Coalescence of Cluster Beam Generated Sub‐2 nm Bare Au Nanoparticles and Analysis of Au Film Growth Parameters

Abstract

In this work is presented the growth model for Au films grown on a carbon substrate at room temperature by using as building blocks Au nanoparticles (NPs) with 1.4 nm mean size generated via remote cluster beam synthesis and soft landing on the substrate. The key results highlighted in this work are that 1) the deposited nanoparticles coalesce at substrate level in such a way that the film growth is 3D, 2) newly formed nanoparticles at substrate level are predominantly magic number clusters and 3) coalescensce takes place as soon as two neighboring nanopartciles come closer than a critical distance. The film growth was investigated by TEM as a function of Au load, in the range 0-1.2 μg/cm 2 . Two distinct regimes are identified: the "landing regime" and the "coalescence regime". During the latter the film growth is 3D with a dynamic scaling exponent z of 2.13. Particular attention was devoted to the study of the evolution of the NP population from the moment they are generated with the cluster beam generator to the moment they land on the substrate and coalesce with other NPs. Our results show that 1) the NPs generated by the cluster beam are heterogeneous in size and are made by more than 95% by Au Magic numbers, mainly Au 20 and Au 55 and 2) kinetic processes (coalescence) at substrate level is capable of producing NPs populations made of larger Au magic numbers containing up to several thousands of Au atoms. Experimental and simulation results provide insight into the coalescence mechanism and provide strong evidence that the NPs coalesce when the nearest neighbor distance is below a critical mark. The critical distance is at its minimum 0.4-0.5 nm and it is still unclear whether it is constant or not although the best matching simulation results seem to point to a superlinear dependence from the NP size difference between two neighboring candidate coalescing NPs. The coalescence phenomenon investigated in this work pinpoints the unique self-organization properties of these small Au NPs in creating films with a stable edge-to-edge mean nearest neighbor distance of the order of 1.4 nm.

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“…X-ray diffraction patterns (XRD) of ZnO NPs film, shown in figure 1B, confirming the wurtzite crystalline phase of ZnO NPs. The kinetics of Au nanostructures formation during the deposition process are strongly dependent on the atomsubstrate interactions, inherently linked to the substrate nature, and are ultimately found to follow the Wolmer-Weber [32] film growth model, often leading to the formation of 3D Au nanoislands [33] . Consequently, the formation of well-defined Au nanoislands on PEDOT:PSS results from the molecular scale structures of the PEDOT:PSS surface composition, [34] which has been shown to hinder the diffusion of gold atoms on the surface and facilitate the gold nucleation process [33,35] .…”