Theoretical prediction and experimental confirmation of unusual ternary ordered semiconductor compounds in Sr-Pb-S system

Shiqiang Hao, Li Dong Zhao, Chang Qiang Chen, Vinayak P. Dravid, Mercouri G. Kanatzidis, Christopher M. Wolverton

Research output: Contribution to journalArticle

19 Citations (Scopus)


We examine the thermodynamics of phase separation and ordering in the ternary CaxPb1-xS and SrxPb1-xS 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: SrPb3S4, SrPbS2, and Sr3PbS4. 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.

Original languageEnglish
Pages (from-to)1628-1635
Number of pages8
JournalJournal of the American Chemical Society
Issue number4
Publication statusPublished - Jan 29 2014


ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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