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M. Falge, V. Engel, S. Gräfe:
"Fingerprints of Adiabatic versus Diabatic Vibronic Dynamics in the Asymmetry of Photoelectron Momentum Distributions";
Journal of Physical Chemistry Letters, 3 (2012), 2617 - 2620.

When the Born-Oppenheimer approximation is valid, electrons adiabatically follow the nuclear motion in molecules. For strong nonadiabatic coupling between electronic states, one encounters a diabatic motion where the electrons remain local and do not adapt to molecular geometry changes. We show that the mentioned limiting cases are reflected differently in the asymmetry of time-resolved photoelectron momentum distributions. Whereas for adiabatic dynamics, the asymmetry directly maps the time-dependent average nuclear momentum, in the diabatic case, the asymmetry is determined by a nonclassical interference effect arising from the mixing of wave function components in different electronic states, which is present at times nonadiabatic transitions take place.

http://dx.doi.org/10.1021/jz3009826

Project Head Stefanie Gräfe:
Korrelierte Elektronendynamik in ultrakurzen, starken mehr-Farben Laserfeldern