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Different Types of Vibrations Interacting with Electronic Excitations in Phycoerythrin 545 and Fenna–Matthews–Olson Antenna Systems

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School of Engineering and Science, Jacobs University Bremen, Campus Ring 1, 28759 Bremen, Germany
‡ § Center for Biophysics and Computational Biology and Beckman Institute and §Department of Physics, University of Illinois at Urbana−Champaign, Urbana, Illinois 61801, United States
Cite this: J. Phys. Chem. Lett. 2014, 5, 18, 3131–3137
Publication Date (Web):August 27, 2014
https://doi.org/10.1021/jz501351p
Copyright © 2014 American Chemical Society

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    Abstract

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    The interest in the phycoerythrin 545 (PE545) photosynthetic antenna system of marine algae and the Fenna–Matthews–Olson (FMO) complex of green sulfur bacteria has drastically increased since long-lived quantum coherences were reported for these complexes. For the PE545 complex, this phenomenon is clearly visible even at ambient temperatures, while for the FMO system it is more prominent at lower temperatures. The key to elucidate the role of the environment in these long-lived quantum effects is the spectral density. Here, we employ molecular dynamics simulations combined with quantum chemistry calculations to study the coupling between the biological environment and the vertical excitation energies of the bilin pigment molecules in PE545 and compare them to prior calculations on the FMO complex. It is found that the overall strength of the resulting spectral densities for the PE545 system is similar to the experiment-based counterpart but also to those in the FMO complex. Molecular analysis, however, reveals that the origin for the spectral densities in the low frequency range, which is most important for excitonic transitions, is entirely different. In the case of FMO, this part of the spectral density is due to environmental fluctuations, while, in case of PE545, it is essentially only due to internal modes of the bilin molecules. This finding sheds new light on possible explanations of the long-lived quantum coherences and that the reasons might actually be different in dissimilar systems.

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    Computed energy gap distributions, autocorrelation functions and spectral densities of the individual bilins in the PE545 complex are shown. This material is available free of charge via the Internet at http://pubs.acs.org/.

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