Vanadium dioxide has been identified as a promising phase-changing material for use in tunable plasmonic devices. In this study, we present a comprehensive modal analysis of single-phase and multi-phase vanadium dioxide nanoparticles. In-situ high-resolution electron energy loss spectroscopy was utilized to experimentally resolve the dipole plasmon peak, higher-order and breathing plasmonic modes, and bulk losses as a function of nanoparticle size. Furthermore, the focus is directed toward capturing the dynamic nanoscale optical response throughout the metal-insulator transition in a vanadium dioxide nanoparticle. This system possesses the ability to be gradually switched on and off in terms of the emergence of near-infrared plasmonic absorption. The switching is accompanied by a gradual spectral shift of the absorption peak, amounting to 0.18 eV for a 120 nm nanoparticle. It is envisioned that this phenomenon can be generalized to larger nanostructures with a higher aspect ratio, thereby introducing a wider tunability of the system, which is essential for functional nanodevices based on vanadium dioxide.

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