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首页> 外文期刊>journal of chemical physics >Transient photophysical holehyphen;burning spectroscopy of the hydrated electron: A quantum dynamical simulation
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Transient photophysical holehyphen;burning spectroscopy of the hydrated electron: A quantum dynamical simulation

机译:Transient photophysical holehyphen;burning spectroscopy of the hydrated electron: A quantum dynamical simulation

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摘要

Results for the timehyphen;dependent adiabatic eigenspectrum of an electron in water evolving in dynamic equilibrium have been obtained via quantum molecular dynamics simulation and used to evaluate the results expected from timehyphen;resolved transient optical holehyphen;burning experiments. The dependence on excitation frequency and pulse length have been explored. The calculated results indicate that a relatively broad hole is created, but that, for ultrashort pumpndash;probe time delays (le;100 fs) and comparably short pulses, the shape is distinctly different from the equilibrium spectrum. A slower component in the spectral evolution is also present, but appears likely to be difficult to distinguish experimentally. The shape of the absorption deficit is characteristic of the inhomogeneously broadened 1s, 2phyphen;type electronic state structure found previously to underlie the equilibrium spectrum, and distinguishes between this description and a number of proposed alternatives. With pulse durations comparable to the best now available, the phenomenon appears experimentally accessible.

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