Effect of the excitation pulse carrier frequency on the ultrafast charge recombination dynamics of donor-acceptor complexes: Stochastic simulations and experiments

Fedunov, Roman G.; Feskov, Serguei V.; Ivanov, Anatoly I.; Nicolet, Olivier; Pages, Stéphane; Vauthey, Eric

doi:10.1063/1.1772362

Scientific article

English

Effect of the excitation pulse carrier frequency on the ultrafast charge recombination dynamics of donor-acceptor complexes: Stochastic simulations and experiments

Contributors

Fedunov, Roman G.; Feskov, Serguei V.; Ivanov, Anatoly I.; Nicolet, Olivier; Pages, Stéphane; Vauthey, Eric

Published in

The Journal of chemical physics, vol. 121, no. 8, p. 3643-3656

Publication date

2004

Abstract

The influence of the excitation pulse carrier frequency on the ultrafast charge recombination dynamics of excited donor-acceptor complexes has been explored both theoretically and experimentally. The theoretical description involves the explicit treatment of both the optical formation of the nuclear wave packet on the excited free energy surface and its ensuing dynamics. The wave packet motion and the electronic transition are described within the framework of the stochastic point-transition approach. It is shown that the variation of the pulse carrier frequency within the absorption band can significantly change the effective charge recombination dynamics. The mechanism of this phenomenon is analyzed and a semiquantitative interpretation is suggested. The role of the vibrational coherence in the recombination dynamics is discussed. An experimental investigation of the ultrafast charge recombination dynamics of two donor-acceptor complexes in valeronitrile also is presented. The decays of the excited state population were found to be highly nonexponential, the degree of non-exponentiality depending on the excitation frequency. For one complex, the charge recombination dynamics was found to slow down upon increasing the excitation frequency, while the opposite behavior was observed with the other complex. These experimental observations follow qualitatively the predictions of the simulations.

UNIGE affiliation entities

Faculté des sciences / Section de chimie et biochimie / Département de chimie physique

UNIGE research groups

Groupe Vauthey

Citation (ISO format)

FEDUNOV, Roman G. et al. Effect of the excitation pulse carrier frequency on the ultrafast charge recombination dynamics of donor-acceptor complexes: Stochastic simulations and experiments. In: The Journal of chemical physics, 2004, vol. 121, n° 8, p. 3643–3656. doi: 10.1063/1.1772362

Article (Published version)

Identifiers

PID : unige:3616
DOI : 10.1063/1.1772362

Journal ISSN

0021-9606

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Creation

02/10/2009 15:18:56

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02/10/2009 15:18:56

Update

14/03/2023 15:15:39

Status update

14/03/2023 15:15:39

Last indexation

10/06/2025 21:30:56

Effect of the excitation pulse carrier frequency on the ultrafast charge recombination dynamics of donor-acceptor complexes: Stochastic simulations and experiments

Contributors

Published in

Publication date

Abstract

UNIGE affiliation entities

UNIGE research groups

Citation (ISO format)

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Journal ISSN

Technical informations

Creation

First validation

Update

Status update

Last indexation