Spin polarization, orbital occupation and band gap opening in vanadium dioxide: The effect of screened Hartree-Fock exchange
Type
ArticleKAUST Department
Computational Physics and Materials Science (CPMS)Material Science and Engineering Program
Physical Science and Engineering (PSE) Division
Date
2014-07Permanent link to this record
http://hdl.handle.net/10754/563615
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The metal-insulator transition of VO2 so far has evaded an accurate description by density functional theory. The screened hybrid functional of Heyd, Scuseria and Ernzerhof leads to reasonable solutions for both the low-temperature monoclinic and high-temperature rutile phases only if spin polarization is excluded from the calculations. We explore whether a satisfactory agreement with experiment can be achieved by tuning the fraction of Hartree Fock exchange (α) in the density functional. It is found that two branches of locally stable solutions exist for the rutile phase for 12.5%≤α≤20%. One is metallic and has the correct stability as compared to the monoclinic phase, the other is insulating with lower energy than the metallic branch. We discuss these observations based on the V 3d orbital occupations and conclude that α=10% is the best possible choice for spin-polarized VO2 calculations. © 2014 Elsevier B.V. All rights reserved.Citation
Wang, H., Mellan, T. A., Grau-Crespo, R., & Schwingenschlögl, U. (2014). Spin polarization, orbital occupation and band gap opening in vanadium dioxide: The effect of screened Hartree–Fock exchange. Chemical Physics Letters, 608, 126–129. doi:10.1016/j.cplett.2014.05.070Sponsors
We thank the EPSRC for funding (EP/J001775/1) and for access to the HECToR supercomputer via the Materials Chemistry Consortium (EP/L000202).Publisher
Elsevier BVJournal
Chemical Physics Lettersae974a485f413a2113503eed53cd6c53
10.1016/j.cplett.2014.05.070