Perspectives on double-excitations in TDDFT

Peter Elliott, Sharma Goldson, Chris Canahui, Neepa T. Maitra

Research output: Contribution to journalArticlepeer-review

127 Scopus citations

Abstract

The adiabatic approximation in time-dependent density functional theory (TDDFT) yields reliable excitation spectra with great efficiency in many cases, but fundamentally fails for states of double-excitation character. We discuss how double-excitations are at the root of some of the most challenging problems for TDDFT today. We then present new results for (i) the calculation of autoionizing resonances in the helium atom, (ii) understanding the nature of the double excitations appearing in the quadratic response function, and (iii) retrieving double-excitations through a real-time semiclassical approach to correlation in a model quantum dot.

Original languageEnglish (US)
Pages (from-to)110-119
Number of pages10
JournalChemical Physics
Volume391
Issue number1
DOIs
StatePublished - Nov 24 2011
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Keywords

  • Adiabatic approximation
  • Autoionization
  • DFT
  • Density functional
  • Density matrix
  • Double excitations
  • Frozen Gaussian
  • Kohn-Sham
  • Linear-response
  • Quadratic response
  • Second-order response
  • Semiclassical
  • TDDFT

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