Real-time observation of the charge transfer to solvent dynamics

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...

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Vydáno v:Nature communications Ročník 4; číslo 1; s. 2119
Hlavní autoři: Messina, Fabrizio, Bräm, Olivier, Cannizzo, Andrea, Chergui, Majed
Médium: Journal Article
Jazyk:angličtina
Vydáno: London Nature Publishing Group UK 02.07.2013
Nature Publishing Group
Témata:
639/766/119
639/766/189
Electrochemistry
Electrons
Emissions
Humanities and Social Sciences
Iodides
multidisciplinary
Science
Science (multidisciplinary)
Simulation
Solution chemistry
Solvents
Switzerland
ISSN:2041-1723, 2041-1723
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Shrnutí: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. Electron transfer from solute to solvent has a crucial role in chemistry, but this process has not yet been visualized in real time. Messina et al. provide the first real-time observation of the dynamic rearrangement of water cages around aqueous halides before full electron ejection.
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ISSN:2041-1723
2041-1723
DOI:10.1038/ncomms3119