Estimation of damped oscillation associated spectra from ultrafast transient absorption spectra

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F16%3A10364740" target="_blank" >RIV/00216208:11320/16:10364740 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1063/1.4966196" target="_blank" >http://dx.doi.org/10.1063/1.4966196</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1063/1.4966196" target="_blank" >10.1063/1.4966196</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Estimation of damped oscillation associated spectra from ultrafast transient absorption spectra

Popis výsledku v původním jazyce

When exciting a complex molecular system with a short optical pulse, all chromophores present in the system can be excited. The resulting superposition of electronically and vibrationally excited states evolves in time, which is monitored with transient absorption spectroscopy. We present a methodology to resolve simultaneously the contributions of the different electronically and vibrationally excited states from the complete data. The evolution of the excited states is described with a superposition of damped oscillations. The amplitude of a damped oscillation cos(omega(n)t) exp(-gamma(n)t) as a function of the detection wavelength constitutes a damped oscillation associated spectrum DOAS(n)(lambda) with an accompanying phase characteristic phi(n)(lambda). In a case study, the cryptophyte photosynthetic antenna complex PC612 which contains eight bilin chromophores was excited by a broadband optical pulse. Difference absorption spectra from 525 to 715 nm were measured until 1 ns. The population dynamics is described by four lifetimes, with interchromophore equilibration in 0.8 and 7.5 ps. We have resolved 24 DOAS with frequencies between 130 and 1649 cm(-1) and with damping rates between 0.9 and 12 ps(-1). In addition, 11 more DOAS with faster damping rates were necessary to describe the &quot;coherent artefact.&quot; The DOAS contains both ground and excited state features. Their interpretation is aided by DOAS analysis of simulated transient absorption signals resulting from stimulated emission and ground state bleach. (C) 2016 Author(s).

Název v anglickém jazyce

Estimation of damped oscillation associated spectra from ultrafast transient absorption spectra

Popis výsledku anglicky

When exciting a complex molecular system with a short optical pulse, all chromophores present in the system can be excited. The resulting superposition of electronically and vibrationally excited states evolves in time, which is monitored with transient absorption spectroscopy. We present a methodology to resolve simultaneously the contributions of the different electronically and vibrationally excited states from the complete data. The evolution of the excited states is described with a superposition of damped oscillations. The amplitude of a damped oscillation cos(omega(n)t) exp(-gamma(n)t) as a function of the detection wavelength constitutes a damped oscillation associated spectrum DOAS(n)(lambda) with an accompanying phase characteristic phi(n)(lambda). In a case study, the cryptophyte photosynthetic antenna complex PC612 which contains eight bilin chromophores was excited by a broadband optical pulse. Difference absorption spectra from 525 to 715 nm were measured until 1 ns. The population dynamics is described by four lifetimes, with interchromophore equilibration in 0.8 and 7.5 ps. We have resolved 24 DOAS with frequencies between 130 and 1649 cm(-1) and with damping rates between 0.9 and 12 ps(-1). In addition, 11 more DOAS with faster damping rates were necessary to describe the &quot;coherent artefact.&quot; The DOAS contains both ground and excited state features. Their interpretation is aided by DOAS analysis of simulated transient absorption signals resulting from stimulated emission and ground state bleach. (C) 2016 Author(s).

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10300 - Physical sciences

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2016

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

145

Číslo periodika v rámci svazku

17

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

12

Strana od-do

—

Kód UT WoS článku

000388105100017

EID výsledku v databázi Scopus

2-s2.0-84994251911