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

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  • Benjamin Shepperson
  • ,
  • Anders A. Sondergaard
  • ,
  • Lars Christiansen
  • ,
  • Jan Kaczmarczyk, Institute of Science & Technology - Austria
  • ,
  • Robert E. Zillich, Johannes Kepler University
  • ,
  • Mikhail Lemeshko, Institute of Science & Technology - Austria
  • ,
  • Henrik Stapelfeldt

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.

TidsskriftPhysical Review Letters
Antal sider6
StatusUdgivet - 19 maj 2017

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