Two-dimensional electronic spectroscopy using incoherent light: Theoretical analysis

Daniel B. Turner, Dylan J. Howey, Erika J. Sutor, Rebecca A. Hendrickson, M. W. Gealy, Darin J. Ulness

Research output: Contribution to journalArticlepeer-review

Abstract

Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations in two-dimensional electronic spectroscopy measurements of pigment-protein complexes measured with femtosecond laser pulses. A persistent issue in the field is to reconcile the results of measurements performed using femtosecond laser pulses with physiological illumination conditions. Noisy-light spectroscopy can begin to address this question. In this work we present the theoretical analysis of incoherent two-dimensional electronic spectroscopy, I(4) 2D ES. Simulations reveal diagonal peaks, cross peaks, and coherent oscillations similar to those observed in femtosecond two-dimensional electronic spectroscopy experiments. The results also expose fundamental differences between the femtosecond-pulse and noisy-light techniques; the differences lead to new challenges and new opportunities.

Original languageEnglish (US)
Pages (from-to)5926-5954
Number of pages29
JournalJournal of Physical Chemistry A
Volume117
Issue number29
DOIs
StatePublished - Jul 25 2013

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

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