Atomistic Study of the Long-Lived Quantum Coherences in the Fenna-Matthews-Olson Complex

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Atomistic Study of the Long-Lived Quantum Coherences in the Fenna-Matthews-Olson Complex

Show simple item record Aspuru-Guzik, Alan Shim, Sangwoo Rebentrost, Patrick Valleau, Stephanie 2012-03-14T18:01:23Z 2011
dc.identifier.citation Shim, Sangwoo, Patrick Rebentrost, Stéphanie Valleau, Alán Aspuru-Guzik. 2012. Atomistic study of the long-lived quantum coherences in the Fenna-Matthews-Olson Complex. Biophysical Journal 102(3): 649–660. en_US
dc.identifier.issn 0006-3495 en_US
dc.identifier.issn 1542-0086 en_US
dc.description.abstract A remarkable amount of theoretical research has been carried out to elucidate the physical origins of the recently observed long-lived quantum coherence in the electronic energy transfer process in biological photosynthetic systems. Although successful in many respects, several widely used descriptions only include an effective treatment of the protein-chromophore interactions. In this work, by combining an all-atom molecular dynamics simulation, time-dependent density functional theory, and open quantum system approaches, we successfully simulate the dynamics of the electronic energy transfer of the Fenna-Matthews-Olson pigment-protein complex. The resulting characteristic beating of populations and quantum coherences is in good agreement with the experimental results and the hierarchy equation of motion approach. The experimental absorption, linear, and circular dichroism spectra and dephasing rates are recovered at two different temperatures. In addition, we provide an extension of our method to include zero-point fluctuations of the vibrational environment. This work thus presents, to our knowledge, one of the first steps to explain the role of excitonic quantum coherence in photosynthetic light-harvesting complexes based on their atomistic and molecular description. en_US
dc.description.sponsorship Chemistry and Chemical Biology en_US
dc.language.iso en_US en_US
dc.publisher Biophysical Society en_US
dc.relation.isversionof doi:10.1016/j.bpj.2011.12.021 en_US
dash.license LAA
dc.subject quantum physics en_US
dc.title Atomistic Study of the Long-Lived Quantum Coherences in the Fenna-Matthews-Olson Complex en_US
dc.type Journal Article en_US
dc.description.version Accepted Manuscript en_US
dc.relation.journal Biophysical Journal en_US Aspuru-Guzik, Alan
dash.waiver 2011-12-05 2012-03-14T18:01:23Z

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