Highly Excited States from a Time Independent Density Functional Method

Abstract

Abstract:A constrained optimized effective potential (COEP) methodology proposed earlier by us for singly low-lying excited states is extended to highly excited states having the same spatial and spin symmetry. Basic tenets of time independent density functional theory and its COEP implementation for excited states are briefly reviewed. The amended Kohn-Sham-like equations for excited state orbitals and their specific features for highly excited states are discussed. The accuracy of the method is demonstrated using exchange-only calculations for highly excited states of the He and Li atoms.

Density Functional Theory of Highly Excited States of Coulomb Systems

“…Table 1 presents the total energies for the ground state and the excited states with configuration 1s 2 ms, m = 2, ..., 7 for the Li atom. The KLI values can be directly compared with the exchange-only results of the spin-dependent localized Hartree-Fock (SLHF) [63], xCOEP [64], and Hartree-Fock (HF) [65] methods. x-COEP refers to exchange-only constrained optimized effective potential (xCOEP) methodology [64].…”

“…The KLI values can be directly compared with the exchange-only results of the spin-dependent localized Hartree-Fock (SLHF) [63], xCOEP [64], and Hartree-Fock (HF) [65] methods. x-COEP refers to exchange-only constrained optimized effective potential (xCOEP) methodology [64]. SLHFc is localized Hartree-Fock combined with Lee-Yang-Parr (LYP) correlation [66].…”

Special Issue “50th Anniversary of the Kohn–Sham Theory—Advances in Density Functional Theory”

“…Glushkov et al [16] treat highly excited states by a time-independent DFT method with the constrained optimized effective potential (COEP) methodology. They propose Kohn-Sham-like equations for excited states and discuss the accuracy of their scheme for selected cases.…”

Combining extrapolation with ghost interaction correction in range-separated ensemble density functional theory for excited states

“…4 Some of these limitations can be overcome by the use of Savin's idea of range separation [21][22][23] and double-hybrid kernels. 24 The need for time-independent alternatives to TD-DFT for modeling excited states has attracted increasing attention over the years [25][26][27][28][29][30][31][32][33] . In this work we focus on one of them, namely ensemble DFT (eDFT), which is an in-principle-exact approach for the calculation of excitation energies.…”