Self-consistent generalized Kohn-Sham local hybrid functionals of screened exchange: Combining local and range-separated hybridization
- 28 September 2008
- journal article
- research article
- Published by AIP Publishing in The Journal of Chemical Physics
- Vol. 129 (12), 124110
- https://doi.org/10.1063/1.2980056
Abstract
We present local hybrid functionals that incorporate a position-dependent admixture of short-range (screened) nonlocal exact [Hartree-Fock-type (HF)] exchange. We test two limiting cases: screened local hybrids with no long-range HF exchange and long-range-corrected local hybrids with 100% long-range HF exchange. Long-range-corrected local hybrids provide the exact asymptotic exchange-correlation potential in finite systems, while screened local hybrids avoid the problems inherent to long-range HF exchange in metals and small-bandgap systems. We treat these functionals self-consistently using the nonlocal exchange potential constructed from Kohn-Sham orbital derivatives. Generalized Kohn-Sham calculations with screened and long-range-corrected local hybrids can provide accurate molecular thermochemistry and kinetics, comparable to existing local hybrids of full-range exchange. Generalized Kohn-Sham calculations with existing full-range local hybrids provide results consistent with previous non-self-consistent and “localized local hybrid” calculations. These new functionals appear to provide a promising extension of existing local and range-separated hybrids.Keywords
This publication has 92 references indexed in Scilit:
- Generalized-gradient exchange-correlation hole obtained from a correlation factor ansatzThe Journal of Chemical Physics, 2008
- Generalized gradient approximation model exchange holes for range-separated hybridsThe Journal of Chemical Physics, 2008
- Effective local potentials for orbital-dependent density functionalsThe Journal of Chemical Physics, 2006
- Efficient hybrid density functional calculations in solids: Assessment of the Heyd–Scuseria–Ernzerhof screened Coulomb hybrid functionalThe Journal of Chemical Physics, 2004
- Comparative assessment of a new nonempirical density functional: Molecules and hydrogen-bonded complexesThe Journal of Chemical Physics, 2003
- Efficient localized Hartree–Fock methods as effective exact-exchange Kohn–Sham methods for moleculesThe Journal of Chemical Physics, 2001
- Toward reliable density functional methods without adjustable parameters: The PBE0 modelThe Journal of Chemical Physics, 1999
- Steady state simulation of planar elongation flow by nonequilibrium molecular dynamicsThe Journal of Chemical Physics, 1999
- A new mixing of Hartree–Fock and local density-functional theoriesThe Journal of Chemical Physics, 1993
- Direct-space analysis of the Hartree-Fock energy bands and density of states for metallic extended systemsPhysical Review B, 1987