Dual Redox-active Covalent Organic Framework-based Memristors for Highly-efficient Neuromorphic Computing.

Organic memristors based on covalent organic frameworks (COFs) exhibit significant potential for future neuromorphic computing applications. The preparation of high-quality COF nanosheets through appropriate structural design and building block selection is critical for the enhancement of memristor performance. In this study, a novel room-temperature single-phase method was used to synthesize Ta-Cu3 COF, which contains two redox-active units: trinuclear copper and triphenylamine. The resultant COF nanosheets were dispersed through acid-assisted exfoliation and subsequently spin-coated to fabricate a high-quality COF film on an indium tin oxide (ITO) substrate. The synergistic effect of the dual redox-active centers in the COF film, combined with its distinct crystallinity, significantly reduces the redox energy barrier, enabling the efficient modulation of 128 non-volatile conductive states in the Al/Ta-Cu3 COF/ITO memristor. Utilizing a convolutional neural network (CNN) based on these 128 conductance states, image recognition for ten representative campus landmarks was successfully executed, achieving a high recognition accuracy of 95.13% after 25 training epochs. Compared to devices based on binary conductance states, the memristor with 128 conductance states exhibits a 45.56% improvement in recognition accuracy and significantly enhances the efficiency of neuromorphic computing.

Molecular-Potential and Redox Coregulated Cathodic Electrosynthesis toward Ionic Azulene-Based Thin Films for Organic Memristors.

Organic memristors as promising electronic units are attracting significant attention owing to their simplicity of molecular structure design. However, fabricating high-quality organic films via novel synthetic technologies and exploring unprecedented chemical structures to achieve excellent memory performance in organic memristor devices are highly challenging. In this work, we report a cathodic electropolymerization to synthesize an ionic azulene-based memristive film (PPMAz-Py+Br-) under the molecular-potential and redox coregulation. During the cathodic electropolymerization process, electropositive pyridinium salts migrate to the cathode under an electric field, undergo a reduction-coupling deprotonation reaction, and polymerize into a uniform film with a controllable thickness on the electrode surface. The prepared Al/PPMAz-Py+Br-/ITO devices not only exhibit a high ON/OFF ratio of 1.8 × 103, high stability, long memory retention, and endurance under a wide range of voltage scans, but also achieve excellent multilevel storage and history-dependent memristive performance. In addition, the devices can mimic important biosynaptic functions, such as learning/forgetting function, synaptic enhancement/inhibition, paired-pulse facilitation/depression, and spiking-rate-dependent plasticity. The tunable memristive performances are attributed to the capture of free electrons on pyridinium cations, the migration of the aluminum ions (Al3+), and the form of Al conductive filaments under voltage scans.

MoS2 Quantum Dot-Optimized Conductive Channels for a Conjugated Polymer-Based Synaptic Memristor.

Donor-acceptor-type conjugated polymers are widely used in memristors due to their unique push-pull electron structures and charge transfer mechanisms. However, the inherently inhomogeneous microstructure of polymer films and their low crystallinity produce randomness that destabilizes formed conductive channels, giving polymer-based memristors unstable switching behavior. In this contribution, we prepared a synaptic device based on PM6-MoS2 QD (molybdenum disulfide quantum dot) nanocomposites. In the composites, MoS2 QDs provided the active centers for forming conductive channels via electron trapping and detrapping. They also controlled the directional formation of conductive channels between PM6 and MoS2 QDs, reducing randomness and giving devices a narrow switching voltage range and cycling longevity. The device exhibited continuous multistage conductance states under a direct current voltage sweep and simulated a variety of synaptic functions, including long-term potentiation, long-term depression, short-term potentiation, short-term depression, paired-pulse facilitation, spiking-rate-dependent plasticity, and "learning experience" behavior. The memristor could also perform arithmetic, including "counting" and "subtraction" operations. This work provides a new approach to improving the performance of memristors for neuromorphic computing.

Interface-confined synthesis of a nonplanar redox-active covalent organic framework film for synaptic memristors.

The development of novel synthetic methodologies and unprecedented structures of covalent organic framework (COF) films is of great importance for exploring their potential applications in optoelectronic devices, sensors, and membrane separation. From the point of view of monomer selection, rigid building blocks are always the first choice for synthesizing crystalline COF films. However, the preparation of COF films with flexible building units remains challenging. Herein, by introducing flexible triphenylamine-based building units, a nonplanar COF film (TFPA-TAPA film) is fabricated via liquid-liquid interface-confined synthesis at room temperature and atmospheric pressure. The growth mechanism of the flexible building units at the liquid-liquid interface is related to the transformation of strip-type slices into free-standing COF films by dynamic covalent chemistry. As a proof-of-concept, the as-fabricated Al/TFPA-TAPA/ITO device shows excellent multilevel storage and history-dependent memristive switching behavior. The synaptic potentiation/depression, human learning and memorization functions, as well as the transition from short-term synaptic plasticity to long-term plasticity, are successfully emulated by using this synaptic memristor.

Novel Ternary Heterogeneous Reduction Graphene Oxide (RGO)/BiOCl/TiO2 Nanocomposites for Enhanced Adsorption and Visible-Light Induced Photocatalytic Activity toward Organic Contaminants.

Herein, we describe a simple and cost-effective design for the fabrication of a novel ternary RGO/BiOCl/TiO2 nanocomposites through a simple hydrothermal process. The prepared nanocomposites were characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (UV-vis DRS) and N2 adsorption-desorption analysis. Organic contaminants-such as methylene blue (MB), methyl orange (MO), rhodamine B (RhB) and amido black-10B (AB-10B)-were employed as the target pollutants to evaluate the adsorption capacity and photocatalytic activity of RGO/BiOCl/TiO2 nanocomposites. From experimental data, it was also found that the amount of TiO2 impressed the photocatalytic performance, and the nanocomposites with 10% of TiO2 showed the best photocatalytic activity. The improved photocatalytic performance may be mainly due to the narrow band gap, and the charge separation and migration of RGO. Moreover, good recyclability was obtained from RGO/BiOCl/TiO2 nanocomposites, and scavenger tests indicated that photogenerated holes were the main active species in the reaction system. Therefore, the prepared RGO/BiOCl/TiO2 nanocomposites have broad applications foreground in pollutants purification.