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.

中文翻译：

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用于有机忆阻器的离子甘菊基薄膜的分子势和氧化还原共调节阴极电合成

有机忆阻器作为有前途的电子单元由于其分子结构设计的简单性而引起了人们的广泛关注。然而，通过新颖的合成技术制造高质量的有机薄膜并探索前所未有的化学结构以在有机忆阻器器件中实现优异的存储性能非常具有挑战性。在这项工作中，我们报告了在分子势和氧化还原共调节下阴极电聚合合成基于离子甘菊环的忆阻膜（PPMAz-Py ⁺ Br ^– ）。在阴极电聚合过程中，带正电的吡啶鎓盐在电场作用下迁移到阴极，发生还原偶联去质子化反应，并在电极表面聚合成厚度可控的均匀薄膜。所制备的Al/PPMAz-Py ⁺ Br ^{– /ITO器件不仅表现出1.8×10 3}的高开关比、高稳定性、长记忆保持力和大范围电压扫描下的耐久性，而且还实现了优异的多电平存储和历史相关的忆阻性能。此外，该装置可以模仿重要的生物突触功能，例如学习/遗忘功能、突触增强/抑制、配对脉冲促进/抑制以及尖峰速率依赖性可塑性。可调节的忆阻性能归因于吡啶鎓阳离子上自由电子的捕获、铝离子(Al ³⁺ )的迁移以及电压扫描下Al导电丝的形成。