Self-consistent approach to the dynamics of excitation energy transfer in multichromophoric systems

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F24%3A10494625" target="_blank" >RIV/00216208:11320/24:10494625 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=gBz35FEg8K" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=gBz35FEg8K</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1063/5.0237483" target="_blank" >10.1063/5.0237483</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Self-consistent approach to the dynamics of excitation energy transfer in multichromophoric systems

Popis výsledku v původním jazyce

Computationally tractable and reliable, albeit approximate, methods for studying exciton transport in molecular aggregates immersed in structured bosonic environments have been actively developed. Going beyond the lowest-order (Born) approximation for the memory kernel of the quantum master equation typically results in complicated and possibly divergent expressions. Starting from the memory kernel in the Born approximation, and recognizing the quantum master equation as the Dyson equation of Green&apos;s functions theory, we formulate the self-consistent Born approximation to resum the memory-kernel perturbation series in powers of the exciton-environment interaction. Our formulation is in the Liouville space and frequency domain and handles arbitrary exciton-environment spectral densities. In a molecular dimer coupled to an overdamped oscillator environment, we conclude that the self-consistent cycle significantly improves the Born-approximation energy-transfer dynamics. The dynamics in the self-consistent Born approximation agree well with the solutions of hierarchical equations of motion over a wide range of parameters, including the most challenging regimes of strong exciton-environment interactions, slow environments, and low temperatures. This is rationalized by the analytical considerations of coherence-dephasing dynamics in the pure-dephasing model. We find that the self-consistent Born approximation is good (poor) at describing energy transfer modulated by an underdamped vibration resonant (off-resonant) with the exciton energy gap. Nevertheless, it reasonably describes exciton dynamics in the seven-site model of the Fenna-Matthews-Olson complex in a realistic environment comprising both an overdamped continuum and underdamped vibrations.

Název v anglickém jazyce

Self-consistent approach to the dynamics of excitation energy transfer in multichromophoric systems

Popis výsledku anglicky

Computationally tractable and reliable, albeit approximate, methods for studying exciton transport in molecular aggregates immersed in structured bosonic environments have been actively developed. Going beyond the lowest-order (Born) approximation for the memory kernel of the quantum master equation typically results in complicated and possibly divergent expressions. Starting from the memory kernel in the Born approximation, and recognizing the quantum master equation as the Dyson equation of Green&apos;s functions theory, we formulate the self-consistent Born approximation to resum the memory-kernel perturbation series in powers of the exciton-environment interaction. Our formulation is in the Liouville space and frequency domain and handles arbitrary exciton-environment spectral densities. In a molecular dimer coupled to an overdamped oscillator environment, we conclude that the self-consistent cycle significantly improves the Born-approximation energy-transfer dynamics. The dynamics in the self-consistent Born approximation agree well with the solutions of hierarchical equations of motion over a wide range of parameters, including the most challenging regimes of strong exciton-environment interactions, slow environments, and low temperatures. This is rationalized by the analytical considerations of coherence-dephasing dynamics in the pure-dephasing model. We find that the self-consistent Born approximation is good (poor) at describing energy transfer modulated by an underdamped vibration resonant (off-resonant) with the exciton energy gap. Nevertheless, it reasonably describes exciton dynamics in the seven-site model of the Fenna-Matthews-Olson complex in a realistic environment comprising both an overdamped continuum and underdamped vibrations.

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/GA22-26376S" target="_blank" >GA22-26376S: Intramolekulární vibrační módy jako strukturální sondy a dynamické modulátory biologických a bio-inspirovaných nanostruktur</a><br>

Návaznosti

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

Rok uplatnění

2024

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

1089-7690

Svazek periodika

161

Číslo periodika v rámci svazku

20

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

21

Strana od-do

204108

Kód UT WoS článku

001364193300006

EID výsledku v databázi Scopus

2-s2.0-85210294543