Atomically precise nanoclusters (NCs) exhibit molecule-like fingerprints, yet their Raman response is usually buried under intense luminescence. Herein, we report the use of surface-enhanced Raman spectroscopy (SERS) to probe the molecular nature of the stable eight-electron silver NC, Ag17(o1-carboranethiolate)123- (abbreviated as Ag17), by integrating it with plasmonic gold nanotriangles (Au NTs), forming an Ag17@Au NT nanohybrid. This is the first demonstration of an atomically precise NC functioning as a stable next-generation Raman probe under harsh laser conditions. Synergistic electromagnetic (EM) and chemical enhancement (CE) mechanisms yield an overall enhancement factor of up to ∼6 × 105, with ∼2 × 102 attributed to CE, consistent with time-dependent density functional theory (TDDFT) calculations. TDDFT reproduces the observed spectra and reveals low-lying hybrid charge-transfer excited states, underpinning the CE pathway. Plasmonic confinement and charge transfer cooperatively amplify the Raman scattering of the Ag-Ag bonds and carborane framework at the nanoscale junctions of the Ag17@Au NT nanohybrid.
Manna et al. (Fri,) studied this question.
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