Inhomogeneous Quantized Single-Electron Charging and Electrochemical-Optical Insights on Transition-Sized Atomically Precise Gold Nanoclusters

ACS Nano
Shuang ChenGangli Wang

Abstract

Small differences in electronic structures, such as an emerging energy band gaps or the splitting of degenerated orbitals, are very challenging to resolve but important for nanomaterials properties. A signature electrochemical property called quantized double layer charging, i.e., "continuous" one-electron transfers (1e, ETs), in atomically precise Au133(TBBT)52, Au144(BM)60, and Au279(TBBT)84 is analyzed to reveal the nonmetallic to metallic transitions (whereas TBBT is 4-tert-butylbenzenethiol and BM is benzyl mercaptan; abbreviated as Au133, Au144, and Au279). Subhundred milli-eV energy differences are resolved among the "often-approximated uniform" peak spacings from multipairs of reversible redox peaks in voltammetric analysis, with single ETs as internal standards for calibration and under temperature variations. Cyclic and differential pulse voltammetry experiments reveal a 0.15 eV energy gap for Au133 and a 0.17 eV gap for Au144 at 298 K. Au279 is confirmed metallic, displaying a "bulk-continuum" charging response without an energy gap. The energy gaps and double layer capacitances of Au133 and Au144 increase as the temperature decreases. The temperature dependences of charging energies and HOMO-LUMO gaps of Au133 and A...Continue Reading

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Citations

Aug 20, 2021·Journal of the American Chemical Society·Meng-Xia MaShi-Ming Li
Oct 6, 2021·Journal of the American Chemical Society·Feng HuQuan-Ming Wang

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