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Herein, we report a solvent\u2010mediated infiltration doping strategy to overcome these challenges based on D18\/L8\u2010BO layer\u2010by\u2010layer (LBL) system. By incorporating F4TCNQ as the p\u2010type dopant in the donor layer and DMBI as the n\u2010type dopant in the acceptor layer, with controlled infiltration via a chlorobenzene:ethanol (CB:EtOH) binary solvent mixture, we constructed a polarized heterojunction that mitigates dopant crosstalk. This approach reduces trap depths (activation energy\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>a<\/jats:sub>\n                    \u00a0=\u00a00.2\u00a0eV vs. 0.84\u00a0eV for direct doping) and narrows lowest unoccupied molecular orbital (LUMO) density of states while enhancing built\u2010in potential and hole transfer rate (\n                    <jats:italic>\u03c4<\/jats:italic>\n                    <jats:sub>1<\/jats:sub>\n                    \u00a0=\u00a00.40\u00a0ps). Consequently, the optimized devices achieved a power conversion efficiency (PCE) of 20.5%, with a fill factor (FF) of 82.3%, surpassing control (19.5%) and direct doping (19.1%) configurations. These findings highlight the efficacy of spatially controlled doping for advancing high\u2010efficiency, scalable OPVs toward sustainable energy applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.202521265","type":"journal-article","created":{"date-parts":[[2025,11,25]],"date-time":"2025-11-25T06:16:59Z","timestamp":1764051419000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Polarized Heterojunction in a Doubly Doped Layer\u2010by\u2010Layer Structure to Obtain an Organic Photovoltaic Device of 20.5% Efficiency"],"prefix":"10.1002","volume":"65","author":[{"given":"Qun","family":"Yin","sequence":"first","affiliation":[{"name":"Faculty of Chemical Engineering and Energy Technology Shanghai Institute of Technology  Shanghai 201418 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xingyu","family":"Gao","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules Center of Hydrogen Science In\u2010situ Center of Physical Science Shanghai Jiao Tong University  Shanghai 200240 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinyang","family":"Yu","sequence":"additional","affiliation":[{"name":"Department of Chemistry Zhejiang University  Hangzhou 310027 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lixuan","family":"Kan","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules Center of Hydrogen Science In\u2010situ Center of Physical Science Shanghai Jiao Tong University  Shanghai 200240 P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fei","family":"Han","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules Center of Hydrogen Science In\u2010situ Center of Physical Science Shanghai Jiao Tong University  Shanghai 200240 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haiming","family":"Zhu","sequence":"additional","affiliation":[{"name":"Department of Chemistry Zhejiang University  Hangzhou 310027 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Supeng","family":"Pei","sequence":"additional","affiliation":[{"name":"Faculty of Chemical Engineering and Energy Technology Shanghai Institute of Technology  Shanghai 201418 P.R. 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