Theoretical study of the time-resolved photoelectron spectrum of Na 2F: effects of thermal initial conditions |
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Authors: | M-C Heitz G Durand F Spiegelman and C Meier |
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Institution: | (1) Laboratoire de Physique Quantique, UMR 5626 du CNRS, IRSAMC, Université Paul Sabatier, 31062 Toulouse, France;(2) Laboratoire Collisions, Agrégats et Réactivité, UMR 5589 du CNRS, IRSAMC, Université Paul Sabatier, 31062 Toulouse, France |
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Abstract: | The excited state dynamics of the
Na2F cluster initiated by a femtosecond
laser pulse is studied considering a thermally excited initial
sample. Within a pump-probe set-up, the time-dependent
photoelectron spectrum is calculated, which is shown to be a
sensitive tool to study intramolecular motion of the cluster.
Temperature effects are taken into account through thermal
averaging over the time-dependent spectra obtained from
different initial vibrational states of the cluster. The nuclear
motion upon laser excitation is described by full-dimensional
quantum wavepacket propagation using explicit, realistic pump
and probe pulses. The characteristic features of the
time-resolved photoelectron spectra of the
Na2F cluster, identified as due to
periodic bending motion of the cluster as well as to the
excitation of the stretching mode, are found to be robust
against increasing vibrational temperature of the cluster beam.
This finding is important for possible future experiments. |
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Keywords: | 36 40 Mr Spectroscopy and geometrical structure of
clusters 36 40 Sx Diffusion and dynamics of clusters 82 53 -k Femtochemistry 82 53 Hn Pump probe experiments with bound
states |
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