Department of Chemistry2024-11-0920111089-563910.1021/jp111825n2-s2.0-79959546704http://dx.doi.org/10.1021/jp111825nhttps://hdl.handle.net/20.500.14288/11669We present in this work the study of small He-4(N)-Cs-2((3)Sigma(u)) aggregates (2 <= N <= 30) through combined variational, diffusion Monte Carlo (DMC), and path integral Monte Carlo (PIMC) calculations. The full surface is modeled as an addition of He-Cs-2 interactions and He-He potentials. Given the negligible strength and large range of the He-CS2 interaction as compared with the one for He-He, a propensity of the helium atoms to pack themselves together, leaving outside the molecular dopant is to be expected. DMC calculations determine the onset of helium gathering at N = 3. To analyze energetic and structural properties as a function of N, PIMC calculations with no bosonic exchange, i.e., Boltzmann statistics, at low temperatures are carried out. At T = 0.1 K, although acceptable one-particle He-Cs-2 distributions are obtained, two-particle He He distributions are not well described, indicating that the proper symmetry should be taken into account. PIMC distributions at T = 1 K already compare well with DMC ones and show minor exchange effects, although binding energies are still far from having converged in terms of the number of quantum beads. As N increases, the He-He PIMC pair correlation function shows a clear tendency to coincide with the experimental boson-liquid helium one at that temperature. It supports the picture of a helium droplet which carries the molecular impurity on its surface, as found earlier for other triplet dimers.Chemistry, physical and theoreticalPhysicsAtomic structureMolecular dynamicsChemical engineeringJournal Article1520-5215291895500019Q29898