Order-by-order control over the nonlinear optical properties of atomically precise nanoclusters
Ying Xu+, Yan Pu+, Qiong Zhang*, Xi Kang*, Manzhou Zhu
Chin. J. Struct. Chem., 2025, 44(10), 100735. DOI: 10.1016/j.cjsc.2025.100735
October 15, 2025
Metal nanoclusters; Alloying; Fluorescence; Nonlinear optics; Optical limiting
ABSTRACT
It remains highly challenging to achieve the high-order nonlinear optical properties of atomically precise metal nanoclusters via template-maintained manipulation. Here, based on the M1Ag24(SR)18 (M=Ag/Au/Pt/Pd; SR = 2,4-dimethylthiophenol) cluster template, we demonstrated that the innermost kernel alloying rendered these nanoclusters highly controllable towards the nonlinear optics. The Pd-alloyed Pd1Ag24(SR)18 only displayed single-photon-excited fluorescence, while the homo-silver Ag25(SR)18 nanocluster generated the two-photon-excited fluorescence characterization. The Au- and Pt-doped M1Ag24(SR)18 nanoclusters showed high-order three- and four-photon-excited fluorescence, respectively, demonstrating that the order-by-order control over the nonlinear optics of nanoclusters has been accomplished. Moreover, Pt1Ag24(SR)18 with high-order nonlinear optical characterization exhibited the best optical limiting performance under 1000 nm excitation, in agreement with its most prominent nonlinear optical property. Overall, this work presents an intriguing cluster template that enables successive order control over the nonlinear optics of atomically precise metal nanoclusters, hopefully paving the way for developing cluster-based nanomaterials with customized optical characterizations.
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