Following the observation of long-lived coherences in the two-dimensional (2D) electronic spectra of the Fenna-Matthews-Olson (FMO) complex, many theoretical works suggest that coherences between excitons may play a role in the efficient energy transfer that occurs in photosynthetic antennae. This interpretation of the dynamics depends on the assignment of quantum beating signals to superpositions of excitons, which is complicated by the possibility of observing both electronic and vibrational coherences in 2D spectra. Here, we explore 2D spectra of bacteriochlorophyll a (BChla) in solution in an attempt to isolate vibrational beating signals in the absence of excitonic signals to identify the origin of the quantum beats in 2D spectra of FMO. Even at high laser power, our BChla spectra show strong beating only from the nonresonant response of the solvent. The beating signals that we can conclusively assign to vibrational modes of BChla are only slightly above the noise and at higher frequencies than those previously observed in spectra of FMO. Our results suggest that the beating observed in spectra of FMO is of a radically different character than the signals observed here and can therefore be attributed to electronic coherences or intermolecular degrees of freedom.
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28 September 2012
Research Article|
September 24 2012
Two-dimensional electronic spectroscopy of bacteriochlorophyll a in solution: Elucidating the coherence dynamics of the Fenna-Matthews-Olson complex using its chromophore as a control
Kelly A. Fransted;
Kelly A. Fransted
Department of Chemistry and The James Franck Institute,
The University of Chicago
, Chicago, Illinois 60637, USA
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Justin R. Caram;
Justin R. Caram
Department of Chemistry and The James Franck Institute,
The University of Chicago
, Chicago, Illinois 60637, USA
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Dugan Hayes;
Dugan Hayes
Department of Chemistry and The James Franck Institute,
The University of Chicago
, Chicago, Illinois 60637, USA
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Gregory S. Engel
Gregory S. Engel
Department of Chemistry and The James Franck Institute,
The University of Chicago
, Chicago, Illinois 60637, USA
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J. Chem. Phys. 137, 125101 (2012)
Article history
Received:
July 09 2012
Accepted:
August 28 2012
Citation
Kelly A. Fransted, Justin R. Caram, Dugan Hayes, Gregory S. Engel; Two-dimensional electronic spectroscopy of bacteriochlorophyll a in solution: Elucidating the coherence dynamics of the Fenna-Matthews-Olson complex using its chromophore as a control. J. Chem. Phys. 28 September 2012; 137 (12): 125101. https://doi.org/10.1063/1.4752107
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