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It is important and challenging to analyze nanocluster structure with atomic precision. Herein, α-hemolysin nanopore was used to identify nanoclusters at the single molecule level by providing two-dimensional (2D) dwell time–current blockage spectra and translocation event frequency which sensitively depended on their structures. Nanoclusters such as Anderson, Keggin, Dawson, and a few lacunary Dawson polyoxometalates with very similar structures, even with only a two-atom difference, could be discriminated. This nanopore device could simultaneously measure multiple nanoclusters in a mixture qualitatively and quantitatively. Furthermore, molecular dynamics (MD) simulations provided microscopic understandings of the nanocluster translocation dynamics and yielded 2D dwell time–current blockage spectra in close agreement with experiments. The nanopore platform provides a novel powerful tool for nanocluster characterization.
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