Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods

Miao Bin Lien, Ji Young Kim, Myung Geun Han, You Chia Chang, Yu Chung Chang, Heather J. Ferguson, Yimei Zhu, Andrew A. Herzing, John C. Schotland, Nicholas A. Kotov, Theodore B. Norris

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

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.

Original languageEnglish
Pages (from-to)5925-5932
Number of pages8
JournalACS Nano
Volume11
Issue number6
DOIs
Publication statusPublished - 2017 Jun 27

Fingerprint

Gold Colloid
Surface plasmon resonance
Nanorods
surface plasmon resonance
Light scattering
nanorods
light scattering
Gold
asymmetry
gold
Harmonic generation
broadband
Damping
damping
Incoherent scattering
Scattering
excitation
Fermi liquids
scaling
Electron gas

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

Cite this

Lien, M. B., Kim, J. Y., Han, M. G., Chang, Y. C., Chang, Y. C., Ferguson, H. J., ... Norris, T. B. (2017). Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods. ACS Nano, 11(6), 5925-5932. https://doi.org/10.1021/acsnano.7b01665
Lien, Miao Bin ; Kim, Ji Young ; Han, Myung Geun ; Chang, You Chia ; Chang, Yu Chung ; Ferguson, Heather J. ; Zhu, Yimei ; Herzing, Andrew A. ; Schotland, John C. ; Kotov, Nicholas A. ; Norris, Theodore B. / Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods. In: ACS Nano. 2017 ; Vol. 11, No. 6. pp. 5925-5932.
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Lien, MB, Kim, JY, Han, MG, Chang, YC, Chang, YC, Ferguson, HJ, Zhu, Y, Herzing, AA, Schotland, JC, Kotov, NA & Norris, TB 2017, 'Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods', ACS Nano, vol. 11, no. 6, pp. 5925-5932. https://doi.org/10.1021/acsnano.7b01665

Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods. / Lien, Miao Bin; Kim, Ji Young; Han, Myung Geun; Chang, You Chia; Chang, Yu Chung; Ferguson, Heather J.; Zhu, Yimei; Herzing, Andrew A.; Schotland, John C.; Kotov, Nicholas A.; Norris, Theodore B.

In: ACS Nano, Vol. 11, No. 6, 27.06.2017, p. 5925-5932.

Research output: Contribution to journalArticle

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AU - Ferguson, Heather J.

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AU - Norris, Theodore B.

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N2 - 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.

AB - 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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