A Highly Crystalline Single Layer Two-dimensional Polymer for Low Variability and Excellent Scalability Molecular Memristors.

Large-scale growth of highly crystalline single layer two-dimensional polymers (SL-2DPs) and their subsequent integration into memristors is key to advancing the development of high-density data storage devices. However, leakage problems resulting from the porous structure of 2DPs continue to make such advances extremely challenging. Herein, we overcome this issue by incorporating long alkoxy chains into key molecular building blocks to obtain a highly crystalline 2DP, as visualized by scanning tunnelling microscopy, and prevent metal permeation in the subsequent device fabrication process. SL-2DP memristors constructed via direct evaporation of the top electrodes exhibit low variability (σ Vset = 0.14) due to the single-monomer-thick feature together with the high regular structure and coordination ability which minimizes the stochastic spatial distribution of conductive filaments (CFs) in both vertical and lateral dimensions. The variability was further decreased to 0.04 by confining the formation and fracture of CFs to the interface through the utilization of bilayer junctions. Using peak force tunnelling atomic force microscopy, we demonstrate the nanometre scalability (< 50 nm 2 ) and low power consumption of these molecular memristor devices. This article is protected by copyright. All rights reserved.