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

2017; American Physical Society; Volume: 118; Issue: 20 Linguagem: Inglês

10.1103/physrevlett.118.203203

1092-0145

Benjamin Shepperson, Anders A. Søndergaard, Lars Christiansen, Jan Kaczmarczyk, Robert E. Zillich, Mikhail Lemeshko, Henrik Stapelfeldt,

Spectroscopy and Quantum Chemical Studies

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.