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, and Leeor Kronik
Phys. Rev. Lett. 109, 226405 – Published 28 November 2012
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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.

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  • Received 9 March 2012

DOI:https://doi.org/10.1103/PhysRevLett.109.226405

© 2012 American Physical Society

Authors & Affiliations

Sivan Refaely-Abramson1, Sahar Sharifzadeh2, Niranjan Govind3, Jochen Autschbach4, Jeffrey B. Neaton2, Roi Baer5, and Leeor Kronik1

  • 1Department of Materials and Interfaces, Weizmann Institute of Science, Rehovoth 76100, Israel
  • 2Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
  • 3William R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, USA
  • 4Department of Chemistry, University at Buffalo, State University of New York, Buffalo, New York 14260-3000, USA
  • 5Fritz Haber Center for Molecular Dynamics, Institute of Chemistry, Hebrew University, Jerusalem 91904, Israel

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Issue

Vol. 109, Iss. 22 — 30 November 2012

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