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However, its generality remains limited by the intrinsic trade\u2010offs in existing photosensitizers (PSs). Noble metal (e.g., Ir, Ru) complexes offer high efficiency yet suffer from cost and sustainability concerns, while organic carbonyl sensitizers suffer from weak visible\u2010light absorption and short\u2010lived triplet states. Herein, we report heavy\u2010atom\u2010free organic PSs featuring a multi\u2010channel through\u2010space charge transfer (TSCT) architecture within a thermally activated delayed fluorescence (TADF) framework. A highly twisted donor\u2010acceptor topology enforces near\u2010complete frontier orbital separation, leading to ultralow singlet\u2010triplet energy gaps (\u0394\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>ST<\/jats:sub>\n                    down to 0.013\u00a0eV) and thereby enabling efficient spin interconversion. Consequently, these PSs simultaneously achieve high intersystem crossing (ISC) quantum yields, microsecond\u2010scale triplet lifetimes, and high triplet energies (\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>T<\/jats:sub>\n                    up to 63.7\u00a0kcal mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), rivaling those of state\u2010of\u2010the\u2010art noble\u2010metal systems. Leveraging these features, we demonstrate the first visible\u2010light\u2010driven intermolecular [2 + 2] cycloaddition of 1,3\u2010diphenylphosphindole 1\u2010oxides with alkenes and alkynes, enabling rapid access to structurally complex cyclobutane\u2010fused phosphindole 3\u2010oxides that hold potential value in drug screening but are typically difficult to obtain. Mechanistic studies support a TEnT pathway, in which minimal \u0394\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>ST<\/jats:sub>\n                    and efficient ISC are key to achieving high TEnT reactivity.\n                  <\/jats:p>","DOI":"10.1002\/anie.1444773","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T10:43:31Z","timestamp":1786358611000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Energy Transfer Catalysis Enabled by Multichannel Through\u2010Space Charge Transfer TADF Photosensitizers: [2 + 2] Photocycloaddition to Cyclobutane\u2010Fused Phosphindole 3\u2010Oxides"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-1447-760X","authenticated-orcid":false,"given":"Jingjing","family":"Zhang","sequence":"first","affiliation":[{"name":"Key Laboratory of Green Chemistry and Technology of 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