Dynamics of molecular rotors in bulk superfluid helium

Abstract

Molecules immersed in liquid helium are excellent probes of superfluidity. Their electronic, vibrational, and rotational dynamics provide valuable clues about the superfluid at the nanoscale. Here we report on the experimental study of the laser-induced rotation of helium dimers inside the superfluid 4He bath at variable temperature. The coherent rotational dynamics of He2͙ is initiated in a controlled way by ultrashort laser pulses and tracked by means of time-resolved laser-induced fluorescence. We detect the decay of rotational coherence on the nanosecond time scale and investigate the effects of temperature on the decoherence rate. The observed temperature dependence suggests a nonequilibrium evolution of the quantum bath, accompanied by the emission of the wave of second sound. The method offers ways of studying superfluidity with molecular nanoprobes under variable thermodynamic conditions.