Quantum solvation and molecular rotations in superfluid helium clusters

Spectroscopic experiments on molecules embedded in free clusters of liquid helium reveal a number of unusual features deriving from the unique quantum behavior of this nanoscale matrix environment. The apparent free rotation of small molecules in bosonic 4He clusters is one of the experimentally most well documented of these features. In this Focus article, we set this phenomenon in the context of experimental and theoretical advances in this field over the last ten years, and describe the microscopic insight which it has provided into the nature and dynamic consequences of quantum solvation in a superfluid. We provide a comprehensive theoretical analysis which is based on a unification of conclusions drawn from diffusion and path integral Monte Carlo calculations. These microscopic quantum calculations elucidate the origin of the empirical free rotor spectrum, and its relation to the boson character and superfluid nature of the quantum nanosolvent. The free rotor behavior of the molecular rotation is pre...

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