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Three novel multiple resonances thermally activated delayed fluorescence (MR\u2010TADF) emitters A\u2010BN, DA\u2010BN, and A\u2010DBN, have been successfully synthesized by integrating highly rigid and three\u2010dimensional adamantane\u2010containing spirofluorene units into the MR framework. These molecules form two distinctive functional parts: part\u20051 comprises a boron\u2010nitrogen (BN)\u2010MR framework with adjacent benzene and fluorene units forming a central luminescent core characterized by an exceptionally rigid planar geometry, allowing for narrow FWHM values; part\u20052 includes peripheral mesitylene, benzene, and adamantyl groups, creating a unique three\u2010dimensional \u201cumbrella\u2010like\u201d conformation to mitigate intermolecular interactions and suppress exciton annihilation. The resulting A\u2010BN, DA\u2010BN, and A\u2010DBN exhibit remarkably narrow FWHM values ranging from 18 to 14\u2005nm and near\u2010unity photoluminescence quantum yields. Particularly, OLEDs based on DA\u2010BN and A\u2010DBN demonstrate outstanding efficiencies of 35.0\u2009% and 34.3\u2009%, with FWHM values as low as 22\u2005nm and 25\u2005nm, respectively, effectively accomplishing the integration of high color purity and high device performance.<\/jats:p>","DOI":"10.1002\/anie.202409580","type":"journal-article","created":{"date-parts":[[2024,7,5]],"date-time":"2024-07-05T22:26:17Z","timestamp":1720218377000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":49,"title":["Regional Functionalization Molecular Design Strategy: A Key to Enhancing the Efficiency of Multi\u2010Resonance OLEDs"],"prefix":"10.1002","volume":"63","author":[{"given":"Lin","family":"Wu","sequence":"first","affiliation":[{"name":"Zhejiang Provincial Engineering Research Center of Energy Optoelectronic Materials and Devices, Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences  Ningbo 315201 P. 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