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Herein, oxygen (O), sulfur (S), and nitrogen (N) atoms are adopted to bridge the 2D conjugated central cores, yielding three acceptor platforms of CH\u2500O, CH\u2500S, and CH\u2500N that differ in structure by only two atoms. Because of the characteristic atomic outer electron configuration and hybrid orbital orientation, O\u2010, S\u2010, and N\u2010bridged central cores display quite different conformations and electronic properties, namely, dibenzodioxin (planar, non\u2010aromatic), thianthrene (puckered, non\u2010aromatic) and phenazine (planar, aromatic), respectively. A systematic investigation discloses how the central core, especially its p\u2010\u03c0 orbital overlap between lone pair on O\/S\/N and coterminous benzene planes, affect the intrinsic photoelectronic properties of acceptors for the first time. Finally, CH\u2500N\u2010based binary device affords the highest fill factor of 83.13% in organic photovoltaics along with a first\u2010class efficiency of 20.23%. By evaluating the strictly controlled O\u2010, S\u2010, and N\u2010bridged molecular platforms comprehensively, the work reveals the potential uniqueness of diimide in determining the excellent photovoltaic outcomes of acceptors.<\/jats:p>","DOI":"10.1002\/adma.202503131","type":"journal-article","created":{"date-parts":[[2025,5,6]],"date-time":"2025-05-06T03:35:53Z","timestamp":1746502553000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":29,"title":["O, S, and N Bridged Atoms Screening on 2D Conjugated Central Units of High\u2010Performance Acceptors"],"prefix":"10.1002","volume":"37","author":[{"given":"Xiangjian","family":"Cao","sequence":"first","affiliation":[{"name":"State Key Laboratory and Institute of Elemento\u2010Organic Chemistry The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials Renewable Energy Conversion and Storage Center (RECAST) Frontiers Science Center for New 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