Thermally activated delayed fluorescence Au‐Ag‐oxo nanoclusters : From photoluminescence to radioluminescence
Yuan, P., Zhang, H., Zhou, Y., He, T., Malola, S., Gutiérrez‐Arzaluz, L., Li, Y., Deng, G., Dong, C., Huang, R., Song, X., Teo, B. K., Mohammed, O. F., Häkkinen, H., Bakr, O. M., & Zheng, N. (2024). Thermally activated delayed fluorescence Au‐Ag‐oxo nanoclusters : From photoluminescence to radioluminescence. Aggregate, Early View. https://doi.org/10.1002/agt2.475
Julkaistu sarjassa
AggregateTekijät
Päivämäärä
2024Tekijänoikeudet
© 2024 The Authors. Aggregate published by SCUT, AIEI, and John Wiley & Sons Australia, Ltd.
Thermally activated delayed fluorescence (TADF) materials have numerous applications in energy conversion and luminescent imaging. However, they are typically achieved as metal-organic complexes or pure organic molecules. Herein, we report the largest Au-Ag-oxo nanoclusters to date, Au18Ag26(R1COO)12(R2C≡C)24(μ4-O)2(μ3-O)2 (Au18Ag26, where R1 = CH3-, Ph-, CHOPh- or CF3Ph-; R2 = Ph- or FPh-). These nanoclusters exhibit exceptional TADF properties, including a small S1-T1 energy gap of 55.5 meV, a high absolute photoluminescence quantum yield of 86.7%, and a microseconds TADF decay time of 1.6 μs at ambient temperature. Meanwhile, Au18Ag26 shows outstanding stability against oxygen quenching and ambient conditions. Atomic level analysis reveals the strong π⋯π and C-H⋯π interactions from the aromatic alkynyl ligands and the enhancement of metal-oxygen-metal interactions by centrally coordinated O2−. Modeling of the electronic structure shows spatially separated highest occupied molecular orbital and lowest unoccupied molecular orbital, which promote charge transfer from the ligand shell, predominantly carboxylate ligands, to O2−-embedded metal core. Furthermore, TADF Au-Ag-oxo nanoclusters exhibit promising radioluminescence properties, which we demonstrate for X-ray imaging. Our work paves the way for the design of TADF materials based on large metal nanoclusters for light-emission and radioluminescence applications.
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Julkaisija
John Wiley & SonsISSN Hae Julkaisufoorumista
2692-4560Asiasanat
Julkaisu tutkimustietojärjestelmässä
https://converis.jyu.fi/converis/portal/detail/Publication/197719171
Metadata
Näytä kaikki kuvailutiedotKokoelmat
Rahoittaja(t)
Suomen AkatemiaRahoitusohjelmat(t)
Akatemiaprofessorin tehtävä, SA; Akatemiaprofessorin tutkimuskulut, SALisätietoja rahoituksesta
The authors acknowledge the National Natural Science Foundation of China (grant numbers: 92261207 and 21890752) and NSFC Center for Single-Atom Catalysis (grant number: 22388102), the New Cornerstone Science Foundation, the 111 Project (grant number: B08027) and the King Abdullah University of Science and Technology (KAUST) for financial support. The computational work at the University of Jyväskylä was supported by the Academy of Finland (grant numbers: 292352 and 319208). ...Lisenssi
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