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Abstract
Diamantane clusters formed inside superfluid helium nanodroplets were analyzed by time-of-flight mass spectrometry. Distinct cluster sizes were identified as “magic numbers” and the corresponding feasible structures for clusters consisting of up to 19 diamantane molecules were derived from meta-dynamics simulations and subsequent DFT computations. The obtained interaction energies were attributed to London dispersion attraction. Our findings demonstrate that diamantane units readily form assemblies even at low pressures and near-zero Kelvin temperatures, confirming the importance of the intermolecular dispersion effect for condensation of matter.
Highlights
Superfluid helium nanodroplets (HNDs) are unique hosts for the study of weak interactions between molecules
We previously studied the effect of London dispersion (LD) interactions on diamondoid self-assembly on metal surfaces using scanning tunneling microscopy (STM) and atomic force microscopy (AFM) in combination with computational tools.[21,22,23]
We used superfluid helium nanodroplets as an ideal medium to explore clusters consisting of diamantane molecules by means of mass spectrometry
Summary
Superfluid helium nanodroplets (HNDs) are unique hosts for the study of weak interactions between molecules. HNDs are utilized as small reaction chambers where large clusters can form, with the released binding energy being dissipated by the evaporation of helium atoms.[4,5,6,7,8,9] Since helium has very low polarizability that results in weak HeÁ Á ÁHe interactions, it becomes superfluid at low pressures and near-zero Kelvin temperatures, with emerging properties like vanishing viscosity and high heat conductivity.[10] HNDs, have an almost negligible perturbative effect on dopant molecules and are an ideal medium for trapping weakly binding van der Waals complexes.[11,12] In previous experiments we already used the exceptional properties of HNDs to investigate molecular clusters like (V2O5)n8 or the very weakly bound alkali tripletdimers[13] and quartet-trimers.[14] Particles consisting of many units of doped molecules immersed inside HNDs are usually welldefined and can be deposited in a soft manner on surfaces for detection, thereby offering a non-destructive way to analyze complexes held together by quite weak forces
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