Rate expressions for excitation transfer. IV. Energy migration and superexchange phenomena

Gregory D. Scholes, Kenneth P. Ghiggino

Research output: Contribution to journalArticlepeer-review

32 Scopus citations

Abstract

General microscopic mechanisms of electronic excitation (energy) transfer (EET) in multichromophoric assemblies are investigated. Aspects of superexchange-mediated EET and energy migration (EM) and their contribution to the efficiency of donor-to-trap energy transport processes in macromolecules are discussed from a quantum mechanical viewpoint. The possibility of superexchange pathways for EM via higher excited states of the intermediate chromophores is introduced. The role of quasicoherent EM pathways, and how they are manifested in the quantum mechanical rate expression, is investigated and the significance of contributions to the rate arising through quantum mechanical interference between pathways is elucidated. The theory indicates conditions under which coherent EM pathways may significantly increase the efficiency of energy transport and trapping and the applications to natural and synthetic light-harvesting systems are outlined.

Original languageEnglish (US)
Pages (from-to)8873-8883
Number of pages11
JournalThe Journal of chemical physics
Volume103
Issue number20
DOIs
StatePublished - Jan 1 1995
Externally publishedYes

All Science Journal Classification (ASJC) codes

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

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