One-Dimensional Covalent Organic Framework-Based Multilevel Memristors for Neuromorphic Computing.

Memristors are essential components of neuromorphic systems that mimic the synaptic plasticity observed in biological neurons. In this study, a novel approach employing one-dimensional covalent organic framework (1D COF) films was explored to enhance the performance of memristors. The unique structural and electronic properties of two 1D COF films (COF-4,4'-methylenedianiline (MDA) and COF-4,4'-oxydianiline (ODA)) offer advantages for multilevel resistive switching, which is a key feature in neuromorphic computing applications. By further introducing a TiO2 layer on the COF-ODA film, a built-in electric field between the COF-TiO2 interfaces could be generated, demonstrating the feasibility of utilizing COFs as a platform for constructing memristors with tunable resistive states. The 1D nanochannels of these COF structures contributed to the efficient modulation of electrical conductance, enabling precise control over synaptic weights in neuromorphic circuits. This study also investigated the potential of these COF-based memristors to achieve energy-efficient and high-density memory devices.

Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide.

The artificial photosynthesis of H2O2 from water and oxygen using semiconductor photocatalysts is attracting increasing levels of attention owing to its green, environmentally friendly, and energy-saving characteristics. Although covalent organic frameworks (COFs) are promising materials for promoting photocatalytic H2O2 production owing to their structural and functional diversity, they typically suffer from low charge-generation and -transfer efficiencies as well as rapid charge recombination, which restricts their use as catalysts for photocatalytic H2O2 production. Herein, we report a strategy for anchoring vinyl moieties to a COF skeleton to facilitate charge separation and migration, thereby promoting photocatalytic H2O2 generation. This vinyl-group-bearing COF photocatalyst exhibits a H2O2-production rate of 84.5 µmol h-1 (per 10 mg), which is ten-times higher than that of the analog devoid of vinyl functionality and superior to most reported COF photocatalysts. Both experimental and theoretical studies provide deep insight into the origin of the improved photocatalytic performance. These findings are expected to facilitate the rational design and modification of organic semiconductors for use in photocatalytic applications.

Switching the memory behaviour from binary to ternary by triggering S62- relaxation in polysulfide-bearing zinc-organic complex molecular memories.

The use of crystalline metal-organic complexes with definite structures as multilevel memories can enable explicit structure-property correlations, which is significant for designing the next generation of memories. Here, four Zn-polysulfide complexes with different degrees of conjugation have been fabricated as memory devices. ZnS6(L)2-based memories (L = pyridine and 3-methylpyridine) can exhibit only bipolar binary memory performances, but ZnS6(L)-based memories (L = 2,2'-bipyridine and 1,10-phenanthroline) illustrate non-volatile ternary memory performances with high ON2/ON1/OFF ratios (104.22/102.27/1 and 104.85/102.58/1) and ternary yields (74% and 78%). Their ON1 states stem from the packing adjustments of organic ligands upon the injection of carriers, and the ON2 states are a result of the ring-to-chain relaxation of S62- anions. The lower conjugated degrees in ZnS6(L)2 result in less compact packing; consequently, the adjacent S62- rings are too long to trigger the S62- relaxation. The deep structure-property correlation in this work provides a new strategy for implementing multilevel memory by triggering polysulfide relaxation based on the conjugated degree regulation of organic ligands.

Embedding Azobenzol-Decorated Tetraphenylethylene into the Polymer Matrix to Implement a Ternary Memory Device with High Working Temperature/Humidity.

The development of new high-density memories that can work in harsh environments such as high temperature and humidity will be significant for some special occasions such as oil and geothermal industries. Herein, a facial strategy for implementing a ternary memory device with high working temperature/humidity was executed. In detail, an asymmetric aggregation-induced-emission active molecule (azobenzol-decorated tetraphenylethylene, i.e., TPE-Azo) was embedded into flexible poly(ethylene-alt-maleic anhydride) (PEM) to prepare a TPE-Azo@PEM composite, which served as an active layer to fabricate the FTO/TPE-Azo@PEM/Ag device. This device can demonstrate excellent ternary memory performances with a current ratio of 1:104.2:101.6 for "OFF", "ON1", and "ON2" states. Specially, it can exhibit good environmental endurance at high working temperature (350 °C) and humidity (RH = 90%). The ternary memory mechanism can be explained as the combination of aggregation-induced current/conductance and conformational change-induced charge transfer in the TPE-Azo molecule, which was verified by Kelvin probe force microscopy, UV-vis spectra, X-ray diffraction, and single-crystal structural analysis. This strategy can be used as a universal method for the construction of high-density multilevel memristors with good environmental tolerance.