We present a quantitative exploration, combining experiment and simulation, of the mechanical and electronic properties, as well as the modifications induced by an alkylthiolated coating, at the single NP level. We determine the response of the NPs to external pressure in a controlled manner by using an atomic force microscope tip. We find a strong reduction of their Young modulus, as compared to bulk gold, and a significant influence of strain in the electronic properties of the alkylthiolated NPs. Electron transport measurements of tiny molecular junctions (NP/alkylthiol/CAFM tip) show that the effective tunnelling barrier through the adsorbed monolayer strongly decreases with increasing the applied load, which translates in a remarkable and unprecedented increase of the tunnel current. These observations are successfully explained using simulations based on finite element analysis (FEA) and first-principles calculations that permit to consider the coupling between the mechanical response of the system and the electric dipole variations at the interface.
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