Calamitic Blatter Radicals for Large‐Area Solution‐Coated Resistive Memories

Abstract Radical molecules exhibit fast redox kinetics, are widely explored for data processing and energy storage. However, the insulating aliphatic matrix isolates the radical units, thus resulting in a weak charge transporting ability. Herein, calamitic Blatter radicals (CBR) with highly conductive [1]benzothieno[3,2‐ b ]benzothiophene (BTBT) as the conjugated backbone are designed and synthesized. It is found that bistable redox character associated with large conjugated backbone allows these Blatter radical derivatives to be switched with ON/OFF ratio reaching 10 6 and retention time exceeding 10 4 s in solution processed devices. In addition, these radicals are unveiled to perform tunable, multi‐mode field‐responsive resistance behaviors, including write‐once‐read‐many (WORM), FLASH, and dynamic random access memory (DRAM), by molecular engineering strategy. This finding provides fundamental understanding for charge transferring dynamics and redox‐switching mechanism of radical molecules with respect to electronic applications.