Ultrafast energy transfer with competing channels: Non-equilibrium Forster and Modified Redfield theories

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F17%3A10370638" target="_blank" >RIV/00216208:11320/17:10370638 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1063/1.4981523" target="_blank" >http://dx.doi.org/10.1063/1.4981523</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1063/1.4981523" target="_blank" >10.1063/1.4981523</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Ultrafast energy transfer with competing channels: Non-equilibrium Forster and Modified Redfield theories

Popis výsledku v původním jazyce

We derive equations of motion for the reduced density matrix of a molecular system which undergoes energy transfer dynamics competing with fast internal conversion channels. Environmental degrees of freedom of such a system have no time to relax to quasi-equilibrium in the electronic excited state of the donor molecule, and thus the conditions of validity of Forster and Modified Redfield theories in their standard formulations do not apply. We derive non-equilibrium versions of the two well-known rate theories and apply them to the case of carotenoid-chlorophyll energy transfer. Although our reduced density matrix approach does not account for the formation of vibronic excitons, it still confirms the important role of the donor ground-state vibrational states in establishing the resonance energy transfer conditions. We show that it is essential to work with a theory valid in a strong system-bath interaction regime to obtain correct dependence of the rates on donor-acceptor energy gap. Published by AIP Publishing.

Název v anglickém jazyce

Ultrafast energy transfer with competing channels: Non-equilibrium Forster and Modified Redfield theories

Popis výsledku anglicky

We derive equations of motion for the reduced density matrix of a molecular system which undergoes energy transfer dynamics competing with fast internal conversion channels. Environmental degrees of freedom of such a system have no time to relax to quasi-equilibrium in the electronic excited state of the donor molecule, and thus the conditions of validity of Forster and Modified Redfield theories in their standard formulations do not apply. We derive non-equilibrium versions of the two well-known rate theories and apply them to the case of carotenoid-chlorophyll energy transfer. Although our reduced density matrix approach does not account for the formation of vibronic excitons, it still confirms the important role of the donor ground-state vibrational states in establishing the resonance energy transfer conditions. We show that it is essential to work with a theory valid in a strong system-bath interaction regime to obtain correct dependence of the rates on donor-acceptor energy gap. Published by AIP Publishing.

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/GA14-25752S" target="_blank" >GA14-25752S: Mikroskopické enviromentální determinanty a samoregulace přenosu energie ve fotosyntéze</a><br>

Návaznosti

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

Rok uplatnění

2017

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

146

Číslo periodika v rámci svazku

17

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

12

Strana od-do

—

Kód UT WoS článku

000400625800010

EID výsledku v databázi Scopus

2-s2.0-85018977815