Non-ohmic behavior and resistive switching of Au cluster-assembled films beyond the percolation threshold

Networks based on nanoscale resistive switching junctions are considered promising for the fabrication of neuromorphic computing architectures. To date random networks of nanowires, nanoparticles, and metal clusters embedded in a polymeric matrix or passivated by shell of ligands or oxide layers have been used to produce resistive switching systems. The strategies applied to tailor resistive switching behavior are currently based on the careful control of the volume fraction of the nanoscale conducting phase that must be fixed close to the electrical percolation threshold. Here, by blending laboratory and computer experiments, we demonstrate that metallic nanostructured Au films fabricated by bare gold nanoparticles produced in the gas phase and with thickness well beyond the electrical percolation threshold, show a non-ohmic electrical behavior and complex and reproducible resistive switching. We observe that the nanogranular structure of the Au films does not evolve with thickness: this introduces a huge number of defects and junctions affecting the electrical transport and causing a dynamic evolution of the nanoscale electrical contacts under the current flow. To uncover the origin of the resistive switching behavior in Au cluster-assembled films, we developed a simple computational model for determining the evolution of a model granular film under bias conditions. The model exploits the information provided by experimental investigation about the nanoscale granular morphology of real films. Our results show that metallic nanogranular materials have functional properties radically different from their bulk counterparts, in particular nanostructured Au films can be fabricated by assembling bare gold clusters which retain their individuality to produce an all-metal resistive switching system.