Quasiparticle spectra from a nonempirical optimally tuned range-separated hybrid density functional

Sivan Refaely-Abramson*, Sahar Sharifzadeh, Niranjan Govind, Jochen Autschbach, Jeffrey B. Neaton, Roi Baer, Leeor Kronik

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

238 Scopus citations

Abstract

We present a method for obtaining outer-valence quasiparticle excitation energies from a density-functional-theory-based calculation, with an accuracy that is comparable to that of many-body perturbation theory within the GW approximation. The approach uses a range-separated hybrid density functional, with an asymptotically exact and short-range fractional Fock exchange. The functional contains two parameters, the range separation and the short-range Fock fraction. Both are determined nonempirically, per system, on the basis of the satisfaction of exact physical constraints for the ionization potential and frontier-orbital many-electron self-interaction, respectively. The accuracy of the method is demonstrated on four important benchmark organic molecules: perylene, pentacene, 3,4,9,10-perylene-tetracarboxylic-dianydride (PTCDA), and 1,4,5,8-naphthalene-tetracarboxylic-dianhydride (NTCDA). We envision that for the outer-valence excitation spectra of finite systems the approach could provide an inexpensive alternative to GW, opening the door to the study of presently out of reach large-scale systems.

Original languageAmerican English
Article number226405
JournalPhysical Review Letters
Volume109
Issue number22
DOIs
StatePublished - 28 Nov 2012

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