John S. Neal

Development of Novel Polycrystalline Ceramic Scintillators

For several decades most of the efforts to develop new scintillator materials have concentrated on high-light-yield inorganic single-crystals while polycrystalline ceramic scintillators, since their inception in the early 1980s, have received relatively little attention. Nevertheless, transparent ceramics offer a promising approach to the fabrication of relatively inexpensive scintillators via a simple mechanical compaction and annealing process that eliminates single-crystal growth. Until recently, commonly accepted concepts restricted the polycrystalline ceramic approach to materials exhibiting a cubic crystal structure. Here, we report our results on the development of two novel ceramic scintillators based on the non-cubic crystalline materials: Lu2SiO5:Ce (LSO:Ce) and LaBr3:Ce. While no evidence for texturing has been found in their ceramic microstructures, our LSO:Ce ceramics exhibit a surprisingly high level of transparency/translucency and very good scintillation characteristics. The LSO:Ce ceramic scintillation reaches a light yield level of about 86% of that of a good LSO:Ce single crystal, and its decay time is even faster than in single crystals. Research on LaBr:Ce shows that translucent ceramics of the high-light-yield rare-earth halides can also be synthesized. Our LaBr3:Ce ceramics have light yields above 42000 photons/MeV (i.e., >70%of the single-crystal light yield).

Evaluation of Melt-Grown, ZnO Single Crystals for Use as Alpha-Particle Detectors

As part of an ongoing investigation of the scintillation properties of zinc-oxide-(ZnO)-based scintillators, several melt-grown, ZnO single crystals have been characterized using alpha-particle excitation, infrared reflectance, and room temperature photoluminescence. The crystals, grown by Cermet, Inc., using an oxygen-pressurized melt-growth process, were doped with Group 1 elements (Li), Group 2 elements (Mg), Group 3 elements (Ga, In) and lanthanides (Gd, Er, Tm). The goals of these studies are to better understand the scintillation mechanisms associated with various members of the ZnO scintillator family and to then use this knowledge to improve the radiation detection capabilities of ZnO-based scintillators. One application for which ZnO is particularly well suited as a scintillator is as the associated particle detector in a deuterium-tritium (D-T) neutron generator. Application requirements include the exclusion of organic materials, outstanding timing resolution, and high radiation resistance. ZnO:Ga and ZnO:In have demonstrated fast (subnanosecond) decay times with relatively low light yields, and ZnO(Ga) has been used in a powder form as the associated particle detector for a D-T neutron generator. Four promising candidate materials, ZnO, ZnO:Ga, ZnO:In,Li, and ZnO:Er,Li, were identified in this study. These four samples demonstrated sub-nanosecond decay times and alpha-particle-excited- luminescence comparable to BC-400 fast plastic scintillator. The ZnO:Mg,Ga, ZnO:Gd, and ZnO:Li samples demonstrated appreciable slow (microsecond) decay components that would be incompatible with high-counting-rate applications.

Effects of phonon coupling and free carriers on band-edge emission at room temperature in n-type ZnO crystals

Room-temperature photoluminescence has been studied in n-type bulk ZnO crystals representing three different growth methods and having free-carrier concentrations (n) ranging from 1013to1018cm−3. The near-band-edge emission has both free-exciton and free-exciton-phonon contributions, with the strength of the phonon coupling dependent on sample defect concentrations. Band-gap shrinkage effects are used to explain a decrease in emission energy for the higher n values. Band filling and band nonparabolicity are predicted to be important for n>1019cm−3. At 300K, in the absence of free carriers, the free-exciton energy is 3.312±0.004eV.

NMIS plus gamma spectroscopy for attributes of HEU, PU and HE detection

Abstract A combined nuclear materials identification system–gamma ray spectrometry system can be used passively to obtain the following attributes of Pu: presence, fissile mass, 240/239 ratio and metal versus oxide. This system can also be used with a small, portable, DT neutron generator to measure the attributes of highly enriched uranium (HEU): presence, fissile mass, enrichment, metal versus oxide; and detect the presence of high explosives (HE). For the passive system, time-dependent coincidence distributions can be used for the presence, fissile mass, metal versus oxide for Pu, 240/239 ratio, and gamma ray spectrometry can also be used for 240/239 ratio and presence, allowing presence and 240/239 ratio to be confirmed by two methods. For the active system with a DT neutron generator, all relevant attributes for both Pu and HEU can be determined from various features of the time-dependent coincidence distribution measurements. Active gamma ray spectrometry would determine the presence of HE. The various features of time-dependent coincidence distributions and gamma ray spectrometry that determine these attributes are discussed with some examples from previous determinations.

Exploratory Research on the Development of Novel

We report the discovery of a new family of Ce3+-activated phosphate glass scintillators that can be formed either with or without the addition of 6Li, for neutron or X-ray/gamma-ray radiation detection, respectively. Trivalent cerium can be efficiently introduced into these phosphate glasses in surprisingly high concentrations in the form of anhydrous cerium tri-chloride. Additionally, these glasses can be melted and poured at the relatively low temperatures of 1000-1050degC (i.e., substantially lower than silicate glasses), and to retain the cerium in the trivalent state it is not necessary to maintain highly reducing conditions during the synthesis process. The family of alkaline-earth-alkali phosphate glasses investigated here represents a system with two dissimilar cations - thereby offering a large range of potential compositional variations, substitutions, and combinations. In order to alter the scintillator characteristics, we have explored part of that compositional space by studying Ca-Na, Ca-Li, Ca-Cs, Ca-Rb, Ca-K and Ca-Ba-Na phosphate glasses, as well as various co-doping and post-synthesis thermal processing schemes. A series of experiments under X-ray, gamma-ray, and neutron excitations was carried out. The broad, peaking at about 354 nm, UV scintillation of these glasses is well suited for applications that use common photomultipliers with bi-alkali photo-cathodes. Pulse shape measurements show that the primary component of the scintillation in most of these glasses corresponds to 75-90% of the emitted photons, and it decays with a time constant of 30 to 40 ns, which classifies these materials as reasonably fast scintillators. Although the gamma-induced light yield of these new scintillating phosphate glasses is, thus far, only about 30% of that of commercial GS20 silicate glass, due to the generally faster scintillation, the initial amplitude of the scintillation pulse of these glasses is close to that of the above-mentioned GS20 scintillator.

{\rm Ce}^{3+}

Bayesian inference techniques, coupled with Markov chain Monte Carlo sampling methods, are used to predict dose-time profiles for energetic solar particle events. Inputs into the predictive methodology are dose and dose-rate measurements obtained early in the event. Surrogate dose values are grouped in hierarchical models to express relationships among similar solar particle events. Models assume nonlinear, sigmoidal growth for dose throughout an event. Markov chain Monte Carlo methods are used to sample from Bayesian posterior predictive distributions for dose and dose rate. Example predictions are provided for the November 8, 2000, and August 12, 1989, solar particle events.

-Activated Phosphate Glass Scintillators

ZnO-based scintillators are particularly well suited for use as the associated particle detector in a deuterium-tritium (D-T) neutron generator. Application requirements include the exclusion of organic materials, outstanding timing resolution, and high radiation resistance. ZnO, ZnO:Ga, ZnO:In, ZnO:In,Li, and ZnO:Er,Li have demonstrated fast (sub-nanosecond) decay times with relatively low light yields. ZnO:Ga has been used in a powder form as the associated particle detector for a D-T neutron generator. Unfortunately, detectors using powders are difficult to assemble and the light yield from powders is less than satisfactory. Single-crystal ZnO of sufficient size has only recently become available. New applications for D-T neutron generators require better timing resolution and higher count rates than are currently available with associated particle detectors using YAP:Ce as the scintillator. Recent work suggests that ZnO-based scintillators can provide alpha-particle-excited light yields comparable to YAP:Ce scintillators. ZnO-based polycrystalline ceramic scintillators offer the advantages of high light yield, ease of fabrication, low cost, and robust mechanical properties. Precursor powders used in these studies include ZnO and ZnO:Ga powders synthesized using solution-phase, urea precipitation, and combustion synthesis techniques as well as ZnO powder from a commercial vendor. Precursor powders have been sintered using uniaxial hot pressing and spark plasma sintering techniques. Photoluminescence measurements have confirmed that, for most samples, the emissions from these sintered bodies consist primarily of slow, visible emissions rather than the desired sub-nanosecond near-band-edge emissions. Subsequent hydrogen treatments have shown significant improvements in the luminescence characteristics of some ceramic bodies, while other samples have shown no change in luminescence.

Predicting dose-time profiles of solar energetic particle events using Bayesian forecasting methods

A new scintillator material consisting of a methanol adduct of cerium trichloride with the composition CeCl3(CH3OH)4 has been discovered and crystallized in the form of large single crystals by solution growth in methanol. The peak emission of the x-ray-excited luminescence spectrum occurs at ∼364 nm. A light yield of up to ∼16 600 photons/MeV and an energy resolution of 11.4% were obtained using 662 keV gamma-ray photons. The scintillator decay time for 662 keV gamma-ray excitation was measured using the time-correlated, single-photon-counting method, and a nominal value of 64.4 ns was obtained. The molecular adduct CeCl3(CH3OH)4 represents the first example of a rare-earth, metal-organic scintillator that is applicable to gamma ray, x ray, and neutron detection.

Investigation of ZnO-Based Polycrystalline Ceramic Scintillators for Use as

We describe a neutron/gamma pulse shape discrimination (PSD) system that overcomes count rate limitations of previous methods for distinguishing neutrons from gammas in liquid scintillation detectors. Previous methods of PSD usually involve pulse shaping time constants that allow throughput of tens of thousands counts per second. Time correlated measurements require many millions of counts per second to accurately characterize nuclear material samples. To rapidly inspect many test articles, a high-throughput system is desired. To add neutron - gamma distinction to the analysis provides a much desired enhancement to the characterizations. However, if the PSD addition significantly slows down the inspection throughput, this PSD feature defeats any analysis advantage. Our goal for the fast PSD system is to provide sorted timing pulses to a fast, multi-channel, time-correlation processor at rates approaching several million counts per second enabling high throughput, enhanced inspection of nuclear materials.

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A new scintillator material for the detection of fast neutrons that consists of a methanol adduct of cerium trichloride with the composition CeCl₃(CH₃OH)₄ has been characterized using 14.1 MeV neutrons from a deuterium-tritium neutron generator and fast neutrons from a bare instrumented ²⁵²Cf source. The timing resolution of the scintillator for fast neutrons was found to be 1~ ns. Neutron interactions in the CeCl₃(CH₃OH)₄ composition were simulated using the MCNP-PoliMi code. These simulations indicate that proton recoils account for most of the deposited energy in CeCl₃(CH₃OH)₄. The crystalline molecular adduct CeCl₃(CH₃OH)₄ represents a rare-earth metal-organic scintillator that can be applied to both fast neutron and gamma-ray detection.