TY - JOUR
T1 - Theoretical prediction and experimental confirmation of unusual ternary ordered semiconductor compounds in Sr-Pb-S system
AU - Hao, Shiqiang
AU - Zhao, Li Dong
AU - Chen, Chang Qiang
AU - Dravid, Vinayak P.
AU - Kanatzidis, Mercouri G.
AU - Wolverton, Christopher M.
PY - 2014/1/29
Y1 - 2014/1/29
N2 - 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.
AB - 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.
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U2 - 10.1021/ja411857y
DO - 10.1021/ja411857y
M3 - Article
AN - SCOPUS:84893514172
VL - 136
SP - 1628
EP - 1635
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 4
ER -