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The compound allows direct excitation of the charge transfer (CT) state, whose energy can be modulated by solvent polarity, providing controlled access to distinct photophysical pathways and promoting triplet formation. This discovery not only addresses the unpredictability of ISC efficiency in twisted \u03c0\u2010conjugated systems but also overcomes the fundamental design constraints of SOCT\u2010ISC, specifically regarding molecular orthogonality and energy dissipation during the CT process. The resulting photosensitizer, FQAOPBI, exhibits broad absorption (300\u2013600\u00a0nm), higher triplet excited state energy (1.5\u00a0eV), a long\u2010lived triplet excited state (101 \u00b5s), and an unprecedented ISC efficiency (\n                    <jats:italic>\u03a6<\/jats:italic>\n                    <jats:sub>\u0394<\/jats:sub>\n                    = 95%). Notably, this PBI derivative was utilized for the first time in energy\u2010transfer\u2010based upconversion, achieving a remarkable efficiency of 13.1%. Furthermore, as a benchmark twisted \u03c0\u2010conjugated material, FQAOPBI was shown to be a highly efficient photocatalyst for green light\u2010driven photooxidation and atom\u2010transfer radical polymerization. These findings are expected to inspire innovative approaches to photosensitizer design, as well as to play a significant role in promoting diverse photochemical applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.2464659","type":"journal-article","created":{"date-parts":[[2026,7,11]],"date-time":"2026-07-11T17:15:07Z","timestamp":1783790107000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Controllable and Exceptionally Efficient Spin\u2010Orbit Charge\u2010Transfer Intersystem Crossing in Twisted \u03c0\u2010Conjugated Perylene Bisimides for High\u2010Performance Photochemical Applications"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-7298-0998","authenticated-orcid":false,"given":"Hui","family":"Liang","sequence":"first","affiliation":[{"name":"Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices Hubei University of Arts and Science  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