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However, their potential is limited by poor electron mobility and suboptimal reaction kinetics. This study explores polarization engineering to modify the local electronic structure of the biaryl units within vinylene\u2010linked COFs. By implementing a conformation\u2010locking strategy that strategically enhances N\n                    <jats:sup>+<\/jats:sup>\n                    polarization and the redox activity of the framework, this design not only decreases the interfacial Schottky barrier but also facilitates efficient electron transfer, thereby promoting the delocalization of framework electrons, which modulates the conductive state in organic memristors. Furthermore, the polarization of ions, amplified by pyridine nitrogen nuclei and robust interlayer stacking, ensures effective counterion deintercalation and migration. The constructed Al\/COF\u2010DIBPY\/Au memristor exhibits a high analog on\u2010off current ratio (I\n                    <jats:sub>max<\/jats:sub>\n                    \/I\n                    <jats:sub>min<\/jats:sub>\n                    = 15.7) under a 0.5 V drive. Utilizing these properties, the device shows great potential in performing speech emotion recognition tasks. When integrated into a convolutional neural network, it achieves a learning recognition accuracy of up to 95% in these tasks. This research offers novel insights into the construction of high\u2010efficiency neuromorphic computing devices based on polarization\u2010modulated COFs.\n                  <\/jats:p>","DOI":"10.1002\/advs.76639","type":"journal-article","created":{"date-parts":[[2026,7,14]],"date-time":"2026-07-14T13:13:44Z","timestamp":1784034824000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Polarization Engineering in Vinylene\u2010Linked COFs Toward Efficient Neuromorphic Computing"],"prefix":"10.1002","volume":"13","author":[{"given":"Hao","family":"Wang","sequence":"first","affiliation":[{"name":"Key Laboratory for Advanced Materials School of Chemistry and Molecular Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lei","family":"Zhao","sequence":"additional","affiliation":[{"name":"Key Laboratory for Advanced Materials School 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