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However, their generally sluggish reverse intersystem crossing (RISC) limits efficient triplet harvesting, thereby constraining device performance and stability. Here, a selenophene \u03c0\u2010core fusion strategy is developed based on a prototypical MR scaffold, in which the central benzene unit is replaced with a selenium\u2010embedded dibenzo[b,d]selenophene (DBSe) \u03c0\u2010core. This structural transformation generates a redefined \u03c0\u2010extended MR framework that simultaneously preserves narrowband emission and accelerates RISC through enhanced spin\u2013orbit coupling, while extending the emission wavelength via para N\u2013\u03c0\u2013Se conjugation. Subsequent peripheral donor engineering further stabilizes the excited state, enabling stepwise bathochromic shifts from green to red emission (520\u2013600\u00a0nm). The resulting DBSe\u2010based emitters exhibit ultrafast RISC rates of up to 10\n                    <jats:sup>7<\/jats:sup>\n                    s\n                    <jats:sup>\u22121<\/jats:sup>\n                    and afford narrowband green\u2010to\u2010red TADF\u2010OLEDs with external quantum efficiencies exceeding 30%, accompanied with suppressed efficiency roll\u2010off and prolonged operational lifetimes. These findings demonstrate that efficient triplet harvesting and long\u2010wavelength narrowband emission can be integrated within a single emitter platform and establish DBSe \u03c0\u2010core fusion as an effective design strategy for next\u2010generation high\u2010performance MR\u2010TADF materials and OLED technologies.\n                  <\/jats:p>","DOI":"10.1002\/anie.2882594","type":"journal-article","created":{"date-parts":[[2026,8,25]],"date-time":"2026-08-25T11:34:57Z","timestamp":1787657697000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Selenophene \u03c0\u2010Core Fusion for Simultaneous Fast Reverse Intersystem Crossing and Narrowband Long\u2010Wavelength TADF"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-7267-9728","authenticated-orcid":false,"given":"Jingpeng","family":"Zhang","sequence":"first","affiliation":[{"name":"Department of Applied Chemistry 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