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

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

*Corresponding author af dette arbejde

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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.

OriginalsprogEngelsk
Artikelnummer203203
TidsskriftPhysical Review Letters
Vol/bind118
Nummer20
Antal sider6
ISSN0031-9007
DOI
StatusUdgivet - 19 maj 2017

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