Laser-induced rotation of iodine molecules in He-nanodroplets: revivals and breaking-free Journal Article


Author(s): Shepperson, Benjamin; Søndergaard, Anders A; Christiansen, Lars; Kaczmarczyk, Jan; Zillich, Robert E; Lemeshko, Mikhail; Stapelfeldt, Henrik
Article Title: Laser-induced rotation of iodine molecules in He-nanodroplets: revivals and breaking-free
Affiliation IST Austria
Abstract: Rotation of molecules embedded in He 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 He shell. Our results open novel opportunities for studying non-equilibrium solute-solvent dynamics and quantum thermalization.
Journal Title: Physical Review Letters
Volume: 118
ISSN: 1079-7114
Publisher: American Physical Society  
Date Published: 2017-05-19
Start Page: Article number: 203203
URL:
DOI: 10.1103/PhysRevLett.118.203203
Notes: We thank Richard Schmidt for insightful discussions. JK acknowledges support from People Programme (Marie Curie Actions) of the European Union’s Seventh Framework Programme (FP7/2007-2013) under REA grant agreement No. [291734]. REZ acknowledges support from the Austrian Science Fund (FWF) under grant No. P23535-N20. ML acknowledges support from the Austrian Science Foundation (FWF), under grant No. P29902-N27. HS acknowledges support from the Eu- ropean Research Council-AdG (Project No. 320459, DropletControl) and the Villum Foundation.
Open access: no