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Halide perovskites with naturally coupled electron‐ion dynamics hold great potential for nonvolatile memory applications. Self‐rectifying memristors are promising as they can avoid sneak currents and simplify device configuration. Here we report a self‐rectifying memristor firstly achieved in a single perovskite (NHCINH3)3PbI5 (abbreviated as (IFA)3PbI5), which is sandwiched by Ag and ITO electrodes as the simplest cell in a crossbar array device configuration. The iodide ions of (IFA)3PbI5 can be easily activated, of which the migration in the bulk contributes to the resistance hysteresis and the reaction with Ag at the interface contributes to the spontaneous formation of AgI. The perfect combination of n‐type AgI and p‐type (IFA)3PbI5 gives rise to the rectification function like a p–n diode. Such a self‐rectifying memristor exhibits the record‐low set power consumption and voltage. This work emphasizes that the multifunction of ions in perovskites can simplify the fabrication procedure, decrease the programming power, and increase the integration density of future memory devices. [ABSTRACT FROM AUTHOR]

The liquid‐air interface offers a platform for the in‐plane growth of free‐standing materials. However, it is rarely used for inorganic perovskites and ultrathin non‐layered perovskites. Herein the liquid‐air interfacial synthesis of inorganic perovskite nanosheets (Cs3Bi2I9, Cs3Sb2I9) is achieved simply by drop‐casting the precursor solution with only the addition of iodine. The products are inaccessible without iodine addition. The thickness and lateral size of these nanosheets can be adjusted through the iodine concentration. The high volatility of the iodine spontaneously drives precursors that normally stay in the liquid to the liquid‐air interface. The iodine also repairs in situ iodine vacancies during perovskite growth, giving enhanced optical and optoelectronic properties. The liquid‐air interfacial growth of ultrathin perovskites provides multi‐degree‐of‐freedom for constructing perovskite‐based heterostructures and devices at atomic scale. [ABSTRACT FROM AUTHOR]