Wu XChen, DGDGChenLiu, DHDHLiuLiu, SHSHLiuShen, SWSWShenWu, CICIWuXie, GHGHXieZhou, JWJWZhouHuang, ZXZXHuangHuang, CYCYHuangSu, SJSJSuZhu, WGWGZhuCHIH-I WUPI-TAI CHOU2021-09-022021-09-02202000027863https://www.scopus.com/inward/record.uri?eid=2-s2.0-85086589808&doi=10.1021%2fjacs.9b13956&partnerID=40&md5=7ed8a30327398115ad2bcd23183a189chttps://scholars.lib.ntu.edu.tw/handle/123456789/580708Dinuclear Pt(III) complexes were commonly reported to have short-lived lowest-lying triplet states, resulting in extremely weak or no photoluminescence. To overcome this obstacle, a new series of dinuclear Pt(III) complexes, named Pt2a-Pt2c, were strategically designed and synthesized using donor (D)-acceptor (A)-type oxadiazole-thiol chelates as bridging ligands. These dinuclear Pt(III) complexes possess a d7-d7 electronic configuration and exhibit intense phosphorescence under ambient conditions. Among them, Pt2a exhibits orange phosphorescence maximized at 618 nm in degassed dichloromethane solution (φp ? 8.2%, τp ? 0.10 μs) and near-infrared (NIR) emission at 749 nm (φp ? 10.1% τp ? 0.66 μs) in the crystalline powder and at 704 nm (φp ? 33.1%, τp ? 0.34 μs) in the spin-coated neat film. An emission blue-shifted by more than 3343 cm-1 is observed under mechanically ground crystalline Pt2a, affirming intermolecular interactions in the solid states. Time-dependent density functional theory (TD-DFT) discloses the lowest-lying electronic transition of Pt2a-Pt2c complexes to be a bridging ligand-metal-metal charge transfer (LMMCT) transition. The long-lived triplet states of these dinuclear platinum(III) complexes may find potential use in lighting. Employing Pt2a as an emitter, high-performance organic light-emitting diodes (OLEDs) were fabricated with NIR emission at 716 nm (η = 5.1%), red emission at 614 nm (η = 8.7%), and white-light emission (η = 11.6%) in nondoped, doped (in mCP), and hybrid (in CzACSF) devices, respectively. Copyright ? 2020 American Chemical Society.Blue shift; Charge transfer; Density functional theory; Dichloromethane; Infrared devices; Ligands; Organic light emitting diodes (OLED); Phosphorescence; Polymer films; Synthesis (chemical); Dichloromethane solutions; Electronic configuration; Electronic transition; Intermolecular interactions; Near-infrared emissions; Organic light emitting diodes(OLEDs); Time dependent density functional theory; White light emission; Platinum compounds; chelate; dichloromethane; ligand; metal; organic compound; platinum complex; thiol; Article; blue light; chemical analysis; chemical structure; crystal structure; density functional theory; devices; ligand binding; molecular interaction; phosphorescence; photoluminescence; powder; red light; synthesis; time factor; white light[SDGs]SDG7journal article10.1021/jacs.9b139562-s2.0-85086589808