Exact description of excitonic dynamics in molecular aggregates weakly driven by light

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dc.citation.issue24
dc.citation.rankM21
dc.citation.spage244122
dc.citation.volume153
dc.contributor.authorJanković, Veljko
dc.contributor.authorMančal, Tomáš
dc.date.accessioned2024-06-14T10:46:38Z
dc.date.available2024-06-14T10:46:38Z
dc.date.issued2020-12-29
dc.description.abstractWe present a rigorous theoretical description of excitonic dynamics in molecular light-harvesting aggregates photoexcited by weak-intensity radiation of arbitrary properties. While the interaction with light is included up to the second order, the treatment of the excitation–environment coupling is exact and results in an exact expression for the reduced excitonic density matrix that is manifestly related to the spectroscopic picture of the photoexcitation process. This expression takes fully into account the environmental reorganization processes triggered by the two interactions with light. This is particularly important for slow environments and/or strong excitation–environment coupling. Within the exponential decomposition scheme, we demonstrate how our result can be recast as the hierarchy of equations of motion (HEOM) that explicitly and consistently includes the photoexcitation step. We analytically describe the environmental reorganization dynamics triggered by a delta-like excitation of a single chromophore and demonstrate how our HEOM, in appropriate limits, reduces to the Redfield equations comprising a pulsed photoexcitation and the nonequilibrium Förster theory. We also discuss the relation of our formalism to the combined Born–Markov–HEOM approaches in the case of excitation by thermal light.
dc.identifier.doi10.1063/5.0029914
dc.identifier.issn0021-9606
dc.identifier.issn1089-7690
dc.identifier.scopus2-s2.0-85099248219
dc.identifier.urihttps://pub.ipb.ac.rs/handle/123456789/101
dc.identifier.wos000605582600005
dc.language.isoen
dc.publisherAmerican Institute of Physics Inc.
dc.relation.ispartofThe Journal of Chemical Physics
dc.relation.ispartofabbrJ. Chem. Phys.
dc.rightsrestrictedAccess
dc.titleExact description of excitonic dynamics in molecular aggregates weakly driven by light
dc.typeArticle
dc.type.versionpublishedVersion
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