Long-lived nuclear coherences inside helium nanodroplets

Abstract

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 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 wavepacket motion of indium dimers (In${}_2$) for over 50 ps, 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 to study processes depending on long nuclear coherence in a dissipative environment. Furthermore, tailor-made microsolvation environments inside droplets will enable to investigate the solvent influence on intramolecular dynamics in a wide tuning range from molecular isolation to strong molecule-solvent coupling.

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Cited by in corpus (5)

• Rotational coherence spectroscopy of molecules in helium nanodroplets: Reconciling the time and the frequency domains
• Quantum-State-Sensitive Detection of Alkali Dimers on Helium Nanodroplets by Laser-Induced Coulomb Explosion
• Laser-induced Coulomb Explosion Imaging of Alkali Dimers on Helium Nanodroplets
• High-resolution two-dimensional electronic spectroscopy reveals homogeneous line profiles in isolated nanoparticles
• Time-resolved Coulomb explosion imaging of vibrational wave packets in alkali dimers on helium nanodroplets