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However, considering the advancements in materials and device performance, it is necessary to reexamine the photoelectric conversion in current\u2010stage efficient OSCs. Here, we propose that the conjugated materials with specific three\u2010dimensional donor\u2010acceptor conjugated packing potentially exhibit distinctive charge photogeneration mechanism, which spontaneously split Wannier\u2010Mott excitons to free carriers in pure phases. Subsequently, the pure planar p\u2010n heterojunction (PHJ) OSCs based on green orthogonal solvents were prepared and exhibited comparable even greater performance to that of BHJ OSCs. More interestingly, by introducing PVDF\u2010TrFE as intrinsic region to regulate built\u2010in electric field of the device, the planar p\u2010i\u2010n PHJ OSCs achieved much higher efficiency (&gt;18%) and stability. Moreover, a prominent efficiency of over 19% has been obtained via ternary optimization, which is the new efficiency record for PHJ OSCs up to date. This study points towards the distinguishing intrinsic free charge generation mechanism, opens up a new avenue for OSCs to collectively realize high\u2010efficiency, long\u2010term duration, and simplified device engineering for future commercialization.<\/jats:p>","DOI":"10.1002\/anie.202417143","type":"journal-article","created":{"date-parts":[[2025,1,8]],"date-time":"2025-01-08T01:54:42Z","timestamp":1736301282000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":29,"title":["Revealing Intrinsic Free Charge Generation: Promoting the Construction of Over 19% Efficient Planar p\u2010n Heterojunction Organic Solar Cells"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1980-8507","authenticated-orcid":false,"given":"Junjie","family":"Wang","sequence":"first","affiliation":[{"name":"Key Laboratory of Photoelectric Conversion and Utilization of Solar Energy Qingdao Institute of Bioenergy and 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