Ultrafast exciton-exciton coherent transfer in molecular aggregates and its application to light-harvesting systems

Kim Hyeon-Deuk, Yoshitaka Tanimura, Minheang Cho

Research output: Contribution to journalArticle

18 Citations (Scopus)

Abstract

Effects of the exciton-exciton coherence transfer (EECT) in strongly coupled molecular aggregates are investigated from the reduced time-evolution equation which we have developed to describe EECT. Starting with the nonlinear response function, we obtained explicit contributions from EECT to four-wave-mixing spectrum such as photon echo, taking into account double exciton states, static disorder, and heat-bath coupling represented by arbitrary spectral densities. By using the doorway-window picture and the projection operator technique, the transfer rates between two different electronic coherent states are obtained within a framework of cumulant expansion at high temperature. Applications of the present theory to strongly coupled B850 chlorophylls in the photosynthetic light harvesting system II (LH2) are discussed. It is shown that EECT is indispensable in properly describing ultrafast phenomena of strongly coupled molecular aggregates such as LH2 and that the EECT contribution to the two-dimensional optical spectroscopy is not negligible.

Original languageEnglish
Article number075101
JournalJournal of Chemical Physics
Volume127
Issue number7
DOIs
Publication statusPublished - 2007

ASJC Scopus subject areas

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

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