LAUSR

Oxides that exhibit an insulator–metal transition can be used to fabricate energy‐efficient relaxation oscillators for use in hardware‐based neural networks but there are very few oxides with transition temperatures above room temperature. Here the structural, electrical, and thermal properties of V3O5 thin films and their application as the functional oxide in metal/oxide/metal relaxation oscillators are reported. The V3O5 devices show electroforming‐free volatile threshold switching and negative differential resistance (NDR) with stable (<3% variation) cycle‐to‐cycle operation. The physical mechanisms underpinning these characteristics are investigated using a combination of electrical measurements, in situ thermal imaging, and device modeling. This shows that conduction is confined to a narrow filamentary path due to self‐confinement of the current distribution and that the NDR response is initiated at temperatures well below the insulator–metal transition temperature where it is dominated by the temperature‐dependent conductivity of the insulating phase. Finally, the dynamics of individual and coupled V3O5‐based relaxation oscillators is reported, showing that capacitively coupled devices exhibit rich non‐linear dynamics, including frequency and phase synchronization. These results establish V3O5 as a new functional material for volatile threshold switching and advance the development of robust solid‐state neurons for neuromorphic computing.