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Updated: Jun 12, 2026

Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry
Published on: April 8, 2020
Finite-temperature quantum simulations of mixed rare gas clusters
1Department of Chemistry, University of Basel, Klingelbergstrasse 80, CH-4056 Basel, Switzerland. m.meuwly@unibas.ch
Abstract:
Finite-temperature quantum Monte Carlo simulations are presented for mixed neon/argon rare gas clusters containing up to n=10 atoms. For the smallest clusters (n=3) comparison with rigorous bound state calculations and experiments shows that the present approach is accurate to within fractions of wavenumbers for energies and to within a few percent or better for rotational constants. For larger cluster sizes, for which no rigorous quantum calculations are available, comparison with experiment becomes even more favorable. In all simulations accurate pair potentials for the rare gas-rare gas interactions are employed and comparison with high-level electronic structure calculations suggest that many-body interactions play a minor role. For the largest clusters investigated (Ne(4)Ar(6)) gradual melting of the neon phase is observed while the argon-phase remains structurally intact.
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