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  • The Thirteenth International Conference on Ultrafast Phenomena
  • 2002 OSA Technical Digest Series (Optica Publishing Group, 2002),
  • paper ME25
  • https://doi.org/10.1364/UP.2002.ME25

Molecular Mechanisms for Photodetachment in Water

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Abstract

Threshold electron ejection processes, such as photodetachment via optical charge-transfer-to-solvent (CTTS) excitation, provide very simple models for understanding solvent-controlled electron transfer (ET). In previous work, we have demonstrated that ejection from the prototypical CTTS system, the aqueous iodide anion, is to short range into a caged pair [1]. The electron subsequently either diffuses out of the cage, an activated process due to the attractive interaction between the nascent electron and the polarizable iodine neutral, or undergoes reverse electron transfer to reform I [2]. In the current experiments, our goal was to gain additional insight into the molecular mechanism of ejection by exploring the effect of a large increase in the excitation energy and by isotopic substitution of the solvent. The results are rather unexpected and an ab initio characterization of the vertically prepared bulk CTTS wavefunction turns out to be particularly useful in rationalizing the dynamics of the electron.

© 2002 Optical Society of America

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