Designing and synthesizing cuprous halide phosphors unifying efficient low-energy emission and a broad excitation band is still a great challenge. Herein, by rational component design, three novel Cu(i)-based metal halides, DPCu4X6 [DP = (C6H10N2)4(H2PO2)6; X = Cl, Br, I], were synthesized by reacting p-phenylenediamine with cuprous halide (CuX), and they show similar structures, consisting of isolated [Cu4X6]2- units separated by organic layers. Photophysical studies uncover that the highly localized excitons and rigid environment give rise to highly efficient yellow-orange photoluminescence in all compounds with the excitation band spanning from 240 to 450 nm. The bright PL in DPCu4X6 (X = Cl, Br) originates from self-trapped excitons due to the strong electron-phonon coupling. Intriguingly, DPCu4I6 features a dual-band emissive characteristic, attributed to the synergistic effect of halide/metal-to-ligand charge-transfer (X/MLCT) and triplet cluster-centered (3CC) excited states. Benefiting from the broadband excitation, a high-performance white-light emitting diode (WLED) with a high color rendering index of 85.1 was achieved using single-component DPCu4I6 phosphor. This work not only unveils the role of halogens in the photophysical processes of cuprous halides, but also provides new design principles for high-performance single-component WLEDs.
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