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• W2260759114 abstract "The use of pyrite FeS2 as an earth-abundant, low-cost, nontoxic thin film photovoltaic hinges on improved understanding and control of certain physical and chemical properties. Phase stability, phase purity, stoichiometry, and defects, are central in this respect, as they are frequently implicated in poor solar cell performance. Here, phase-pure polycrystalline pyrite FeS2 films, synthesized by ex situ sulfidation, are subject to systematic reduction by vacuum annealing (to 550 °C) to assess phase stability, stoichiometry evolution, and their impact on transport. Bulk probes reveal the onset of pyrrhotite (Fe1−δS) around 400 °C, rapidly evolving into the majority phase by 425 °C. This is supported by X-ray photoelectron spectroscopy on (001) crystals, revealing surface Fe1−δS formation as low as 160 °C, with rapid growth near 400 °C. The impact on transport is dramatic, with Fe1−δS minority phases leading to a crossover from diffusive transport to hopping (due to conductive Fe1−δS nanoregions in an FeS2 matrix), followed by metallicity when Fe1−δS dominates. Notably, the crossover to hopping leads to an inversion of the sign, and a large decrease in magnitude of the Hall coefficient. By tracking resistivity, magnetotransport, magnetization, and structural/chemical parameters vs annealing, we provide a detailed picture of the evolution in properties with stoichiometry. A strong propensity for S-deficient minority phase formation is found, with no wide window where S vacancies control the FeS2 carrier density. These findings have important implications for FeS2 solar cell development, emphasizing the need for (a) nanoscale chemical homogeneity, and (b) caution in interpreting carrier types and densities." @default.
• W2260759114 created "2016-06-24" @default.
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• W2260759114 date "2015-06-18" @default.
• W2260759114 modified "2023-10-01" @default.
• W2260759114 title "Phase Stability and Stoichiometry in Thin Film Iron Pyrite: Impact on Electronic Transport Properties" @default.
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• W2260759114 doi "https://doi.org/10.1021/acsami.5b03422" @default.
• W2260759114 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/26087015" @default.
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