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Scientific article
English

Driving Force Dependence of Charge Recombination in Reactive and Nonreactive Solvents

Published inThe journal of physical chemistry. A, vol. 116, no. 38, p. 9473-9483
Errata
  • "We noticed a few errors and typos in some of the equations in our article. All calculations and simulations have been performed with the correct equations (as outlined in this correction), and therefore, these errors have no consequences on the discussion of the results and the conclusions."
  • DOI : 10.1021/jp4047825
Publication date2012
Abstract

This study addresses the free energy dependence of charge recombination following photoinduced bimolecular electron transfer in three different solvents of either inert (acetonitrile and benzyl acetate) or reactive (N,N-dimethylaniline) character. Femtosecond time-resolved fluorescence and transient absorption have been used to determine the time scales for charge recombination. In pure N,N-dimethylaniline, charge recombination is found to be substantially slower than charge separation in a range of driving forces covering 1.5 eV. In all three solvents, the so-called Marcus inverted region is clearly observed for charge recombination. Additionally, the charge recombination step is found to be influenced by the solvent relaxation dynamics. A diffusion-reaction equation approach using an electron transfer model accounting for solvent relaxation is used to rationalize the experimental results.

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Citation (ISO format)
ROSSPEINTNER, Arnulf, ANGULO, Gonzalo, VAUTHEY, Eric. Driving Force Dependence of Charge Recombination in Reactive and Nonreactive Solvents. In: The journal of physical chemistry. A, 2012, vol. 116, n° 38, p. 9473–9483. doi: 10.1021/jp306629v
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ISSN of the journal1089-5639
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Creation09/28/2012 8:18:00 AM
First validation09/28/2012 8:18:00 AM
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