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 (Vo) 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 Vo configuration. Here, we show that the rational designing of RS memory devices with cationic dopants (Ta), in particular, Au/Ti1-xTaxO2-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 Vo configurations and the columnar-like dendritic structures is crucial for achieving ultralow-voltage bipolar RS characteristics. In fact, the dopant-mediated Vo 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.

Induced Vacancy-Assisted Filamentary Resistive Switching Device Based on RbPbI3-xClx Perovskite for RRAM Application.

Halide perovskite (HP) materials are actively researched for resistive switching (RS) memory devices due to their current-voltage hysteresis along with low-temperature processability, superior charge mobility, and simple fabrication. In this study, all-inorganic RbPbI3 perovskite has been doped with Cl in the halide site and incorporated as a switching media in the Ag/RbPbI3-xClx/ITO structure, since pure RbPbI3 is nonswitchable. Five compositions of the RbPbI3-xClx (x = 0, 0.3, 0.6, 0.9, and 1.2) films are fabricated, and the conductivity was found to be increasing upon increase in Cl concentration, as revealed by dielectric and I-V measurements. The device with a 20% chloride-substituted film exhibits a higher on/off ratio, extended endurance, long retention, and high-density storage ability. Finally, a plausible explanation of the switching mechanism from iodine vacancy-mediated growth of conducting filaments (CFs) is provided using conductive atomic force microscopy (c-AFM). The c-AFM measurements reveal that pure RbPbI3 is insulating in nature, whereas Cl-doped films demonstrate resistive switching behavior.