Femtosecond photoexcitation dynamics inside a quantum solvent

Bernhard Thaler, Sascha Ranftl, Pascal Heim, Stefan Cesnik, Leonhard Treiber, Ralf Meyer, Andreas W. Hauser, Wolfgang E. Ernst, and Markus Koch

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Received: 28th March 18

The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of novel classes of molecules that have eluded dynamical studies so far. However, photoexcitation inside this quantum solvent triggers a pronounced response of the solvation shell, which is not well understood. Here we present a mechanistic description of the solvent response to photoexcitation of dopant atoms inside helium nanodroplets, obtained from femtosecond pump-probe spectroscopy and time-dependent density functional theory simulations. Part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective oscillation of the superfliuid helium with a period of (28 +- 1) ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.

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