Helium droplet-mediated deposition and aggregation of nanoscale silver clusters on carbon surfaces

10 pags., 7 figs. -- ACS Liveslides presentation: http://pubs.acs.org/doi/suppl/10.1021/acs.jpcc.7b08109We 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 105 4He atoms. The fluid nature of the 4He droplet is accounted for by the renormalization of 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.This work has been partly supported by the Spanish Agencia Estatal de Investigación (AEI) and the Fondo Europeo de Desarrollo Regional (FEDER, UE) under Grant No. MAT2016-75354-P, the National Science Foundation (UnitedStates) under Grant Nos. CHE-1362535 and CHE-1664990, and the COST Action CM1405 “Molecules in Motion” (MOLIM). M.P. thanks the finantial support by the AEI and FEDER under Grant No. FIS2014-52285-C2-1-P. M.P.d.L.-C. thanks Andreas W. Hauser, Nadine Halberstadt, and Marius Lewerenz for very helpful discussions. The CTI (CSIC) and CESGA supercomputer facilities (Spain) are acknowledged for the provided resources.We acknowledge support by the CSIC Open Access Publication Initiative through its Unit of Information Resources for Research (URICI).Peer reviewe