Coherent energy transfer under incoherent light conditions

Francesca Fassioli, Alexandra Olaya-Castro, Gregory D. Scholes

Research output: Contribution to journalArticle

49 Scopus citations

Abstract

Recent two-dimensional electronic spectroscopy (2DES) experiments have reported evidence of coherent dynamics of electronic excitations in several light-harvesting antennae. However, 2DES uses ultrafast coherent laser pulses as an excitation source; therefore, there is a current debate on whether coherent excitation dynamics is present under natural sunlight - incoherent - illumination conditions. In this letter, we show that even if incoherent light excites an electronic state with no initial quantum superpositions among excitonic states, energy transfer can proceed quantum coherently if nonequilibrium dynamics of the phonon environment takes place. Such nonequilibrium behavior manifests itself in non-Markovian evolution of electronic excitations and is typical of many photosynthetic systems. We therefore argue that light-harvesting antennae have mechanisms that could support coherent evolution under incoherent illumination.

Original languageEnglish (US)
Pages (from-to)3136-3142
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume3
Issue number21
DOIs
StatePublished - Nov 1 2012
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

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