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However, their practical implementation is hindered by the limited ion modulation diversity at the active layer\u2013electrolyte interface. To overcome this limitation, we introduce a metal\u2013organic framework (MOF) as a selective ion\u2010conducting layer to modulate ion\u2010pair dissociation. The MOF layer is based on benzoic acid\u2010modified MIL\u2010125\u2010NH\n                    <jats:sub>2<\/jats:sub>\n                    (BA\u2010MOF), which provides active sites that promote the efficient incorporation of ionic liquid ([EMIM][TFSI]) through intentional defect sites. The defective, highly porous architecture of BA\u2010MOF possesses open\u2010metal sites to tightly bound the ionic liquid. This integration suppresses ion diffusion through BA\u2010MOF, enhancing mobility and overall OECT performance. The effectiveness of this strategy is further demonstrated by MNIST pattern recognition simulations, achieving a maximum accuracy of 94.72%, which is close to the ideal benchmark of 95.22%. This observation is supported by density functional theory (DFT)\u00a0calculations, which revealed that the confinement of [EMIM][TFSI] ion pairs within BA\u2010MOF reduces the ion\u2010pair dissociation energy, thereby leading to an increased concentration of free anions. These findings highlight that defect\u2010sites of MOF not only facilitate ionic\u2010liquid dissociation but also enable and stable synaptic responses, providing a promising strategy for high\u2010performance brain\u2010inspired organic computing.\n                  <\/jats:p>","DOI":"10.1002\/smll.73608","type":"journal-article","created":{"date-parts":[[2026,5,1]],"date-time":"2026-05-01T08:45:15Z","timestamp":1777625115000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Confinement at Defect Sites Dissociates Ionic\u2010Liquid Pairs for Brain\u2010Like Organic Computing"],"prefix":"10.1002","volume":"22","author":[{"given":"Chang Min","family":"Lee","sequence":"first","affiliation":[{"name":"Department of Chemical Engineering Pukyong National University  Busan Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hye 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