Femtosecond spectroscopy of solvated electrons from sodium-ammonia-d3 solutions: temperature jump versus local density jump

The Journal of Chemical Physics
Jörg LindnerPeter Vöhringer

Abstract

The relaxation dynamics of solvated electrons from sodium-ammonia-d3 solutions was studied by femtosecond time-resolved near-infrared spectroscopy. The experimental pump-probe data reveal a pulse-width limited pump-induced redshift of the absorption spectrum of the ammoniated electron and a subsequent slower blueshift on a time scale of roughly 200 fs. The spectrotemporal response is interpreted using the nonadiabatic relaxation mechanism for cavity-bound solvated electrons in condensed phases. In particular, we develop a local density-jump model, which traces the dynamic spectrum back to a sequence of a pump-induced cavity expansion due to Pauli repulsion and a succeeding cavity contraction upon nonadiabatic return of the electron back to its ground state. Using the existing thermodynamic data of the solvent and experimental temperature and density-dependent absorption spectra of metal-ammonia solutions, an overall increase in the interparticle distance within the solvent cavity of 25% is crudely estimated. The density-jump model is compared to the temperature-jump model we proposed previously for the femtosecond relaxation dynamics of metal-NH(3) solutions.

References

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Feb 8, 2006·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Jörg LindnerPeter Vöhringer
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Citations

Dec 11, 2014·Annual Review of Physical Chemistry·Peter Vöhringer
Oct 6, 2018·Physical Chemistry Chemical Physics : PCCP·Tim Vogler, Peter Vöhringer
Aug 18, 2010·Physical Chemistry Chemical Physics : PCCP·Stephan KratzPeter Vöhringer
Oct 15, 2011·Physical Chemistry Chemical Physics : PCCP·Joel Torres-AlacanPeter Vöhringer
Jul 25, 2012·Physical Chemistry Chemical Physics : PCCP·Tim SchäferDirk Schwarzer
Jan 26, 2012·The Journal of Physical Chemistry. B·Janus UrbanekPeter Vöhringer
Jul 3, 2013·The Journal of Physical Chemistry. B·Janus Urbanek, Peter Vöhringer

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Methods Mentioned

BETA
nuclear magnetic resonances

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