High‐Performance and Environmentally Robust Multilevel Lead‐Free Organotin Halide Perovskite Memristors

Abstract

With a striking explosion of digital information, organic–inorganic halide perovskite (OHP) memristors have been regarded as a promising solution to break the von Neumann bottleneck as the nonvolatile computing‐in‐memory architecture. However, toxicity and stability under ambient conditions are two critical issues for practical applications. Here, lead‐free MASnI3 (MASI) perovskites are reported with improved resistive switching (RS) performance via defects passivating by introducing PEACl. In‐Sn/PEACl‐MASI/PEDOT:PSS/ITO memristor arrays (10 × 10) exhibit reproducible RS with low SET/RESET voltage (VSET/VRESET, +0.58/−0.49 V), ultrahigh ON/OFF ratio (8.5 × 103), stable endurance (2 × 103 cycles), excellent retention (2 × 104 s), high device yield (88%), and multilevel storage. RS remains robust in harsh environments, including high temperature and humidity, long‐term light irradiation, and open‐air conditions. Importantly, a complete physical simulation model that quantitatively and accurately describes RS in vacancy concentration, temperature, and electric potential is proposed originating from conductive filaments formation/rupture. Additionally, PEACl‐MASI memristors are successfully fabricated on polyethylene terephthalate (PET) and Si substrates to explore the potential for large‐scale application on different substrates. The PEACl‐MASI memristors provide an opportunity to develop the next generation of high‐performance and environmentally robust multilevel information storage devices.

Influence of Lithium Doping on Volcanic-like Perovskite Memristors and Artificial Synaptic Simulation for Neurocomputing

“…C HRS and C LRS represent the coefficients of variations of HRS and LRS, respectively. The formula is C = σ/μ, 42 where σ is the resistance standard deviation and μ is the mean value, and the relevant comparison is shown in Figures S7b,c. In comparison with other devices reported in the literature shown in Table S2, our device has advantages in terms of the operating voltage, retention time, and other memristive properties.…”

“…The results show that the HRS is independent of I cc , and the LRS increases with increasing I cc , forming five levels of LRS (10, 5, 1, 0.5, and 0.1 mA). I cc affects the robustness of CF consistent with other studies Figure b shows that the endurance of HRS and five levels of LRS, which can clearly distinguish the five different resistance states for different I cc values.…”

Halide perovskite photoelectric artificial synapses: materials, devices, and applications

“…93 Although passivation or adding buffer layers can now properly improve its service life, it will sacrifice other performance indicators of HP-based devices. 94,95 For example, the durability of the memristor prepared by Yoo et al using MA 3 PbI 3−x Cl x can reach 2 × 10 4 times and has potential for neural simulation, but its on-off resistance ratio is less than 10 2 . 96 Therefore, the discovery of memristor properties brings both opportunities and new challenges to HP materials.…”

Organic multilevel (opto)electronic memories towards neuromorphic applications

“…Perovskites were also employed by Liu et al who reported an organic lead-free MASnI 3 materials that improved resistive switching performance via defect passivation by the introduction of phenethylammonium chloride. In-Sn/Phenethylammonium chloride MASnI 3 (PEACl-MASI)/poly(3,4-ethylenedioxythiophene) polystyrene sulfonate/indium tin oxide (ITO) memristor arrays (10 × 10) exhibited reproducible resistive switching with low set/reset voltages below ±1 V, an ON–OFF ratio of almost 10 4 , endurance over 10 3 cycles, retention times reaching 10 4 s and 5-level data storage 137 (Fig. 15g and h).…”