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Therefore, it is imperative to develop efficient organic photovoltaic materials compatible with halogen\u2010free solvents. Herein, a series of benzo[<jats:italic>a<\/jats:italic>]phenazine (BP)\u2010core\u2010based small\u2010molecule acceptors (SMAs) achieved through an isomerization chlorination strategy is presented, comprising unchlorinated NA1, 10\u2010chlorine substituted NA2, 8\u2010chlorine substituted NA3, and 7\u2010chlorine substituted NA4. Theoretical simulations highlight NA3's superior orbit overlap length and tight molecular packing, attributed to interactions between the end group and BP unit. Furthermore, NA3 demonstrates dense 3D network structures and a record electronic coupling of 104.5 meV. These characteristics empower the ortho\u2010xylene (<jats:italic>o<\/jats:italic>\u2010XY) processed PM6:NA3 device with superior power conversion efficiency (PCE) of 18.94%, surpassing PM6:NA1 (15.34%), PM6:NA2 (7.18%), and PM6:NA4 (16.02%). Notably, the significantly lower PCE in the PM6:NA2 device is attributed to excessive self\u2010aggregation characteristics of NA2 in <jats:italic>o<\/jats:italic>\u2010XY. Importantly, the incorporation of D18\u2010Cl into the PM6:NA3 binary blend enhances crystallographic ordering and increases the exciton diffusion length of the donor phase, resulting in a ternary device efficiency of 19.75% (certified as 19.39%). These findings underscore the significance of incorporating new electron\u2010deficient units in the design of efficient SMAs tailored for environmentally benign solvent processing of OSCs.<\/jats:p>","DOI":"10.1002\/adma.202407517","type":"journal-article","created":{"date-parts":[[2024,8,14]],"date-time":"2024-08-14T02:55:06Z","timestamp":1723604106000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":112,"title":["Approaching 20% Efficiency in Ortho\u2010Xylene Processed Organic Solar Cells by a Benzo[<i>a<\/i>]phenazine\u2010Core\u2010Based 3D Network Acceptor with Large Electronic Coupling and Long Exciton Diffusion Length"],"prefix":"10.1002","volume":"36","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3503-828X","authenticated-orcid":false,"given":"Zhenghui","family":"Luo","sequence":"first","affiliation":[{"name":"Guangdong Provincial Key Laboratory of New Energy Materials Service Safety Shenzhen Key Laboratory of New Information Display and Storage Materials College of Materials Science and Engineering Shenzhen University  Shenzhen 518060 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weifei","family":"Wei","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of New Energy Materials Service Safety Shenzhen Key Laboratory of New Information Display and Storage Materials College of Materials Science and Engineering Shenzhen University  Shenzhen 518060 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruijie","family":"Ma","sequence":"additional","affiliation":[{"name":"Department of Electronic and Information Engineering Research Institute for Smart Energy (RISE) Guangdong\u2010Hong Kong\u2010Macao (GHM) Joint Laboratory for Photonic\u2010Thermal\u2010Electrical Energy Materials and Devices The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong 999077 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