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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Bernhard Thaler: Graz University of Technology
Sascha Ranftl: Graz University of Technology
Pascal Heim: Graz University of Technology
Stefan Cesnik: Graz University of Technology
Leonhard Treiber: Graz University of Technology
Ralf Meyer: Graz University of Technology
Andreas W. Hauser: Graz University of Technology
Wolfgang E. Ernst: Graz University of Technology
Markus Koch: Graz University of Technology

Nature Communications, 2018, vol. 9, issue 1, 1-6

Abstract: Abstract 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 indium (In) dopant atoms inside helium nanodroplets (HeN), obtained from femtosecond pump–probe spectroscopy and time-dependent density functional theory simulations. For the In–HeN system, part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective shell oscillation with a period of about 30 ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.

Date: 2018
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DOI: 10.1038/s41467-018-06413-9

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