Helium Droplet-Mediated Deposition and Aggregation of Nanoscale Silver Clusters on Carbon Surfaces

R Fernandez-Perea and LF Gomez and C Cabrillo and M Pi and AO Mitrushchenkov and AF Vilesov and MP de Lara-Castells, JOURNAL OF PHYSICAL CHEMISTRY C, 121, 22248-22257 (2017).

DOI: 10.1021/acs.jpcc.7b08109

We present experiments and calculations of the deposition and aggregation of silver clusters embedded in helium droplets onto an amorphous carbon surface at room temperature. Calculations were also performed for deposition onto a graphene surface. They involve potentials for the interaction of carbon atoms with silver and helium atoms, provided by ab initio calculations. The numerical simulations were performed for few-nanometer-sized silver clusters including up to 5000 Ag atoms and He droplets with up to 10(5) He-4 atoms. The fluid nature of the He-4 droplet is accounted for by the renormalizationof the He-He interaction potential. The numerical results are consistent with deposition experiments with an average number of 3000 Ag atoms per 4He droplet and indicate that the aggregation of the silver clusters on the carbon surface is mediated by secondary droplet impacts. They also reveal nontrivial dynamics of the Ag clusters within the carrier droplet, showing a tendency to drift toward the droplet surface. These findings are of relevance in understanding the heterogeneous deposition patterns (large ramified islands) developed for very large droplets with an average number of Ag atoms per droplet within the million range. Finally, the simulations of large (5000 atoms) Ag cluster deposition on graphene reveals strong superdiffusive behavior. In stark contrast, the diffusion is negligible on the amorphous carbon surface.

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