Tight-binding approximations to time-dependent density functional theory - A fast approach for the calculation of electronically excited states

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Robert Rüger - , Software for Chemistry & Materials, Vrije Universiteit Amsterdam (VU), Leipzig University (Author)
  • Erik Van Lenthe - , Software for Chemistry & Materials (Author)
  • Thomas Heine - , Leipzig University (Author)
  • Lucas Visscher - , Vrije Universiteit Amsterdam (VU) (Author)

Abstract

We propose a new method of calculating electronically excited states that combines a density functional theory based ground state calculation with a linear response treatment that employs approximations used in the time-dependent density functional based tight binding (TD-DFTB) approach. The new method termed time-dependent density functional theory TD-DFT+TB does not rely on the DFTB parametrization and is therefore applicable to systems involving all combinations of elements. We show that the new method yields UV/Vis absorption spectra that are in excellent agreement with computationally much more expensive TD-DFT calculations. Errors in vertical excitation energies are reduced by a factor of two compared to TD-DFTB.

Details

Original languageEnglish
Article number184103
JournalJournal of Chemical Physics
Volume144
Issue number18
Publication statusPublished - 14 May 2016
Peer-reviewedYes
Externally publishedYes