Evidence of Correlated Static Disorder in the Fenna-Matthews-Olson Complex

Alexander S. Fokas, Daniel J. Cole, Nicholas D.M. Hine, Stephen A. Wells, Michael C. Payne, Alex W. Chin

Research output: Contribution to journalArticlepeer-review

9 Citations (SciVal)


Observation of excitonic quantum beats in photosynthetic antennae has prompted wide debate regarding the function of excitonic coherence in pigment-protein complexes. Much of this work focuses on the interactions of excitons with the femto-to-picosecond dynamical fluctuations of their environment. However, in experiments these effects can be masked by static disorder of the excited-state energies across ensembles, whose microscopic origins are challenging to predict. Here the excited-state properties of ∼2000 atom clusters of the Fenna-Matthews-Olson complex are simulated using a unique combination of linear-scaling density functional theory and constrained geometric dynamics. While slow, large amplitude protein motion leads to large variations in the Qy transitions of two pigments, we identify pigment-protein correlations that greatly reduce variations in the energy gap across the ensemble, which is consistent with experimental observations of suppressed inhomogeneous dephasing of quantum beats.

Original languageEnglish
Pages (from-to)2350-2356
Number of pages7
JournalJournal of Physical Chemistry Letters
Issue number10
Publication statusPublished - 18 May 2017

ASJC Scopus subject areas

  • General Materials Science


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