Fluorescence-Detected Wavepacket Interferometry Reveals Time-Varying Exciton Relaxation Pathways in Single Light-Harvesting Complexes

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388971%3A_____%2F25%3A00641316" target="_blank" >RIV/61388971:_____/25:00641316 - isvavai.cz</a>

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/jacs.5c12416" target="_blank" >https://pubs.acs.org/doi/10.1021/jacs.5c12416</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/jacs.5c12416" target="_blank" >10.1021/jacs.5c12416</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Fluorescence-Detected Wavepacket Interferometry Reveals Time-Varying Exciton Relaxation Pathways in Single Light-Harvesting Complexes

Popis výsledku v původním jazyce

Photosynthesis relies on efficient energy relaxation within the excited-state manifold of pigment-protein complexes. Since the protein scaffold is rather flexible, the resulting energetic and structural disorder gives rise to a complex excited-state energy level structure that fluctuates on all time scales. Although the impact of such fluctuations on relaxation processes is known, the precise exciton states involved in relaxation as well as the nature of the vibrational modes driving relaxation are under debate. Here, single pigment-protein complexes from a photosynthetic purple bacterium are excited with two identical ultrashort phase-locked pulses, producing two exciton wave packets that can interfere. This leads to a modulation of the emission intensity as a function of the delay time between the pulses that fades out within about approximate to 100 fs due to fluctuating environments on those time scales. For several single complexes, we find variations in the interference patterns on a time scale of several tens of seconds that reveal fluctuations in the energy relaxation pathways toward the lowest-energy exciton states. This relaxation is driven by temporal variations in the coupling between electronic excitations and low-frequency vibrational modes.

Název v anglickém jazyce

Fluorescence-Detected Wavepacket Interferometry Reveals Time-Varying Exciton Relaxation Pathways in Single Light-Harvesting Complexes

Popis výsledku anglicky

Photosynthesis relies on efficient energy relaxation within the excited-state manifold of pigment-protein complexes. Since the protein scaffold is rather flexible, the resulting energetic and structural disorder gives rise to a complex excited-state energy level structure that fluctuates on all time scales. Although the impact of such fluctuations on relaxation processes is known, the precise exciton states involved in relaxation as well as the nature of the vibrational modes driving relaxation are under debate. Here, single pigment-protein complexes from a photosynthetic purple bacterium are excited with two identical ultrashort phase-locked pulses, producing two exciton wave packets that can interfere. This leads to a modulation of the emission intensity as a function of the delay time between the pulses that fades out within about approximate to 100 fs due to fluctuating environments on those time scales. For several single complexes, we find variations in the interference patterns on a time scale of several tens of seconds that reveal fluctuations in the energy relaxation pathways toward the lowest-energy exciton states. This relaxation is driven by temporal variations in the coupling between electronic excitations and low-frequency vibrational modes.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10606 - Microbiology

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

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

Název periodika

Journal of the American Chemical Society

ISSN

0002-7863

e-ISSN

1520-5126

Svazek periodika

147

Číslo periodika v rámci svazku

44

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

10

Strana od-do

40537-40546

Kód UT WoS článku

001597399400001

EID výsledku v databázi Scopus

2-s2.0-105020674063