Overcoming Efficiency Limitation of Cluster Light-Emitting Diodes with Asymmetrically Functionalized Biphosphine Cu4I4 Cubes

Abstract

Electroluminescent (EL) nanoclusters holding promise for new-generation cluster light-emitting devices (CLEDs) rapidly emerge. However, slow radiation and serious quenching of cluster emitters largely limit the device performance. Herein, we report two monofunctionalized biphosphine chelated Cu₄I₄ clusters [DMACDBFDP]₂Cu₄I₄ and [DPACDBFDP]₂Cu₄I₄. The asymmetric modification and electron-donating effect of acridine groups lead to the iodine-to-ligand charge transfer predominant excited states of the clusters, which feature thermally activated delayed fluorescence with markedly improved singlet radiative rate constants and reduced triplet nonradiative rate constants. As consequence, compared to the nonfunctionalized parent cluster, [DPACDBFDP]₂Cu₄I₄ achieves 16-fold increased photoluminescence (81%) and 20-fold increased EL (19.5%) quantum efficiencies. Such new-record efficiencies make CLEDs achieve the state-of-the-art performance of all kinds of EL technologies.