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.

Nonvolatile resistive switching and synaptic characteristics of lead-free all-inorganic perovskite-based flexible memristive devices for neuromorphic systems.

Recently, several types of lead halide perovskites have been actively researched for resistive switching (RS) memory or artificial synaptic devices due to their current-voltage hysteresis along with the feasibility of fabrication, low-temperature processability and superior charge mobility. However, the toxicity and environmental pollution potential of lead halide perovskites severely restrict their large-scale commercial prospects. In the present work, the environmentally friendly and uniform CsSnCl3 perovskite films are introduced to act as an active layer in the flexible memristors. Ag/CsSnCl3/ITO devices demonstrate bipolar RS with excellent electrical properties such as forming free characteristics, good uniformity, low operating voltages, a high ON/OFF ratio (102) and a long retention time (>104 s). The RS mechanism has been well explained in the outline of electric field-induced formation and rupture of Ag filaments in the CsSnCl3 layer. The metallic nature of the conducting filament has been further confirmed by temperature-dependent variation of low and high resistance states. Additionally, various pulse measurements have been carried out to mimic some of the basic synaptic functions including postsynaptic current, paired-pulse facilitation, long-term potentiation and long-term depression under normal as well as bending conditions. Our work provides the opportunity for exploring artificial synapses based on lead-free halide perovskites for the development of next-generation flexible electronics.