Direct Extraction of Excitation Energies from Ensemble Density-Functional Theory

Zeng-hui Yang, Aurora Pribram-Jones, Kieron Burke, and Carsten A. Ullrich
Phys. Rev. Lett. 119, 033003 – Published 21 July 2017
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Abstract

A very specific ensemble of ground and excited states is shown to yield an exact formula for any excitation energy as a simple correction to the energy difference between orbitals of the Kohn-Sham ground state. This alternative scheme avoids either the need to calculate many unoccupied levels as in time-dependent density functional theory (TDDFT) or the need for many self-consistent ensemble calculations. The symmetry-eigenstate Hartree-exchange (SEHX) approximation yields results comparable to standard TDDFT for atoms. With this formalism, SEHX yields approximate double excitations, which are missed by adiabatic TDDFT.

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  • Received 30 March 2017

DOI:https://doi.org/10.1103/PhysRevLett.119.033003

© 2017 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Zeng-hui Yang1,*, Aurora Pribram-Jones2,3, Kieron Burke4, and Carsten A. Ullrich5

  • 1Microsystem and Terahertz Research Center, China Academy of Engineering Physics, Chengdu 610200, China
  • 2Department of Chemistry, University of California, Berkeley, California 94720, USA
  • 3Lawrence Livermore National Laboratory, Livermore, California 94550, USA
  • 4Department of Chemistry, University of California-Irvine, Irvine, California 92697, USA
  • 5Department of Physics and Astronomy, University of Missouri, Columbia, Missouri 65211, USA

  • *Corresponding author. yangzenghui@mtrc.ac.cn

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Issue

Vol. 119, Iss. 3 — 21 July 2017

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