Surface hopping modeling of two-dimensional spectra

Roel Tempelaar, Cornelis P. Van Der Vegte, Jasper Knoester, Thomas L.C. Jansen

Research output: Contribution to journalArticle

37 Scopus citations

Abstract

Recently, two-dimensional (2D) electronic spectroscopy has become an important tool to unravel the excited state properties of complex molecular assemblies, such as biological light harvesting systems. In this work, we propose a method for simulating 2D electronic spectra based on a surface hopping approach. This approach self-consistently describes the interaction between photoactive chromophores and the environment, which allows us to reproduce a spectrally observable dynamic Stokes shift. Through an application to a dimer, the method is shown to also account for correct thermal equilibration of quantum populations, something that is of great importance for processes in the electronic domain. The resulting 2D spectra are found to nicely agree with hierarchy of equations of motion calculations. Contrary to the latter, our method is unrestricted in describing the interaction between the chromophores and the environment, and we expect it to be applicable to a wide variety of molecular systems.

Original languageEnglish (US)
Article number164106
JournalJournal of Chemical Physics
Volume138
Issue number16
DOIs
StatePublished - Apr 28 2013

ASJC Scopus subject areas

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

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