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Title: Understanding the origin of bandgap problem in transition and post-transition metal oxides

Abstract

Improving electronic structure calculations for practical and technologically-important materials has been a never-ending pursue. This is especially true for transition and post-transition metal oxides for which the current first-principles approaches still suffer various drawbacks. Here we present a hierarchical-hybrid functional approach built on the use of pseudopotentials. The key is to introduce a discontinuity in the exchange functional between core and valence electrons. It allows for treating the localization errors of sp and d electrons differently, which have been known to be an important source of error for the band structure. Using ZnO as a prototype, we show the approach is successful in simultaneously reproducing the band gap and d-band position. Remarkably, the same approach, without having to change the hybrid mixing parameters from those of Zn, works reasonably well for other binary 3d transition and post-transition metal oxides across board. Finally, our findings point to a new direction of systematically improving the exchange functional in first-principles calculations.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4];  [5]
  1. Tsinghua Univ., Beijing (China)
  2. Inst. of Applied Physics and Computational Mathematics, Beijing (China)
  3. Beijing Inst. of Technology (China)
  4. Tsinghua Univ., Beijing (China); Tsinghua Univ., Beijing (China)
  5. Rensselaer Polytechnic Inst., Troy, NY (United States)
Publication Date:
Research Org.:
Rensselaer Polytechnic Inst., Troy, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1594893
Grant/Contract Number:  
SC0002623; 51788104; 2016YFA0301001; 11674071; 11874089; 11674188
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 12; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; first-principles; pseudopotentials

Citation Formats

Tan, Hengxin, Liu, Haitao, Li, Yuanchang, Duan, Wenhui, and Zhang, Shengbai. Understanding the origin of bandgap problem in transition and post-transition metal oxides. United States: N. p., 2019. Web. doi:10.1063/1.5111188.
Tan, Hengxin, Liu, Haitao, Li, Yuanchang, Duan, Wenhui, & Zhang, Shengbai. Understanding the origin of bandgap problem in transition and post-transition metal oxides. United States. doi:10.1063/1.5111188.
Tan, Hengxin, Liu, Haitao, Li, Yuanchang, Duan, Wenhui, and Zhang, Shengbai. Wed . "Understanding the origin of bandgap problem in transition and post-transition metal oxides". United States. doi:10.1063/1.5111188. https://www.osti.gov/servlets/purl/1594893.
@article{osti_1594893,
title = {Understanding the origin of bandgap problem in transition and post-transition metal oxides},
author = {Tan, Hengxin and Liu, Haitao and Li, Yuanchang and Duan, Wenhui and Zhang, Shengbai},
abstractNote = {Improving electronic structure calculations for practical and technologically-important materials has been a never-ending pursue. This is especially true for transition and post-transition metal oxides for which the current first-principles approaches still suffer various drawbacks. Here we present a hierarchical-hybrid functional approach built on the use of pseudopotentials. The key is to introduce a discontinuity in the exchange functional between core and valence electrons. It allows for treating the localization errors of sp and d electrons differently, which have been known to be an important source of error for the band structure. Using ZnO as a prototype, we show the approach is successful in simultaneously reproducing the band gap and d-band position. Remarkably, the same approach, without having to change the hybrid mixing parameters from those of Zn, works reasonably well for other binary 3d transition and post-transition metal oxides across board. Finally, our findings point to a new direction of systematically improving the exchange functional in first-principles calculations.},
doi = {10.1063/1.5111188},
journal = {Journal of Chemical Physics},
number = 12,
volume = 151,
place = {United States},
year = {2019},
month = {9}
}

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