Physics of bandgap formation in Cu-Sb-Se based novel thermoelectrics: the role of Sb valency and Cu d levels

被引：30

作者：

Do, Dat ^{[1
]}

Ozolins, Vidvuds ^{[2
]}

Mahanti, S. D. ^{[1
]}

Lee, Mal-Soon ^{[1
]}

Zhang, Yongsheng ^{[3
]}

Wolverton, C. ^{[3
]}

机构：

[1] Michigan State Univ, Dept Phys & Astron, E Lansing, MI 48824 USA

[2] Univ Calif Los Angeles, Dept Mat Sci & Engn, Los Angeles, CA 90095 USA

[3] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA

来源：

JOURNAL OF PHYSICS-CONDENSED MATTER | 2012年 / 24卷 / 41期

关键词：

TOTAL-ENERGY CALCULATIONS; CRYSTAL-STRUCTURE; WAVE; SPECTRA;

D O I：

10.1088/0953-8984/24/41/415502

中图分类号：

O469 [凝聚态物理学];

学科分类号：

070205 ;

摘要：

In this paper we discuss the results of ab initio electronic structure calculations for Cu3SbSe4 (Se4) and Cu3SbSe3 (Se3), two narrow bandgap semiconductors of thermoelectric interest. We find that Sb is trivalent in both the compounds, in contrast to a simple nominal valence (ionic) picture which suggests that Sb should be 5+ in Se4. The gap formation in Se4 is quite subtle, with hybridization between Sb 5s and the neighboring Se 4s, 4p orbitals, position of Cu d states, and non-local exchange interaction, each playing significant roles. Thermopower calculations show that Se4 is a better p-type system. Our theoretical results for Se4 agree very well with recent experimental results obtained by Skoug et al (2011 Sci. Adv. Mater. 3 602).

引用

页数：7

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