title: Lindblad equations for strongly coupled populations and coherences in photosynthetic complexes.
abstract: Recent experimental observations of time-resolved multidimensional signals in the light-harvesting antennae Fenna-Mathews-Olson [G. S. Engel et al., Nature (London) 446, 782 (2007)] show large oscillations of exciton populations coupled to the long-lived coherences. These effects may not be reproduced by the standard Redfield theory which assumes weak coupling to a bath. A more general relaxation superoperator which holds for all system-bath coupling parameter regimes is constructed by taking into account the statistics (covariances) of Lindblad equation parameters. Simulations for a model dimer reproduce all observed strong coupling effects.
authors.affiliation: Department of Chemistry, University of California, Irvine, California 92697-2025, USA.
authors.forename: Benoit
authors.initials: B
authors.lastname: Palmieri
authors.forename: Darius
authors.initials: D
authors.lastname: Abramavicius
authors.forename: Shaul
authors.initials: S
authors.lastname: Mukamel
mesh_terms: D041883:Chlorobium / Q000378:metabolism; D008027:Light; D008956:Models, Chemical; D008958:Models, Molecular; D010788:Photosynthesis / Q000502:physiology*; D045322:Photosynthetic Reaction Center Complex Proteins; D010789:Phototherapy; D055585:Physical Phenomena; D011789:Quantum Theory; D013816:Thermodynamics
chemical_list: D045322:Photosynthetic Reaction Center Complex Proteins