapy. The patients treated often were in poor general medical condition and had multiple chronic medical illnesses for which conventional radiation and surgery usually would not be recommended. 252Cf allowed short implant treatment time (hours), was usable in a small number of insertions (the average number of insertions was two), and was useful for treating large volume tumors. Stage and grade of the tumor were important determinants of patient survival. The 5-year actuarial survival was 83% for patients with Stage I disease but only 37% for those with Stage II disease (primarily adenosquamous cell carcinomas). The 5-year survival was 100% for patients with Grade 1 tumors, 88% for those with Grade 2 tumors, and 21% for those with Grade 3 tumors. CONCLUSION: 252Cf neutron brachytherapy was found to be an effective and well-tolerated therapy for endometrial carcinoma. The excellent therapeutic efficacy and good patient tolerance make it suitable for additional evaluation in future Phase II-III trials.