Photosynthetic Energy Transfer: Missing in Action (Detected Spectroscopy)?

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388971%3A_____%2F24%3A00603229" target="_blank" >RIV/61388971:_____/24:00603229 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/00216208:11320/24:10491580

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/acs.jpclett.4c02665" target="_blank" >https://pubs.acs.org/doi/10.1021/acs.jpclett.4c02665</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpclett.4c02665" target="_blank" >10.1021/acs.jpclett.4c02665</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Photosynthetic Energy Transfer: Missing in Action (Detected Spectroscopy)?

Popis výsledku v původním jazyce

In recent years, action-detected ultrafast spectroscopies have gained popularity offering distinct advantages over their coherently detected counterparts, such as spatially resolved and operando measurements with high sensitivity. However, there are also fundamental limitations connected to the process of signal generation in action-detected experiments. Here we perform fluorescence-detected two-dimensional electronic spectroscopy (F-2DES) of the light-harvesting II (LH2) complex from purple bacteria. We demonstrate that the B800-B850 energy transfer process in LH2 is weak but observable in F-2DES, unlike in coherently detected 2DES where the energy transfer is visible with 100% contrast. We explain the weak signatures using a disordered excitonic model that accounts for experimental conditions. We further derive a general formula for the presence of excited-state signals in multichromophoric aggregates, dependent on the aggregate geometry, size, excitonic coupling and disorder. We find that the prominence of excited-state dynamics in action-detected spectroscopy offers a unique probe of excitonic delocalization in multichromophoric systems.

Název v anglickém jazyce

Photosynthetic Energy Transfer: Missing in Action (Detected Spectroscopy)?

Popis výsledku anglicky

In recent years, action-detected ultrafast spectroscopies have gained popularity offering distinct advantages over their coherently detected counterparts, such as spatially resolved and operando measurements with high sensitivity. However, there are also fundamental limitations connected to the process of signal generation in action-detected experiments. Here we perform fluorescence-detected two-dimensional electronic spectroscopy (F-2DES) of the light-harvesting II (LH2) complex from purple bacteria. We demonstrate that the B800-B850 energy transfer process in LH2 is weak but observable in F-2DES, unlike in coherently detected 2DES where the energy transfer is visible with 100% contrast. We explain the weak signatures using a disordered excitonic model that accounts for experimental conditions. We further derive a general formula for the presence of excited-state signals in multichromophoric aggregates, dependent on the aggregate geometry, size, excitonic coupling and disorder. We find that the prominence of excited-state dynamics in action-detected spectroscopy offers a unique probe of excitonic delocalization in multichromophoric systems.

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

2024

Kód důvěrnosti údajů

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

Název periodika

Journal of Physical Chemistry Letters

ISSN

1948-7185

e-ISSN

—

Svazek periodika

15

Číslo periodika v rámci svazku

50

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

11

Strana od-do

12376-12386

Kód UT WoS článku

001374184600001

EID výsledku v databázi Scopus

2-s2.0-85211633442