Rotational spectrum of CO2 in helium clusters

Abstract

We present a theoretical study, based on Reptation Quantum Monte Carlo simulations, of a single CO2 molecule embedded in a Helium cluster (4He)N, with 2 ≤ N ≤ 50. Upon studying density profiles and rotational dynamics, we find a nontrivial behaviour that corresponds to the formation of the first solvation shell. We determine the value of N for which the rotational constant begins to approach the nanodroplet limit. We also give an example of computational spectroscopy, illustrating the complementarity of simulations and experiments.