4.8 Article

Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods

Journal

ACS NANO
Volume 11, Issue 6, Pages 5925-5932

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.7b01665

Keywords

plasmonics; nonlinear optics; nanophotonics; condensed matter science; gold nanorods

Funding

  1. National Science Foundation through NSF DMR [1120923]
  2. Materials Science and Engineering Divisions, Office of Basic Energy Sciences of the U.S. Department of Energy [DESC0012704]

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A systematic study is presented of the intensity dependent nonlinear light scattering spectra of gold nanorods under resonant excitation of the longitudinal surface plasmon resonance (SPR). The spectra exhibit features due to coherent second and third harmonic generation as well as a broadband feature that has been previously attributed to multiphoton photoluminescence arising primarily from interband optical transitions in the gold. A detailed study of the spectral dependence of the scaling of the scattered light with excitation intensity shows unexpected scaling behavior of the coherent signals, which is quantitatively accounted for by optically induced damping of the SPR mode through a Fermi liquid model of the electronic scattering. The broadband feature is shown to arise not from luminescence, but from scattering of the second-order longitudinal SPR mode with the electron gas, where efficient excitation of the second order mode arises from an optical asymmetry of the nanorod. The electronic-temperature dependent plasmon damping and the Fermi-Dirac distribution together determine the intensity dependence of the broadband emission, and the structure-dependent absorption spectrum determines the spectral shape through the fluctuation dissipation theorem. Hence a complete self-consistent picture of both coherent and incoherent light scattering is obtained with a single set of physical parameters.

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