skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods

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 secondorder longitudinal SPR mode with the electron gas, where efficient excitation of the 2nd 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.

Authors:
ORCiD logo [1];  [1];  [2];  [1];  [3];  [1];  [2];  [4];  [1]; ORCiD logo [1];  [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. National Changua Univ. of Education (China)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1389238
Report Number(s):
BNL-114214-2017-JA
Journal ID: ISSN 1936-0851; R&D Project: MA015MACA; KC0201010
Grant/Contract Number:
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 6; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Plasmonics; Nonlinear Optics; Nanophotonics; Condensed Matter Science

Citation Formats

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., and Norris, Theodore B.. Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods. United States: N. p., 2017. Web. doi: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. United States. doi: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., and Norris, Theodore B.. 2017. "Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods". United States. doi:10.1021/acsnano.7b01665.
@article{osti_1389238,
title = {Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods},
author = {Lien, Miao-Bin and Kim, Ji-Young and Han, Myung-Geun and Chang, You-Chia and Chang, Yu-Chung and Ferguson, Heather J. and Zhu, Yimei and Herzing, Andrew A. and Schotland, John C. and Kotov, Nicholas A. and Norris, Theodore B.},
abstractNote = {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 secondorder longitudinal SPR mode with the electron gas, where efficient excitation of the 2nd 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.},
doi = {10.1021/acsnano.7b01665},
journal = {ACS Nano},
number = 6,
volume = 11,
place = {United States},
year = 2017,
month = 5
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 16, 2018
Publisher's Version of Record

Save / Share:
  • The paper represents a novel approach to investigating localized surface plasmon (LSP) resonance modes of nanoporous Au nanorods (NRs) in a solution phase with control over surface morphology. Au NRs, which have distinctive features such as nanopores and ligaments, showed interesting LSP resonance modes depending on the surface morphology and the total length of the structure. Compared with the analogous smooth surface NRs, the LSP modes of nanoporous NRs are red-shifted, which can be interpreted as a longer effective rod length and larger amplitude of plasmon oscillation.
  • Assisted with transmission electron microscopy and extinction spectra, the enhanced light scattering (ELS) experiments were performed with gold nanoparticles. Although both the nanospheres and nanorods can enhance light scattering in study aggregation, the spectral characteristics of gold nanorods is relatively simple compared to that of nanospheres. This will further extend the application range of ELS method to determinate the amounts of inorganic ions in analytical field and investigate on the macromolecular aggregation in polymeric research due to its simplicity, rapidity, and sensitivity.
  • The nonlinear optical responses of gold nanoparticles dispersed in castor oil produced by sputtering deposition were investigated, using the thermally managed Z-scan technique. Particles with spherical shape and 2.6 nm of average diameter were obtained and characterized by transmission electron microscopy and small angle X-ray scattering. This colloid was highly stable, without the presence of chemical impurities, neither stabilizers. It was observed that this system presents a large refractive third-order nonlinear response and a negligible nonlinear absorption. Moreover, the evaluation of the all-optical switching figures of merit demonstrated that the colloidal nanoparticles prepared by sputtering deposition have a good potentialmore » for the development of ultrafast photonic devices.« less
  • We have developed a reflection-mode scattering-type scanning near-field optical microscope using a laser trapped gold colloidal particle as a scattering probe and succeeded in observing the reflectance change of an opaque semiconductor sample with the alternating layers of GaAs and Al{sub 0.55}Ga{sub 0.45}As. The spatial resolution became as high as 200 nm when using a 200 nm gold colloidal particle. The results indicated that the resolution obtained in the experiment is in good agreement with the trapped particle size and overcame the diffraction limit (420 nm) of the lens system. {copyright} 2001 American Institute of Physics.
  • We demonstrate strong-field photoelectron emission from gold nanorods driven by femtosecond mid-infrared optical pulses. The maximum photoelectron yield is reached at the localized surface plasmon resonance, indicating that the photoemission is governed by the resonantly-enhanced optical near-field. The wavelength- and field-dependent photoemission yield allows for a noninvasive determination of local field enhancements, and we obtain intensity enhancement factors close to 1300, in good agreement with finite-difference time domain computations.