Theoretical Prediction and Experimental Confirmation of Unusual Ternary Ordered Semiconductor Compounds in Sr-Pb-S System.

We examine the thermodynamics of phase separation and ordering in the ternary CaPbS and SrPbS systems by density-functional theory combined with a cluster expansion and Monte Carlo simulations. Similar to most other ternary III-V or IV-VI semiconductor alloys, we find that bulk phase separation is t...

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Publicado en:Journal of the American Chemical Society Vol. 136; no. 4; pp. 1628 - 1636
Autores principales: Shiqiang Hao, Li-Dong Zhao, Chang-Qiang Chen, Dravid, Vinayak P., Kanatzidis, Mercouri G., Wolverton, Christopher M.
Formato: Artículo
Publicado: American Chemical Society 1/29/2014
Materias:
Acceso en línea:Ver este registro en EBSCOhost
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        10.1021/ja411857y
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        atl: Theoretical Prediction and Experimental Confirmation of Unusual Ternary Ordered Semiconductor Compounds in Sr-Pb-S System.
      aug:
        au:
          Shiqiang Hao
          Li-Dong Zhao
          Chang-Qiang Chen
          Dravid, Vinayak P.
          Kanatzidis, Mercouri G.
          Wolverton, Christopher M.
        affil:
          Department of Materials Science & Engineering, Evanston, Illinois 60208, United States
          Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
      su:
        Ternary semiconductors
        Thermodynamics
        Monte Carlo method
        Phase separation
        Transmission electron microscopy
        Chalcogenides
        Density functional theory
        Band gaps
      sug:
        subj:
          Ternary semiconductors
          Thermodynamics
          Monte Carlo method
          Phase separation
          Transmission electron microscopy
          Chalcogenides
          Density functional theory
          Band gaps
      ab: We examine the thermodynamics of phase separation and ordering in the ternary CaPbS and SrPbS systems by density-functional theory combined with a cluster expansion and Monte Carlo simulations. Similar to most other ternary III-V or IV-VI semiconductor alloys, we find that bulk phase separation is thermodynamically preferred for PbS-CaS. However, we predict the surprising existence of stable, ordered ternary compounds in the PbS-SrS system. These phases are previously unreported ordered rocksalt-based compounds: SrPbS, SrPbS, and SrPbS. The stability of these predicted ordered phases is confirmed by transmission electron microscopy observations and band gap measurements. We believe this work paves the way for a combined theory-experiment approach to decipher complex phase relations in multicomponent chalcogenide systems.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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