Long-Lived Nuclear Coherences inside Helium Nanodroplets

Much of our knowledge about dynamics and functionality of molecular systems has been achieved with femtosecond time-resolved spectroscopy. Despite extensive technical developments over the past decades, some classes of systems have eluded dynamical studies so far. Here, we demonstrate that superfluid helium nanodroplets, acting as a thermal bath of 0.4 K temperature to stabilize weakly bound or reactive systems, are well suited for time-resolved studies of single molecules solvated in the droplet interior. By observing vibrational wave packet motion of indium dimers ( In 2 ) for tens of picoseconds, we demonstrate that the perturbation imposed by this quantum liquid can be lower by a factor of 10–100 compared to any other solvent, which uniquely allows us to study processes depending on long nuclear coherence in a dissipative environment. Furthermore, tailor-made microsolvation environments inside droplets will enable us to investigate the solvent influence on intramolecular dynamics in a wide tuning range from molecular isolation to strong molecule-solvent coupling.