Femtosecond photoexcitation dynamics inside a quantum solvent

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 (He${}_{\mathrm{N}}$), obtained from femtosecond pump-probe spectroscopy and time-dependent density functional theory simulations. For the In-He${}_{\mathrm{N}}$ 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.

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Cited by in corpus (10)

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• Time-resolved study of resonant interatomic Coulombic decay in helium nanodroplets
• Unravelling the Full Relaxation Dynamics of Superexcited Helium Nanodroplets
• High-resolution two-dimensional electronic spectroscopy reveals homogeneous line profiles in isolated nanoparticles
• Observation of laser-assisted electron scattering in superfluid helium
• Time-resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-doped Helium Nanodroplets
• Zero-phonon lines in the spectra of dysprosium atoms in superfluid helium
• Electron energy loss and angular asymmetry induced by elastic scattering in helium droplets
• Photoelectron spectroscopy of coronene molecules embedded in helium nanodroplets