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Herein, through introducing sulfur atoms into isomeric pentaphene and pentacene frameworks, we demonstrate a set of polycyclic luminophores exhibiting efficient TADF and RTP characters. The incorporation of sulfur atoms confirms a folded molecular plane, while intensifies singlet\u2013triplet spin\u2010orbit coupling. Further, the isomeric effect has a significant effect on the electronic structure of excited state, giving rise to the investigated compounds tunable luminescence mechanisms of TADF and RTP. With efficient triplet harvesting ability, maximum external quantum efficiencies up to 25.1\u2009% and 8.7\u2009% are achieved for the corresponding TADF and RTP OLEDs, verifying the great potential of sulfur\u2010bridged frameworks for highly efficient devices.<\/jats:p>","DOI":"10.1002\/anie.202209343","type":"journal-article","created":{"date-parts":[[2022,7,11]],"date-time":"2022-07-11T15:39:41Z","timestamp":1657553981000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":125,"title":["Molecular Engineering of Sulfur\u2010Bridged Polycyclic Emitters Towards Tunable TADF and RTP Electroluminescence"],"prefix":"10.1002","volume":"61","author":[{"given":"Mengke","family":"Li","sequence":"first","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices and Institute of Polymer Optoelectronic Materials and Devices South China University of Technology  Wushan Road 381 Tianhe District, Guangzhou 510640, Guangdong Province P. 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