Streamlining the Exploration of Chemical Space for Aqueous Molecular Metal Oxides as Thin Film Precursors

Metal oxide thin films based on V, Mo, W, Nb and/or Ta are relevant for a wide range of applications such as high-k dielectric materials or diffusion barriers. Recent advances in manufacturing techniques allowed their production through the spin coating of molecular metal oxide in aqueous solution. This is more environmentally friendly and cost-effectively than the traditional non-aqueous methods, however it is key to understand their speciation and the influence of the experimental conditions such as temperature, pH and/or concentration. Density functional theory calculations were used to construct a complex speciation network up to the formation of hexanuclear molecular metal oxides. These results were used to map the potential energy surface through a normal mode sampling into a neural network potential capable to reproduce the quantum mechanics energetics at a fraction of the cost. The neural network potential can be subsequently used to expand the chemical space and the formation of the nanometric molecular metal oxides which are beyond the reach of quantum mechanics