Real-time observation of the charge-transfer-to-solvent dynamics

Messina, Fabrizio; Bräm, Oliver; Cannizzo, Andrea; Chergui, Majed (2013). Real-time observation of the charge-transfer-to-solvent dynamics. Nature communications, 4(1) Nature Publishing Group 10.1038/ncomms3119

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Intermolecular electron-transfer reactions have a crucial role in biology, solution chemistry and electrochemistry. The first step of such reactions is the expulsion of the electron to the solvent, whose mechanism is determined by the structure and dynamical response of the latter. Here we visualize the electron transfer to water using ultrafast fluorescence spectroscopy with polychromatic detection from the ultraviolet to the visible region, upon photo-excitation of the so-called charge transfer to solvent states of aqueous iodide. The initial emission is short lived (~60 fs) and it relaxes to a broad distribution of lower-energy charge transfer to solvent states upon rearrangement of the solvent cage. This distribution reflects the inhomogeneous character of the solvent cage around iodide. Electron ejection occurs from the relaxed charge transfer to solvent states with lifetimes of 100–400 fs that increase with decreasing emission energy.

Item Type:

Journal Article (Original Article)

Division/Institute:

08 Faculty of Science > Institute of Applied Physics

UniBE Contributor:

Cannizzo, Andrea

Subjects:

600 Technology > 620 Engineering

ISSN:

2041-1723

Publisher:

Nature Publishing Group

Language:

English

Submitter:

Martin Frenz-Lips

Date Deposited:

22 Sep 2014 11:46

Last Modified:

27 May 2018 01:48

Publisher DOI:

10.1038/ncomms3119

BORIS DOI:

10.7892/boris.52953

URI:

https://boris.unibe.ch/id/eprint/52953

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