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Exploration of cation ordering in ternary pnictides via electron microscopy

Mis, Allison V.
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2024-11-29
Abstract
Ternary nitrides and phosphides represent an exciting new space for materials discoveries. These materials, composed of two cations and an anion, are of interest for a wide variety of uses, including tandem PV, water-splitting, solid-state lighting, ferromagnetics, battery applications, and more. An important property of these materials is their potential for tunability with cation ordering, but measurement of the degree of ordering is challenging. Here, the characterization of both long- and short-range cation ordering is explored via electron microscopy, and the potential for these microscopy methods to be applied to high-throughput materials growth and characterization efforts is discussed. First, the novel nitride Zn2SbN2 is studied: high-throughput growth and characterization illuminate the growth space of this material, and microscopy helps establish a putative growth mechanism for these films. Next, the focus shifts to characterizing long-range ordering, in which the cations are placed in a repeated pattern on the cation sublattice, in single-crystal ZnSiP2. An electron-channeling-based approach is applied to measure long-range ordering, and the various challenges of sample preparation, data collection, and modeling relevant to applying this approach to novel materials are discussed. Finally, short-range ordering, a description of the 1st nearest neighbor bonding environment of the anions, is explored in ZnSnN(O) thin films. The bonding environments of N and O are investigated through Electron Energy Loss Spectrometry (EELS) analysis, and differences in short-range ordering are observed both among samples and spatially within each sample. These results are shown to be in moderate agreement with previous X-ray based measurements.
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