Science Advances · 2019 · 132 citations · 36 references
Natural SciencesChemistryMaterials ScienceElectronic MaterialsOptical MaterialsOptoelectronicsCluster ChemistryCluster CompoundsLight-emitting DiodesLuminescent MaterialsOptoelectronic DevicesOptoelectronic MaterialsDelocalized Molecular OrbitalsElectroluminescenceElectron-donating GroupsExternal Quantum EfficiencyOptoelectronic PropertiesOrganic Light-emitting DiodesPhotoluminescence Quantum YieldQuantum Efficiency
Organic light-emitting diodes using cluster emitters have recently emerged as a flexible optoelectronic platform to extend their biological and optical applications. However, their inefficient cluster-centered excited states and deficient electrical properties limit device performance. Here, we introduce donor groups in organic ligands to form ligand-activated clusters, enabling the fabrication of the first cluster-based sky blue-emitting device with a record 30- and 8-fold increased luminance and external quantum efficiency up to ~7000 nits and ~8%, respectively. We show that the electron-donating effect of donor groups can enhance ligand-centered transitions and thoroughly eliminate cluster-centered excited states by delocalizing the molecular transition orbitals from the cluster unit to the ligand, leading to 13-fold increased photoluminescence quantum yield. In turn, the excellent rigidity and photostability of the cluster unit improve the color purity and efficiency stability of the devices. These results will motivate the further development of high-performance optoelectronic clusters by ligand engineering.
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Density-functional thermochemistry. III. The role of exact exchange
Axel D. Becke · The Journal of Chemical Physics · 1993 · 102.8K citations
Natural Sciences, Chemistry, Physics +13
Richard L. Martin · The Journal of Chemical Physics · 2003 · 2.7K citations
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Zhikun Wu, Rongchao Jin · Nano Letters · 2010 · 1.4K citations