Communication: Angular momentum alignment and fluorescence polarization of alkali atoms photodetached from helium nanodroplets

The theory of photofragments angular momentum polarization is applied to the photodetachment of an electronically excited alkali atom from a helium nanocluster (N = 200). The alignment of the electronic angular momentum of the bare excited alkali atoms produced is calculated quantum mechanically by solving the excited states coupled equations with potentials determined by density functional theory (DFT). Pronounced oscillations as a function of excitation energy are predicted for the case of Na@(He)(200), in marked contrast with the absorption cross-section and angular distribution of the ejected atoms which are smooth functions of the energy. These oscillations are due to quantum interference between different coherently excited photodetachment pathways. Experimentally, these oscillations should be reflected in the fluorescence polarization and polarization-resolved photoelectron yield of the ejected atoms, which are proportional to the electronic angular momentum alignment. In addition, this result is much more general than the test case of NaHe200 studied here. It should be observable for larger droplets, for higher excited electronic states, and for other alkali as well as for alkali-earth atoms. Detection of these oscillations would show that the widely used pseudo-diatomic model can be valid beyond the prediction of absorption spectra and could help in interpreting parts of the dynamics, as already hinted by some experimental results on angular anisotropy of bare alkali fragments. (C) 2013 AIP Publishing LLC.

Published in:
Journal Of Chemical Physics, 139, 22
Melville, Amer Inst Physics

 Record created 2014-01-20, last modified 2018-12-03

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