Laser-Induced Rotation of Iodine Molecules in Helium Nanodroplets: Revivals and Breaking Free

Benjamin Shepperson, Anders A. Søndergaard, Lars Christiansen, Jan Kaczmarczyk, Robert E. Zillich, Mikhail Lemeshko, and Henrik Stapelfeldt
Phys. Rev. Lett. 118, 203203 – Published 19 May 2017
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Abstract

Rotation of molecules embedded in helium nanodroplets is explored by a combination of fs laser-induced alignment experiments and angulon quasiparticle theory. We demonstrate that at low fluence of the fs alignment pulse, the molecule and its solvation shell can be set into coherent collective rotation lasting long enough to form revivals. With increasing fluence, however, the revivals disappear—instead, rotational dynamics as rapid as for an isolated molecule is observed during the first few picoseconds. Classical calculations trace this phenomenon to transient decoupling of the molecule from its helium shell. Our results open novel opportunities for studying nonequilibrium solute-solvent dynamics and quantum thermalization.

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  • Received 1 February 2017

DOI:https://doi.org/10.1103/PhysRevLett.118.203203

© 2017 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Benjamin Shepperson1, Anders A. Søndergaard2, Lars Christiansen1, Jan Kaczmarczyk3, Robert E. Zillich4,*, Mikhail Lemeshko3,†, and Henrik Stapelfeldt1,‡

  • 1Department of Chemistry, Aarhus University, 8000 Aarhus C, Denmark
  • 2Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C, Denmark
  • 3IST Austria (Institute of Science and Technology Austria), Am Campus 1, 3400 Klosterneuburg, Austria
  • 4Institute for Theoretical Physics, Johannes Kepler Universität Linz, Altenbergerstraße 69, A-4040 Linz, Austria

  • *Robert.Zillich@jku.at
  • mikhail.lemeshko@ist.ac.at
  • henriks@chem.au.dk

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Issue

Vol. 118, Iss. 20 — 19 May 2017

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