2026-04-13T15:21:39Zhttps://recercat.cat/oai/request

oai:recercat.cat:2445/1757382025-12-05T14:11:29Zcom_2072_1057col_2072_478815col_2072_478917

Spatial and Electronic Correlations in the PE545 Light-Harvesting Complex Viani, Lucas Curutchet Barat, Carles E. Mennucci, Benedetta Llum Fluorescència Química quàntica Química física Light Fluorescence Quantum chemistry Physical and theoretical chemistry The recent discovery of long-lasting quantum coherence effects in photosynthetic pigment-protein complexes has challenged our view of the role that protein motions play in light-harvesting processes. Several groups have suggested that correlated fluctuations involving the pigments site energies and couplings could be at the origin of such unexpected behavior. Here we combine molecular dynamics simulations with quantum mechanics/molecular mechanics calculations to analyze the degree of correlated fluctuations in the PE545 complex of Rhodomonas sp. strain CS24. We find that correlations between the motions of the chromophores, which are significantly assisted by the water solvent, do not translate into appreciable site energy correlations but do lead to significant cross-correlations of energies and couplings. Such behavior, not observed in a recent study on the Fenna-Mathews-Olson complex, seems to provide phycobiliproteins with an additional fundamental mechanism to control quantum coherence and light-harvesting efficiency compared with chlorophyll-containing complexes. 2021-03-25T08:59:04Z 2021-03-25T08:59:04Z 2013-02-07 2021-03-25T08:59:04Z info:eu-repo/semantics/article info:eu-repo/semantics/acceptedVersion Versió postprint del document publicat a: http://dx.doi.org/10.1021/jz301987u Journal of Physical Chemistry Letters, 2013, vol. 4, num. 3, p. 372-377 info:eu-repo/grantAgreement/EC/FP7/277755/EU//ENLIGHT (c) American Chemical Society , 2013 info:eu-repo/semantics/openAccess American Chemical Society Articles publicats en revistes (Farmàcia, Tecnologia Farmacèutica i Fisicoquímica)