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The Journal of Chemical Physics

Comment on ‘‘The weakest bond: Experimental observation of helium dimer’’ [J. Chem. Phys. 9 8, 3564 (1993)]

Eric S. Meyer, John C. Mester, Isaac F. Silvera

Published Mar 1, 1994• 25 citations
Publisher

Abstract

Recently, Luo et al. reported indirect evidence for the formation of dimers in a supersonic expansion of helium. They interpreted their data as confirmation of the existence of a bound state of 4He–4He with a binding energy of order 1 mK. We show that their data are actually consistent with the formation of helium trimers and not dimers. The two control experiments that they performed do not provide any evidence for discarding this alternative hypothesis.

DOI
10.1063/1.466338

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•Jun 18, 2007•3 citations
Recently, Luo et al. reported indirect evidence for the formation of dimers in a supersonic expansion of helium. They interpreted their data as confirmation of the existence of a bound state of 4He–4He with a binding energy of order 1 mK. We show that their data are actually consistent with the formation of helium trimers and not dimers. The two control experiments that they performed do not provide any evidence for discarding this alternative hypothesis.
Van der Waals attraction between helium atoms can lead to the formation of weakly-bound He 2 diatomic molecules stable at temperatures in the millikelvin range. Helium dimers were first detected experimentally in 1993 and 1994. Sophisticated quantum-mechanical computations confirm that the He–He bond is the weakest known, with a binding energy corresponding to 1.176 mK, about 10 -4 eV. The average internuclear distance is computed to be in excess of 50 Å, which makes He 2 the largest known diatomic molecule as well. The authors have introduced an idealized deltafunction model for the helium dimer that succinctly represents its remarkable properties. Despite the weakness of each individual He–He bond, an intriguing mechanism exists for helium to form trimers and larger clusters with much greater binding energies.
Abstract We have shown that a simple model based on pairwise deltafunction potentials can, with an appropriate choice of parameters, represent the general behavior of ultra‐low temperature helium dimers and trimers, including all possible isotopomers. The species 4He2, 4He3, and 4He23He are stable, with binding energies of approximately 1.3, 100, and 10 mK, respectively. An Efimov state for 4He23He is also predicted, bound by 2.4 mK. The remaining dimers and trimers, 4He 3He, 3He2, 4He 3He2, and 3He3, are evidently unstable. © 2001 John Wiley & Sons, Inc. Int J Quantum Chem, 2001
Abstract Small helium clusters Hen (n = 2, 3, ... , 10) in molecular beams produced by supersonic expansion of gaseous helium have been observed in several different experiments. Among these clusters the dimer, which has a single very slightly bound state, and the trimer, which could have many bound states, have especially unusual properties which QMC calculations can explain in detail. In this paper, diffusion QMC calculations were used to determine ground state properties for clusters (n = 2, ... , 10) using two accurate, but slightly different pairwise-additive potential energy expressions, a perturbation-based potential by Tang et al.a and an empirical potential (HFD-B) proposed by Aziz et al.b Trial functions for importance sampling were based on those determined earlier by Rick et alc. Expectation values and probability distributions were determined by the descendent-weighting technique to give results independent of the trial functions. As expected, a single bound state of the dimer was found, and its average internuclear distance was predicted to be 51.5 A. Energies for clusters with n = 2, 7 with the HFD-B potential were in good agreement with those of earlier calculations. Comparisons of the results for the two different potential energy expressions showed energies differing by a few percent. Tests of possible nonadditive interactions showed these to be far less important in their effects on predicted energies.