Equilibration Dependence of Fucoxanthin S-1 and ICT Signatures on Polarity, Proticity, and Temperature by Multipulse Femtosecond Absorption Spectroscopy

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60076658%3A12310%2F18%3A43897245" target="_blank" >RIV/60076658:12310/18:43897245 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/60077344:_____/18:00495163

Výsledek na webu

<a href="https://pubs.acs.org/doi/pdf/10.1021/acs.jpcb.8b04217" target="_blank" >https://pubs.acs.org/doi/pdf/10.1021/acs.jpcb.8b04217</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpcb.8b04217" target="_blank" >10.1021/acs.jpcb.8b04217</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Equilibration Dependence of Fucoxanthin S-1 and ICT Signatures on Polarity, Proticity, and Temperature by Multipulse Femtosecond Absorption Spectroscopy

Popis výsledku v původním jazyce

To demonstrate the value of the multipulse method in revealing the nature of coupling between excited states and explore the environmental dependencies of lowest excited singlet state (S-1) and intramolecular charge transfer (ICT) state equilibration, we performed ultrafast transient absorption pump-dump-probe and pump-repump -probe spectroscopies on fucoxanthin in various solvent conditions. The effects of polarity, proticity, and temperature were tested in solvents methanol at 293 and 190 K, acetonitrile, and isopropanol. We show that manipulation of the kinetic traces can produce one trace reflecting the equilibration kinetics of the states, which reveals that lower polarity, proticity, and temperature delay S-1/ICT equilibration. On the basis of a two-state model representing the S-1 and ICT states on the same S-1/ICT potential energy surface, we were able to show that the kinetics are strictly dependent on the initial relative populations of the states as well as the decay of the ICT state to the ground state. Informed by global analysis, a systematic method for target analysis based on this model allowed us to quantify the population transfer rates throughout the life of the S-1/ICT state as well as separate the S-1 and ICT spectral signatures. The results are consistent with the concept that the S-1 and ICT states are part of one potential energy surface.

Název v anglickém jazyce

Equilibration Dependence of Fucoxanthin S-1 and ICT Signatures on Polarity, Proticity, and Temperature by Multipulse Femtosecond Absorption Spectroscopy

Popis výsledku anglicky

To demonstrate the value of the multipulse method in revealing the nature of coupling between excited states and explore the environmental dependencies of lowest excited singlet state (S-1) and intramolecular charge transfer (ICT) state equilibration, we performed ultrafast transient absorption pump-dump-probe and pump-repump -probe spectroscopies on fucoxanthin in various solvent conditions. The effects of polarity, proticity, and temperature were tested in solvents methanol at 293 and 190 K, acetonitrile, and isopropanol. We show that manipulation of the kinetic traces can produce one trace reflecting the equilibration kinetics of the states, which reveals that lower polarity, proticity, and temperature delay S-1/ICT equilibration. On the basis of a two-state model representing the S-1 and ICT states on the same S-1/ICT potential energy surface, we were able to show that the kinetics are strictly dependent on the initial relative populations of the states as well as the decay of the ICT state to the ground state. Informed by global analysis, a systematic method for target analysis based on this model allowed us to quantify the population transfer rates throughout the life of the S-1/ICT state as well as separate the S-1 and ICT spectral signatures. The results are consistent with the concept that the S-1 and ICT states are part of one potential energy surface.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/GA16-10417S" target="_blank" >GA16-10417S: Světlosběrné a fotoprotektivní funkce karotenoidů - nové přístupy pomocí multipulsní femtosekundové spektroskopie</a><br>

Návaznosti

S - Specificky vyzkum na vysokych skolach<br>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

Journal of Physical Chemistry B

ISSN

1520-6106

e-ISSN

—

Svazek periodika

122

Číslo periodika v rámci svazku

29

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

13

Strana od-do

7264-7276

Kód UT WoS článku

000440519900007

EID výsledku v databázi Scopus

2-s2.0-85049644861