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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. Tue . "Optical Asymmetry and Nonlinear Light Scattering from Colloidal Gold Nanorods". United States. doi:10.1021/acsnano.7b01665. https://www.osti.gov/servlets/purl/1389238.
@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 = {Tue May 16 00:00:00 EDT 2017},
month = {Tue May 16 00:00:00 EDT 2017}
}

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