Theoretical unification of hybrid-DFT andDFT + Umethods for the treatment of localized orbitals

2014/06/11 by Viktor Ivády, Rickard Armiento, Krisztián Szász +4 · 63 citations
Chemistry · Engineering · Physics and Astronomy · #Algorithm #Chemistry #Computer science #Crystallography #Density functional theory #Hexagonal crystal system #Hybrid functional #Impurity #Materials science #Physics #Quantum mechanics #Semiconductor materials and devices #Semiconductor materials and interfaces #Silicon Carbide Semiconductor Technologies #Vanadium #Wurtzite crystal structure #cond-mat.str-el

paper · pdf · doi:10.1103/physrevb.90.035146

published in Physical Review B 90(3) (American Physical Society)

arxiv created 2014/06/11 · openalex publication_date 2014/07/30 · arxiv updated 2015/05/22 · openalex created_date 2016/06/24 · openalex updated_date 2026/08/05

Abstract

Hybrid functionals serve as a powerful practical tool in different fields of computational physics and quantum chemistry. On the other hand, their applicability for the case of correlated d and f orbitals is still questionable and needs more considerations. In this article we formulate the on-site occupation dependent exchange correlation energy and effective potential of hybrid functionals for localized states and connect them to the on-site correction term of the DFT + U method. The resultant formula indicates that the screening of the onsite electron repulsion is governed by the ratio of the exact exchange in hybrid functionals. Our derivation provides a theoretical justification for adding a DFT + U-like on-site potential in hybrid-DFT calculations to resolve issues caused by overscreening of localized states. The resulting scheme, hybrid DFT + V_w, is tested for chromium impurity in wurtzite AlN and vanadium impurity in 4H-SiC, which are paradigm examples of systems with different degrees of localization between host and impurity orbitals.

Citations

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