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  1. Metal-fullerene compounds are characterized by significant electron transfer to the fullerene cage, giving rise to an electric dipole moment. We use the method of electrostatic beam deflection to verify whether such reactions take place within superfluid helium nanodroplets between an embedded C 60 molecule and either alkali (heliophobic) or rare-earth (heliophilic) atoms. The two cases lead to distinctly different outcomes: C 60 Na n ( n = 1–4) display no discernable dipole moment, while C 60 Yb is strongly polar. This suggests that the fullerene and small alkali clusters fail to form a charge-transfer bond in the helium matrix despitemore »their strong van der Waals attraction. The C 60 Yb dipole moment, on the other hand, is in agreement with the value expected for an ionic complex.« less
    Free, publicly-accessible full text available May 4, 2023
  2. Abundance spectra of (CO 2 ) N clusters up to N ≈ 500 acquired under a wide range of adiabatic expansion conditions are analyzed within the evaporative ensemble framework. The analysis reveals that the cluster stability functions display a strikingly universal pattern for all expansion conditions. These patterns reflect the inherent properties of individual clusters. From this analysis the size-dependent cluster binding energies are determined, shell and subshell closing sizes are identified, and cuboctahedral packing ordering for sizes above N ≈ 130 is confirmed. It is demonstrated that a few percent variation in the dissociation energies translates into significant abundancemore »variations, especially for the larger clusters.« less
    Free, publicly-accessible full text available March 2, 2023
  3. Long-range intermolecular forces are able to steer polar molecules submerged in superfluid helium nanodroplets into highly polar metastable configurations. We demonstrate that the presence of such special structures can be identified, in a direct and determinative way, by electrostatic deflection of the doped nanodroplet beam. The measurement also establishes the structures’ electric dipole moments. In consequence, the introduced approach is complementary to spectroscopic studies of low-temperature molecular assembly reactions. It is enabled by the fact that within the cold superfluid matrix the molecular dipoles become nearly completely oriented by the applied electric field. As a result, the massive (tens ofmore »thousands of helium atoms) nanodroplets undergo significant deflections. The method is illustrated here by an application to dimers and trimers of dimethyl sulfoxide (DMSO) molecules. We interpret the experimental results with ab initio theory, mapping the potential energy surface of DMSO complexes and simulating their low temperature aggregation dynamics.« less