Vibronic coupling explains the ultrafast cartotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F15%3A10316374" target="_blank" >RIV/00216208:11320/15:10316374 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1063/1.4919548" target="_blank" >http://dx.doi.org/10.1063/1.4919548</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1063/1.4919548" target="_blank" >10.1063/1.4919548</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Vibronic coupling explains the ultrafast cartotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

Popis výsledku v původním jazyce

The initial energy transfer in photosynthesis occurs between the light-harvesting pigments and on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which leads to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited state as part of the systems Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels

Název v anglickém jazyce

Vibronic coupling explains the ultrafast cartotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

Popis výsledku anglicky

The initial energy transfer in photosynthesis occurs between the light-harvesting pigments and on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which leads to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited state as part of the systems Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels

Druh

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

CEP obor

BO - Biofyzika

OECD FORD obor

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Projekt

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)<br>S - Specificky vyzkum na vysokych skolach<br>I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2015

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

2015

Číslo periodika v rámci svazku

142

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

15

Strana od-do

1-15

Kód UT WoS článku

000355931800038

EID výsledku v databázi Scopus

2-s2.0-84928974836