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However, deterministic multilayer assembly remains challenging due to pervasive interlayer interdiffusion and the lack of generally applicable high-precision deposition strategies. Here, we introduce programmable organic quasi-superlattices enabled by the integration of air\u2013water interfacial monolayer assembly with sequential transfer stacking, allowing polymeric semiconductors to be organized into periodic architectures with molecular-layer precision. By systematically tuning the number of periods, the intraperiod composition, and the thickness of the tunneling spacers, these quasi-superlattices exhibit markedly enhanced photoconductive performance, achieving signal-to-noise ratios of up to 2 \u00d7 106 under white-light illumination together with an ultralow dark current density on the order of 10\u201310\u201310\u201311 A cm\u20132. Superlattices optimized for near-infrared detection (900 nm) achieve a detectivity of 2.06 \u00d7 1012 Jones and a photoresponse time of less than 0.2 s under ultralow illumination (21 \u03bcW cm\u20132). These findings establish programmable molecular organization as a general strategy for accessing emergent optoelectronic functionality from vast chemical spaces via the controlled assembly of organic multilayer architectures.<\/jats:p>","DOI":"10.1021\/jacs.6c10274","type":"journal-article","created":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T16:26:08Z","timestamp":1788452768000},"page":"38904-38912","source":"Crossref","is-referenced-by-count":0,"title":["Programmable Organic\nQuasi-Superlattices with Molecular-Monolayer\nPrecision for Enhanced Photoconductive Response"],"prefix":"10.1021","volume":"148","author":[{"given":"Wenbin","family":"Li","sequence":"first","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"Wang","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhumin","family":"Yu","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun","family":"Li","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming","family":"Li","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Baichuan","family":"Jiang","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cailing","family":"Ou","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tingyu","family":"Ji","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nannan","family":"Dou","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoru","family":"Cao","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zixiao","family":"Han","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1237-3229","authenticated-orcid":true,"given":"Lei","family":"Zhang","sequence":"additional","affiliation":[{"name":"Nanjing University , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,2]]},"reference":[{"issue":"3","key":"2026091609114944700_cit1","doi-asserted-by":"publisher","first-page":"164","DOI":"10.1038\/s41928-022-00718-w","article-title":"Scaled\nindium oxide transistors fabricated using atomic layer deposition","volume":"5","author":"Si","year":"2022","journal-title":"Nat. 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