Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60076658%3A12310%2F18%3A43897572" target="_blank" >RIV/60076658:12310/18:43897572 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/60077344:_____/18:00492932 RIV/61389021:_____/18:00492932

Výsledek na webu

<a href="https://www.nature.com/articles/s41557-018-0060-5" target="_blank" >https://www.nature.com/articles/s41557-018-0060-5</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1038/s41557-018-0060-5" target="_blank" >10.1038/s41557-018-0060-5</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex

Popis výsledku v původním jazyce

The idea that excitonic (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when slowly dephasing quantum beats (QBs) were observed in the two-dimensional electronic spectra of the Fenna-Matthews-Olson (FMO) complex at 77 K. These were assigned to superpositions of excitonic states, a controversial interpretation, as the strong chromophore-environment interactions in the complex suggest fast dephasing. Although it has been pointed out that vibrational motion produces similar spectral signatures, a concrete assignment of these oscillatory signals to distinct physical processes is still lacking. Here we revisit the coherence dynamics of the FMO complex using polarization-controlled two-dimensional electronic spectroscopy, supported by theoretical modelling. We show that the long-lived QBs are exclusively vibrational in origin, whereas the dephasing of the electronic coherences is completed within 240 fs even at 77 K. We further find that specific vibrational coherences are produced via vibronically coupled excited states. The presence of such states suggests that vibronic coupling is relevant for photosynthetic energy transfer.

Název v anglickém jazyce

Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex

Popis výsledku anglicky

The idea that excitonic (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when slowly dephasing quantum beats (QBs) were observed in the two-dimensional electronic spectra of the Fenna-Matthews-Olson (FMO) complex at 77 K. These were assigned to superpositions of excitonic states, a controversial interpretation, as the strong chromophore-environment interactions in the complex suggest fast dephasing. Although it has been pointed out that vibrational motion produces similar spectral signatures, a concrete assignment of these oscillatory signals to distinct physical processes is still lacking. Here we revisit the coherence dynamics of the FMO complex using polarization-controlled two-dimensional electronic spectroscopy, supported by theoretical modelling. We show that the long-lived QBs are exclusively vibrational in origin, whereas the dephasing of the electronic coherences is completed within 240 fs even at 77 K. We further find that specific vibrational coherences are produced via vibronically coupled excited states. The presence of such states suggests that vibronic coupling is relevant for photosynthetic energy transfer.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10306 - Optics (including laser optics and quantum optics)

Projekt

<a href="/cs/project/GBP501%2F12%2FG055" target="_blank" >GBP501/12/G055: Centrum fotosyntetického výzkumu</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2018

Kód důvěrnosti údajů

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

Název periodika

Nature Chemistry

ISSN

1755-4330

e-ISSN

—

Svazek periodika

10

Číslo periodika v rámci svazku

7

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

7

Strana od-do

780-786

Kód UT WoS článku

000436103200017

EID výsledku v databázi Scopus

2-s2.0-85047222958