Controlled Synthesis of Lead-Free Double Perovskite Colloidal Nanocrystals for Nonvolatile Resistive Memory Devices

Although lead-free double perovskites such as Cs₂AgBiBr₆ have been widely explored, they still remain a daunting challenge for the controlled synthesis of lead-free double perovskite nanocrystals with highly tunable morphology and band structure. Here, we report the controlled synthesis of lead-free double perovskite colloidal nanocrystals including Cs₂AgBiBr₆ and Cs₂AgIn_xBi_1-xBr₆ via a facile wet-chemical synthesis method for the fabrication of high-performance nonvolatile resistive memory devices. Cs₂AgBiBr₆ colloidal nanocrystals with well-defined cuboidal, hexagonal, and triangular morphologies are synthesized through a facile wet-chemical approach by tuning the reaction temperature from 150 to 190 °C. Further incorporating indium into Cs₂AgBiBr₆ to synthesize alloyed Cs₂AgIn_xBi_1-xBr₆ nanocrystals not only can induce the indirect-to-direct bandgap transition with enhanced photoluminescence but also can improve its structural stability. After optimizing the active layers and device structure, the fabricated Ag/polymethylene acrylate@Cs₂AgIn_0.25Bi_0.75Br₆/ITO resistive memory device exhibits a low power consumption (the operating voltage is ∼0.17 V), excellent cycling stability (>10 000 cycles), and good synaptic property. Our study would enable the facile wet-chemical synthesis of lead-free double perovskite colloidal nanocrystals in a highly controllable manner for the development of high-performance resistive memory devices. © 2023 American Chemical Society.