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Femtosecond photoexcitation dynamics inside a quantum solvent

Author

Listed:
  • 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)

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.

Suggested Citation

  • Bernhard Thaler & Sascha Ranftl & Pascal Heim & Stefan Cesnik & Leonhard Treiber & Ralf Meyer & Andreas W. Hauser & Wolfgang E. Ernst & Markus Koch, 2018. "Femtosecond photoexcitation dynamics inside a quantum solvent," Nature Communications, Nature, vol. 9(1), pages 1-6, December.
  • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-06413-9
    DOI: 10.1038/s41467-018-06413-9
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    Cited by:

    1. Ulrich Bangert & Frank Stienkemeier & Lukas Bruder, 2022. "High-resolution two-dimensional electronic spectroscopy reveals the homogeneous line profile of chromophores solvated in nanoclusters," Nature Communications, Nature, vol. 13(1), pages 1-8, December.

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