Nonequilibrium steady-state picture of incoherent light-induced excitation harvesting

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dc.citation.issue24
dc.citation.rankM21
dc.citation.spage244110
dc.citation.volume153
dc.contributor.authorJanković, Veljko
dc.contributor.authorMančal, Tomáš
dc.date.accessioned2024-06-14T11:07:48Z
dc.date.available2024-06-14T11:07:48Z
dc.date.issued2020-12-28
dc.description.abstractWe formulate a comprehensive theoretical description of excitation harvesting in molecular aggregates photoexcited by weak incoherent radiation. An efficient numerical scheme that respects the continuity equation for excitation fluxes is developed to compute the nonequilibrium steady state (NESS) arising from the interplay between excitation generation, excitation relaxation, dephasing, trapping at the load, and recombination. The NESS is most conveniently described in the so-called preferred basis in which the steady-state excitonic density matrix is diagonal. The NESS properties are examined by relating the preferred-basis description to the descriptions in the site or excitonic bases. Focusing on a model photosynthetic dimer, we find that the NESS in the limit of long trapping time is quite similar to the excited-state equilibrium in which the stationary coherences originate from the excitation–environment entanglement. For shorter trapping times, we demonstrate how the properties of the NESS can be extracted from the time-dependent description of an incoherently driven but unloaded dimer. This relation between stationary and time-dependent pictures is valid, provided that the trapping time is longer than the decay time of dynamic coherences accessible in femtosecond spectroscopy experiments.
dc.identifier.doi10.1063/5.0029918
dc.identifier.issn0021-9606
dc.identifier.issn1089-7690
dc.identifier.scopus2-s2.0-85099188554
dc.identifier.urihttps://pub.ipb.ac.rs/handle/123456789/102
dc.identifier.wos000603068300010
dc.language.isoen
dc.publisherAmerican Institute of Physics Inc.
dc.relation.ispartofThe Journal of Chemical Physics
dc.relation.ispartofabbrJ. Chem. Phys.
dc.rightsrestrictedAccess
dc.titleNonequilibrium steady-state picture of incoherent light-induced excitation harvesting
dc.typeArticle
dc.type.versionpublishedVersion
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