Desorption of alkali atoms from 4He nanodroplets

Abstract

The dynamics following the photoexcitation of Na and Li atoms located on the surface of helium nanodroplets has been investigated in a joint experimental and theoretical study. Photoelectron spectroscopy has revealed that excitation of the alkali atoms via the (n + 1)s ←ns transition leads to the desorption of these atoms. The mean kinetic energy of the desorbed atoms, as determined by ion imaging, shows a linear dependence on excitation frequency. These experimental findings are analyzed within a three-dimensional, time-dependent density functional approach for the helium droplet combined with a Bohmian dynamics description of the desorbing atom. This hybrid method reproduces well the key experimental observables. The dependence of the observables on the impurity mass is discussed by comparing the results obtained for the (6)Li and (7)Li isotopes. The calculations show that the desorption of the excited alkali atom is accompanied by the creation of highly non-linear density waves in the helium droplet that propagate at supersonic velocities.