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

Result code in 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>

Result on the web

<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>

Result language

angličtina

Original language name

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

Original language description

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.

Czech name

—

Czech description

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Type

J_imp - Article in a specialist periodical, which is included in the Web of Science database

CEP classification

—

OECD FORD branch

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

Project

<a href="/en/project/GA22-26376S" target="_blank" >GA22-26376S: Intramolecular vibrational modes as structural probes and dynamic modulators of biological and bio-inspired nano-structures</a><br>

Continuities

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

Publication year

2024

Confidentiality

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

Name of the periodical

Journal of Chemical Physics

ISSN

0021-9606

e-ISSN

1089-7690

Volume of the periodical

161

Issue of the periodical within the volume

20

Country of publishing house

US - UNITED STATES

Number of pages

21

Pages from-to

204108

UT code for WoS article

001364193300006

EID of the result in the Scopus database

2-s2.0-85210294543