Exact description of excitonic dynamics in molecular aggregates weakly driven by light
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F20%3A10422754" target="_blank" >RIV/00216208:11320/20:10422754 - isvavai.cz</a>
Result on the web
<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=FNHiksvBpG" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=FNHiksvBpG</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1063/5.0029914" target="_blank" >10.1063/5.0029914</a>
Alternative languages
Result language
angličtina
Original language name
Exact description of excitonic dynamics in molecular aggregates weakly driven by light
Original language description
We 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 Forster theory. We also discuss the relation of our formalism to the combined Born-Markov-HEOM approaches in the case of excitation by thermal light.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)
Result continuities
Project
<a href="/en/project/GA18-18022S" target="_blank" >GA18-18022S: Graphene-based Biomimetic Light-Harvesting Systems</a><br>
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)
Others
Publication year
2020
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Journal of Chemical Physics
ISSN
0021-9606
e-ISSN
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Volume of the periodical
153
Issue of the periodical within the volume
24
Country of publishing house
US - UNITED STATES
Number of pages
17
Pages from-to
244122
UT code for WoS article
000605582600005
EID of the result in the Scopus database
2-s2.0-85099248219