  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.
