Spectral Response of Plasmonic Gold Nanoparticles to Capacitive Charging: Morphology Effects

Benjamin S. Hoener, Hui Zhang, Thomas S. Heiderscheit, Silke R. Kirchner, Agampodi S. De Silva Indrasekara, Rashad Baiyasi, Yiyu Cai, Peter Nordlander, Stephan Link, Christy F. Landes, Wei Shun Chang

Research output: Contribution to journalArticlepeer-review


We report a study of the shape-dependent spectral response of the gold nanoparticle surface plasmon resonance at various electron densities to provide mechanistic insight into the role of capacitive charging, a topic of some debate. We demonstrate a morphology-dependent spectral response for gold nanoparticles due to capacitive charging using single-particle spectroscopy in an inert electrochemical environment. A decrease in plasmon energy and increase in spectral width for gold nanospheres and nanorods was observed as the electron density was tuned through a potential window of -0.3 to 0.1 V. The combined observations could not be explained by existing theories. A new quantum theory for charging based on the random phase approximation was developed. Additionally, the redox reaction of gold oxide formation was probed using single-particle plasmon voltammetry to reproduce the reduction peak from the bulk cyclic voltammetry. These results deepen our understanding of the relationship between optical and electronic properties in plasmonic nanoparticles and provide insight toward their potential applications in directed electrocatalysis.

Original languageEnglish (US)
Pages (from-to)2681-2688
Number of pages8
JournalJournal of Physical Chemistry Letters
Issue number12
StatePublished - Jun 15 2017
Externally publishedYes

ASJC Scopus subject areas

  • General Materials Science
  • Physical and Theoretical Chemistry


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