Nano t-Se Peninsulas Embedded in Natively Oxidized 2D TiSe₂ Enable Uniform and Fast Memristive Switching

Memristive devices, regardless of their potential applications in memory and computing scenarios, still suffer from large cycle-to-cycle and device-to-device variations due to the stochastic growth of conductive filaments (CFs). In this work, we fabricated a crossbar memristor using the 2D TiSe₂ material and then oxidized it into TiO₂ in the atmosphere at a moderate temperature. Such a mild oxidation approach fails to evaporate all Se into the air, and after further annealing using thermal or electrical stimulations, the remnant Se atoms gather near the interfaces and grow into nanosized crystals with relatively high conductivity. The resulting peninsula-shaped nanocrystals distort the electric field, forcing CFs to grow on them, which could largely confine the location and length of CFs. As a result, this two-terminal TiSe₂/TiO₂/TiSe₂ device exhibits excellent resistive switching performance with a fairly low threshold voltage (V_set < 0.8 V, V_reset > 0.55 V) and high cycle-to-cycle consistency, enabling resistive switching at narrow operating variations, e.g., 500 ± 48 and 845 ± 39 mV. Our work offers a new approach to minimize the cycle-to-cycle stochasticity of the memristive device, paving the way for its applications in data storage and brain-inspired computing.