Rationally Designing High‐Performance Versatile Organic Memristors through Molecule‐Mediated Ion Movements

Abstract Organic memory has attracted tremendous attention for next‐generation electronic elements for the molecules’ striking ease of structural design. However, due to them being hardly controllable and their low ion transport, it is always essential and challenge to effectively control their random migration, pathway, and duration. There are very few effective strategies, and specific platforms with a view to molecules with specific coordination‐groups‐regulating ions have been rarely reported. In this work, as a generalized rational design strategy, the well‐known tetracyanoquinodimethane (TCNQ) is introduced with multiple coordination groups and small plane structure into a stable polymers framework to modulate Ag migration and then achieve high‐performance devices with ideal productivity, low operation voltage and power, stable switching cycles, and state retention. Raman mapping demonstrates that the migrated Ag can specially coordinate with the embedded TCNQ molecules. Notably, the TCNQ molecule distribution can be modulated inside the polymer framework and regulate the memristive behaviors through controlling the formed Ag conductive filaments (CFs) as demonstrated by Raman mapping, in situ conductive atomic force microscopy (C‐AFM), X‐ray diffraction (XRD) and depth‐profiling X‐ray photoelectron spectroscopy (XPS). Thus the controllable molecule‐mediated Ag movements show its potential in rationally designing high‐performance devices and versatile functions and is enlightening in constructing memristors with molecule‐mediated ion movements.