Aliovalent Ta-Doping-Engineered Oxygen Vacancy Configurations for Ultralow-Voltage Resistive Memory Devices: A DFT-Supported Experimental Study

Alteration of transport properties of any material, especially metal oxides, by doping suitable impurities is not straightforward as it may introduce multiple defects like oxygen vacancies (V_o) in the system. It plays a decisive role in controlling the resistive switching (RS) performance of metal oxide-based memory devices. Therefore, a judicious choice of dopants and their atomic concentrations is crucial for achieving an optimum V_o configuration. Here, we show that the rational designing of RS memory devices with cationic dopants (Ta), in particular, Au/Ti_1−xTa_xO_2−δ/Pt devices, is promising for the upcoming non-volatile memory technology. Indeed, a current window of ∼10⁴ is realized at an ultralow voltage as low as 0.25 V with significant retention (∼10⁴ s) and endurance (∼10⁵ cycles) of the device by considering 1.11 at % Ta doping. The obtained device parameters are compared with those in the available literature to establish its excellent performance. Furthermore, using detailed experimental analyses and density functional theory (DFT)-based first-principles calculations, we comprehend that the meticulous presence of V_o configurations and the columnar-like dendritic structures is crucial for achieving ultralow-voltage bipolar RS characteristics. In fact, the dopant-mediated V_o interactions are found to be responsible for the enhancement in local current conduction, as evidenced from the DFT-simulated electron localization function plots, and these, in turn, augment the device performance. Overall, the present study on cationic-dopant-controlled defect engineering could pave a neoteric direction for future energy-efficient oxide memristors.