Publications

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The development of more reliable scintillator materials can significantly advance the gamma-ray detection technology. Scintillator materials such as lanthanum halides (e.g., LaBr{sub 3}, CsBr{sub 3}), elpasolites (e.g., Cs{sub 2}LiLaBr{sub 6}, Cs{sub 2}NaLaBr{sub 6}, and Cs{sub 2}LiLaI{sub 6}), and alkali halides (e.g., CsI, NaI) are extremely brittle. The fracture of the materials is often a problem causing the failure of the devices. Lanthanum halides typically have a hexagonal crystal structure. These materials have highly anisotropic thermal and mechanical properties, and therefore they are likely to fracture under cyclic thermal and mechanical loading conditions. For example, fracture of lanthanum halides is known to occur in the field. Fracture during synthesis also complicates the growth of large lanthanum halide single crystals needed for sensitive radiation detection, and accounts for the high production cost of these materials. Elpasolites can have both cubic and non-cubic crystal structures depending on the constituent elements and composition of the compounds. This provides an opportunity to design cubic elpasolites with more isotropic properties and therefore improved mechanical performances. However, the design of an optimized cubic elpasolite crystal remains elusive because there is a tremendous number of possible elpasolites and the design criterion for cubic crystals is not clear. Alkali halides have cubic crystal structures. Consequently, large CsI and NaI crystals have been grown and used in devices. However, these materials suffer from an aging problem, i.e., the properties decay rapidly over time especially under harsh environment. Unfortunately, the fundamental mechanisms of this aging have not been understood and the path to improve the alkali halide-based scintillators is not developed. Clearly, improved scintillator materials can be achieved via strengthened/toughened lanthanum halides, optimized cubic elpasolites, or new alkali halide-based crystals that are more resistant to aging. Without a fundamental understanding of the atomic origins of the mechanical and the thermodynamic properties of materials, past experimental efforts to develop improved scintillator materials have been prolonged. Here we report our recent progress on the development of atomistic models that can be used to accelerate the discovery of new scintillator materials with improved properties. First, we have developed a novel embedded-ion method interatomic potential approach that analytically addresses the variable charge interactions between atoms in ionic compound material systems. Based on this potential, molecular dynamics simulations have been used to study the mechanical properties of LaBr3 including slip systems, dislocation core structures, and material strength. We have also developed an atomistic model that can already be used to predict crystal structures and to derive crystal stability rules for alkali halides. This model is under further development for prediction of crystal structures of elpasolites. These efforts will facilitate the design of better scintillator materials.

Past experimental efforts to improve CZT crystals for gamma spectrometer applications have been focused on reducing micron-scale defects such as tellurium inclusions and precipitates. While these micron-scale defects are important, experiments have shown that the micron-scale variations in transport can be caused by the formation and aggregation of atomic-scale defects such as dislocations and point defect clusters. Moreover, dislocation cells have been found to act as nucleation sites that cause the formation of large precipitates. To better solve the uniformity problem of CZT, atomic-scale defects must be understood and controlled. To this end, we have begun to develop an atomistic model that can be used to reveal the effects of small-scale defects and to guide experiments for reducing both atomic- and micron-scale (tellurium inclusions and precipitates) defects. Our model will be based upon a bond order potential (BOP) to enable large-scale molecular dynamics simulations of material structures at a high-fidelity level that was not possible with alternative methods. To establish how BOP improves over existing approaches, we report here our recent work on the assessment of two representative literature CdTe interatomic potentials that are currently widely used: the Stillinger-Weber (SW) potential and the Tersoff-Rockett (TR) potential. Careful examinations of phases, defects, and surfaces of the CdTe system were performed. We began our study by using both potentials to evaluate the lattice constants and cohesive energies of various Cd, Te, and CdTe phases including dimer, trimer, chain, square, rhomboid, tetrahedron, diamond-cubic (dc), simple-cubic (sc), body-centered-cubic (bcc), face-centered cubic (fcc), hexagonal-close-packed (hcp), graphite-sheet, A8, zinc-blende (zb), wurtzite (wz), NaCl, CsCl, etc. We then compared the results with our calculations using the density functional theory (DFT) quantum mechanical method. We also evaluated the suitability of the two potentials to predict the surface reconstructions and surface energies, various defect configurations and defect energies (interstitials and voids), elastic constants, and melting temperatures of different phases. We found that both potentials predicted incorrect energy trends as compared with those predicted by the DFT method. Most seriously, both potentials predicted incorrect lowest energy phases. These studies clearly showed that the existing potentials are not sufficient for correctly predicting the charge transport properties of CdTe demonstrating the need for a new potential. We anticipate that our BOP method will overcome this problem and will accelerate the discovery of a synthesis approach to produce improved CZT crystals.

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This work demonstrated the feasibility and limitations of semiconducting {pi}-conjugated organic polymers for fast neutron detection via n-p elastic scattering. Charge collection in conjugated polymers in the family of substituted poly(p-phenylene vinylene)s (PPV) was evaluated using band-edge laser and proton beam ionization. These semiconducting materials can have high H/C ratio, wide bandgap, high resistivity and high dielectric strength, allowing high field operation with low leakage current and capacitance noise. The materials can also be solution cast, allowing possible low-cost radiation detector fabrication and scale-up. However, improvements in charge collection efficiency are necessary in order to achieve single particle detection with a reasonable sensitivity. The work examined processing variables, additives and environmental effects. Proton beam exposure was used to verify particle sensitivity and radiation hardness to a total exposure of approximately 1 MRAD. Conductivity exhibited sensitivity to temperature and humidity. The effects of molecular ordering were investigated in stretched films, and FTIR was used to quantify the order in films using the Hermans orientation function. The photoconductive response approximately doubled for stretch-aligned films with the stretch direction parallel to the electric field direction, when compared to as-cast films. The response was decreased when the stretch direction was orthogonal to the electric field. Stretch-aligned films also exhibited a significant sensitivity to the polarization of the laser excitation, whereas drop-cast films showed none, indicating improved mobility along the backbone, but poor {pi}-overlap in the orthogonal direction. Drop-cast composites of PPV with substituted fullerenes showed approximately a two order of magnitude increase in photoresponse, nearly independent of nanoparticle concentration. Interestingly, stretch-aligned composite films showed a substantial decrease in photoresponse with increasing stretch ratio. Other additives examined, including small molecules and cosolvents, did not cause any significant increase in photoresponse. Finally, we discovered an inverse-geometric particle track effect wherein increased track lengths created by tilting the detector off normal incidence resulted in decreased signal collection. This is interpreted as a trap-filling effect, leading to increased carrier mobility along the particle track direction. Estimated collection efficiency along the track direction was near 20 electrons/micron of track length, sufficient for particle counting in 50 micron thick films.

Strengthening the crystal lattice of lanthanide halides, which are brittle, anisotropic, ionic crystals, may prove to increase the availability and ruggedness of these scintillators for room-temperature gamma-ray spectroscopy applications. Eight aliovalent dopants for CeBr{sub 3} were explored in an effort to find the optimal aliovalent strengthening agent. Eight dopants, CaBr{sub 2}, SrBr{sub 2}, BaBr{sub 2}, ZrBr{sub 4}, HfBr{sub 4}, ZnBr{sub 2}, CdBr[sub 2}, and PbBr{sub 2}, were explored at two levels of doping, 500 and 1000 ppm. From each ingot, samples were harvested for radioluminescence spectrum measurement and scintillation testing. Of the eight dopants explored, only BaBr{sub 2} and PbBr{sub 2} were found to clearly decrease total light yield. ZnBr{sub 2} and CdBr{sub 2} dopants both affected the radioluminescence emission spectrum very little as compared to undoped CeBr{sub 3}. HfBr{sub 2}- and ZnBr{sub 4}-doped CeBr{sub 3} exhibited the highest light yields.

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