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The abilities to modulate linear and nonlinear optical response of materials in the nanoscale are of central importance in the design and fabrication of photonic devices for applications like optical modulators. Here, based on a simple transition metal oxide/nitride (TiO2/TiN) system, we show that it is possible to tune the optical properties by controlling the nanoscale architecture. Through controlled oxidation of the plasmonic TiN nanoparticle surfaces, we observe a continuous change of linear and nonlinear optical (NLO) properties with