Abstract
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 language | English |
|---|---|
| Pages (from-to) | 1628-1635 |
| Number of pages | 8 |
| Journal | Journal of the American Chemical Society |
| Volume | 136 |
| Issue number | 4 |
| DOIs | |
| Publication status | Published - Jan 29 2014 |
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ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
- Biochemistry
- Colloid and Surface Chemistry
Cite this
Theoretical prediction and experimental confirmation of unusual ternary ordered semiconductor compounds in Sr-Pb-S system. / Hao, Shiqiang; Zhao, Li Dong; Chen, Chang Qiang; Dravid, Vinayak P.; Kanatzidis, Mercouri G; Wolverton, Christopher M.
In: Journal of the American Chemical Society, Vol. 136, No. 4, 29.01.2014, p. 1628-1635.Research output: Contribution to journal › Article
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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.
UR - http://www.scopus.com/inward/record.url?scp=84893514172&partnerID=8YFLogxK
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U2 - 10.1021/ja411857y
DO - 10.1021/ja411857y
M3 - Article
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 -