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Atomistic models for scintillator discovery

Doty, Fred P.; Yang, Pin Y.

A2BLnX6 elpasolites (A, B: alkali; Ln: lanthanide; X: halogen), LaBr3 lanthanum bromide, and AX alkali halides are three classes of the ionic compound crystals being explored for {gamma}-ray detection applications. Elpasolites are attractive because they can be optimized from combinations of four different elements. One design goal is to create cubic crystals that have isotropic optical properties and can be grown into large crystals at lower costs. Unfortunately, many elpasolites do not have cubic crystals and the experimental trial-and-error approach to find the cubic elpasolites has been prolonged and inefficient. LaBr3 is attractive due to its established good scintillation properties. The problem is that this brittle material is not only prone to fracture during services, but also difficult to grow into large crystals resulting in high production cost. Unfortunately, it is not always clear how to strengthen LaBr3 due to the lack of understanding of its fracture mechanisms. The problem with alkali halides is that their properties decay rapidly over time especially under harsh environment. Here we describe our recent progress on the development of atomistic models that may begin to enable the prediction of crystal structures and the study of fracture mechanisms of multi-element compounds.

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TYPE Conference YEAR 2010
OSTI

Cerium doped elpasolite halide scintillators

Doty, Fred P.; Zhou, Xiaowang Z.; Noda, Frank T.

Low-cost, high-performance gamma-ray spectrometers are urgently needed for proliferation detection and homeland security. The cost and availability of large scintillators used in the spectrometer generally hinge on their mechanical property and crystal symmetry. Low symmetry, intrinsically brittle crystals, such as these emerging lanthanide halide scintillators, are particularly difficult to grow in large sizes due to the development of large anisotropic thermomechanical stresses during solidification process. Isotropic cubic scintillators, such as alkali halides, while affordable and can be produced in large sizes, are poor spectrometers due to severe nonproportional response and modest light yield. This work investigates and compares four new elpasolite based lanthanide halides, including Cs2LiLaBr6, Cs2NaLaBr6, Cs2LiLaI6, and Cs2NaLaI6, in terms of their crystal symmetry, characteristics of photoluminescence and optical quantum efficiency. The mechanical property and thermal expansion behavior of the cubic Cs2LiLaBr6 will be reported. The isotropic nature of this material has potential for scaled-up crystal growth, as well as the possibility of low-cost polycrystalline ceramic processing. In addition, the proportional response with gamma-ray energy of directionally solidified Cs2LiLaBr6 will be compared with workhorse alkali halide scintillators. The processing challenges associated with hot forged polycrystalline elpasolite based lanthanide halides will also be discussed.

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TYPE Conference YEAR 2010
OSTI

Towards improved CZT crystals

Ward, Donald K.; Doty, Fred P.; Wong, Bryan M.; Zimmerman, Jonathan A.

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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TYPE Conference YEAR 2010
OSTI

Development of atomistic models to aid the design of new scintillator materials

Doty, Fred P.; Yang, Pin Y.

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.

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TYPE Conference YEAR 2010
OSTI
Results 51–75 of 95
Results 51–75 of 95