Dissipative dynamics of a system passing through a conical intersection: Ultrafast pump-probe observables

David Gelman, Gil Katz, Ronnie Kosloff, Mark A. Ratner

Research output: Contribution to journalArticle

21 Citations (Scopus)

Abstract

The dynamics of a system incorporating a conical intersection, in the presence of a dissipative environment, is studied with the purpose of identifying observable ultrafast spectroscopic signatures. A model system consisting of two vibronically coupled electronic states with two nuclear degrees of freedom is constructed. Dissipation is treated by two different methods, Lindblad semigroup formalism and the surrogate Hamiltonian approach. Pump-probe experimental expectation values such as transient emission and transient absorption are calculated and compared to the adiabatic and diabatic population transfer. The ultrafast population transfer reflecting the conical intersection is not mirrored in transient absorption measurements such as the recovery of the bleach. Emission from the excited state can be suppressed on the ultrafast time scale, but the existence of a conical intersection is only one of the possible mechanisms that can provide ultrafast damping of emission.

Original languageEnglish
Article number134112
JournalJournal of Chemical Physics
Volume123
Issue number13
DOIs
Publication statusPublished - Oct 3 2005

ASJC Scopus subject areas

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

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