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

Abstract

We present a method for obtaining quasiparticle excitation energies from a DFT-based calculation, but with 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 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 non-empirically, per system, based on satisfaction of exact physical constraints for the ionization potential and many-electron self-interaction, respectively. The accuracy of the method is demonstrated on the important benchmark molecule, 3,4,9,10-perylene-tetracarboxylic-dianydride (PTCDA), where it is shown to be the only non-empirical DFT-based method comparable to GW calculations. For any finite system, we envision that the approach could be useful directly as an inexpensive alternative to GW that offers good accuracy for both frontier and non-frontier quasiparticle excitation energies, opening the door to the studyof presently out of reach large-scale systems.

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1059198
Report Number(s):
PNNL-SA-86302
46003; 26690; KP1704020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Physical Review Letters, 109(22):Article No. 226405
Additional Journal Information:
Journal Name: Physical Review Letters, 109(22):Article No. 226405
Country of Publication:
United States
Language:
English
Subject:
Quasiparticle; spectra; hybrid density functional; excitation; calculations; perturbation; Environmental Molecular Sciences Laboratory

Citation Formats

Refaely-Abramson, Sivan, Sharifzadeh, Sahar, Govind, Niranjan, Autschbach, Jochen, Neaton, Jeffrey B, Baer, Roi, and Kronik, Leeor. Quasiparticle spectra from a nonempirical optimally tuned range-separated hybrid density functional. United States: N. p., 2012. Web. doi:10.1103/PhysRevLett.109.226405.
Refaely-Abramson, Sivan, Sharifzadeh, Sahar, Govind, Niranjan, Autschbach, Jochen, Neaton, Jeffrey B, Baer, Roi, & Kronik, Leeor. Quasiparticle spectra from a nonempirical optimally tuned range-separated hybrid density functional. United States. doi:10.1103/PhysRevLett.109.226405.
Refaely-Abramson, Sivan, Sharifzadeh, Sahar, Govind, Niranjan, Autschbach, Jochen, Neaton, Jeffrey B, Baer, Roi, and Kronik, Leeor. Wed . "Quasiparticle spectra from a nonempirical optimally tuned range-separated hybrid density functional". United States. doi:10.1103/PhysRevLett.109.226405.
@article{osti_1059198,
title = {Quasiparticle spectra from a nonempirical optimally tuned range-separated hybrid density functional},
author = {Refaely-Abramson, Sivan and Sharifzadeh, Sahar and Govind, Niranjan and Autschbach, Jochen and Neaton, Jeffrey B and Baer, Roi and Kronik, Leeor},
abstractNote = {We present a method for obtaining quasiparticle excitation energies from a DFT-based calculation, but with 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 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 non-empirically, per system, based on satisfaction of exact physical constraints for the ionization potential and many-electron self-interaction, respectively. The accuracy of the method is demonstrated on the important benchmark molecule, 3,4,9,10-perylene-tetracarboxylic-dianydride (PTCDA), where it is shown to be the only non-empirical DFT-based method comparable to GW calculations. For any finite system, we envision that the approach could be useful directly as an inexpensive alternative to GW that offers good accuracy for both frontier and non-frontier quasiparticle excitation energies, opening the door to the studyof presently out of reach large-scale systems.},
doi = {10.1103/PhysRevLett.109.226405},
journal = {Physical Review Letters, 109(22):Article No. 226405},
number = ,
volume = ,
place = {United States},
year = {2012},
month = {11}
}