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Biophys. J. BioFAST: First Published January 11, 2008. doi:10.1529/biophysj.107.123455
© 2008 by the Biophysical Society.

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PHOTOBIOPHYSICS

Unravelling coherent dynamics and energy dissipation in photosynthetic complexes by 2D spectroscopy

Darius Abramavicius 1, Dmitri V. Voronine 2 and Shaul Mukamel 3*

1 University of California, Irvine
2 University of California Irvine
3 University of California

* To whom correspondence should be addressed. E-mail: smukamel{at}uci.edu.

Submitted on October 10, 2007
Revised on November 26, 2007
Accepted on 11 December 2007


  Abstract
Spectroscopic studies of light harvesting and the subsequent energy conversion in photosynthesis can track quantum dynamics happening on the microscopic level. The Fenna-Matthews-Olson complex (FMO) of the photosynthetic green sulphur bacteria Chlorobium (C.) tepidum is a prototype efficient light harvesting antenna: it stores the captured photon energy in the form of excitons (collective excitations), which are subsequently converted to chemical energy with almost 100% efficiency. These excitons show an elaborate relaxation pattern involving coherent and incoherent pathways. We make use of the complex chirality and fundamental symmetries of multidimensional optical signals to design new sequences of ultrashort laser pulses which can distinguish between coherent quantum oscillations and incoherent energy dissipation during the exciton relaxation. The cooperative dynamical features, which reflect the coherent nature of excitations, are amplified. The extent of quantum oscillations and their timescales in photosynthesis can be readily extracted from the designed signals, showing that cooperativity is maintained during energy transport in FMO. The proposed pulse sequences can also be applied to reveal information on the robustness of quantum states in the presence of fluctuating environments in other nanoscopic complexes and devices.

Key Words: FMO complex, coherence, energy transfer, excitons, photosynthesis, ultrafast spectroscopy




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D. V. Voronine, D. Abramavicius, and S. Mukamel
Chirality-Based Signatures of Local Protein Environments in Two-Dimensional Optical Spectroscopy of Two Species Photosynthetic Complexes of Green Sulfur Bacteria: Simulation Study
Biophys. J., November 15, 2008; 95(10): 4896 - 4907.
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 Proc. Natl. Acad. Sci. USAHome page
D. Abramavicius, D. V. Voronine, and S. Mukamel
Double-quantum resonances and exciton-scattering in coherent 2D spectroscopy of photosynthetic complexes
PNAS, June 24, 2008; 105(25): 8525 - 8530.
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Copyright © 2008 by the Biophysical Society.