Electrical response of molecular systems: the power of self-interaction corrected Kohn-Sham theory

Abstract

The accurate prediction of electronic response properties of extended molecular systems has been a challenge for conventional, explicit density functionals. We demonstrate that a self-interaction correction implemented rigorously within Kohn-Sham theory via the Optimized Effective Potential (OEP) yields polarizabilities close to the ones from highly accurate wavefunction-based calculations and exceeding the quality of exact-exchange-OEP. The orbital structure obtained with the OEP-SIC functional and approximations to it are discussed.

accepted for publication in Physical Review Letters

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• The Generalized SIC-OEP formalism and the Generalized SIC-Slater approximation (stationary and time-dependent cases)
• Polarizibilities as a test of localized approximations to the self-interaction correction
• Density functional description of Coulomb blockade: Adiabatic or dynamic exchange-correlation?
• Implementation of Perdew-Zunger self-interaction correction in real space using Fermi-Löwdin orbitals