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Due to their negative permittivity, plasmonic materials have found increasing number of applications in advanced photonic devices and metamaterials, ranging from visible wavelength through microwave spectrum. In terms of intrinsic loss and permittivity dispersion, however, limitations on available plasmonic materials remain a serious bottleneck preventing practical applications of a few novel nano-photonic device and metamaterial concepts in visible and nearinfrared spectra. To overcome this obstacle, efforts have been made and reported in literature to engineer new plasmonic materials exploring metal alloys, superconductors, graphene, and heavily doped oxide semiconductors. Though promising progress in heavily doped oxide semiconductors was shown in the near-infrared spectrum, there is still no clear path to engineer new plasmonic materials in the visible spectrum that can outperform existing choices noble metals, e.g. gold and silver, due to extremely high free electron density required for high frequency plasma response. This study demonstrates a path to engineer new plasmonic materials in the visible spectrum by significantly altering the electronic properties in existing noble metals through high density charging/discharging and its associated strong local bias effects. A density functional theory model revealed that the optical properties of thin gold films (up to 7 nm thick) can be altered significantly in the visible, in terms of both plasma frequency (up to 12%) and optical permittivity (more than 50%). These corresponding effects were observed in our experiments on surface plasmon resonance of a gold film electrically charged via a high density double layer capacitor induced by a chemically non-reacting electrolyte.
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