Optical spectroscopy and system-bath interactions in molecular aggregates with full configuration interaction Frenkel exciton model

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F16%3A10333734" target="_blank" >RIV/00216208:11320/16:10333734 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1016/j.chemphys.2016.08.017" target="_blank" >http://dx.doi.org/10.1016/j.chemphys.2016.08.017</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.chemphys.2016.08.017" target="_blank" >10.1016/j.chemphys.2016.08.017</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Optical spectroscopy and system-bath interactions in molecular aggregates with full configuration interaction Frenkel exciton model

Popis výsledku v původním jazyce

Standard application of the Frenkel exciton model neglects resonance coupling between collective molecular aggregate states with different number of excitations. These inter-band coupling terms are, however, of the same magnitude as the intra-band coupling between singly excited states. We systematically derive the Frenkel exciton model from quantum chemical considerations, and identify it as a variant of the configuration interaction method. We discuss all non-negligible couplings between collective aggregate states, and provide compact formulae for their calculation. We calculate absorption spectra of molecular aggregate of carotenoids and identify significant band shifts as a result of inter-band coupling. The presence of inter-band coupling terms requires renormalization of the system-bath coupling with respect to standard formulation, but renormalization effects are found to be weak. We present detailed discussion of molecular dimer and calculate its time-resolved two-dimensional Fourier transformed spectra to find weak but noticeable effects of peak amplitude redistribution due to inter-band coupling. (C) 2016 Published by Elsevier B.V.

Název v anglickém jazyce

Optical spectroscopy and system-bath interactions in molecular aggregates with full configuration interaction Frenkel exciton model

Popis výsledku anglicky

Standard application of the Frenkel exciton model neglects resonance coupling between collective molecular aggregate states with different number of excitations. These inter-band coupling terms are, however, of the same magnitude as the intra-band coupling between singly excited states. We systematically derive the Frenkel exciton model from quantum chemical considerations, and identify it as a variant of the configuration interaction method. We discuss all non-negligible couplings between collective aggregate states, and provide compact formulae for their calculation. We calculate absorption spectra of molecular aggregate of carotenoids and identify significant band shifts as a result of inter-band coupling. The presence of inter-band coupling terms requires renormalization of the system-bath coupling with respect to standard formulation, but renormalization effects are found to be weak. We present detailed discussion of molecular dimer and calculate its time-resolved two-dimensional Fourier transformed spectra to find weak but noticeable effects of peak amplitude redistribution due to inter-band coupling. (C) 2016 Published by Elsevier B.V.

Druh

J_x - Nezařazeno - Článek v odborném periodiku (Jimp, Jsc a Jost)

CEP obor

CF - Fyzikální chemie a teoretická chemie

OECD FORD obor

—

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

2016

Kód důvěrnosti údajů

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

Název periodika

Chemical Physics

ISSN

0301-0104

e-ISSN

—

Svazek periodika

481

Číslo periodika v rámci svazku

Neuveden

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

13

Strana od-do

218-230

Kód UT WoS článku

000389589700027

EID výsledku v databázi Scopus

2-s2.0-84995538951