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

Kód výsledku v 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>

Výsledek na webu

<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>

Jazyk výsledku

angličtina

Název v původním jazyce

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

Popis výsledku v původním jazyce

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.

Název v anglickém jazyce

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

Popis výsledku anglicky

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.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Projekt

<a href="/cs/project/GA18-18022S" target="_blank" >GA18-18022S: Bioinspirované světlosběrné systémy na bázi grafenu</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2020

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Chemical Physics

ISSN

0021-9606

e-ISSN

—

Svazek periodika

153

Číslo periodika v rámci svazku

24

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

17

Strana od-do

244122

Kód UT WoS článku

000605582600005

EID výsledku v databázi Scopus

2-s2.0-85099248219