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Title: Ultrafast Plasmonic Control of Second Harmonic Generation

Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast control pulse is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an even-order nonlinear optical response. The temporal evolution of the plasmonic near-field is characterized with ~100 as resolution using a novel nonlinear interferometric technique. The serrated nanogap is a unique platform in which to investigate optically controlled, plasmonically enhanced harmonic generation in dielectric materials on an ultrafast time scale. Lastly, this metamaterial geometry can also be readily extended to all-optical control of other nonlinear phenomena, such as four-wave mixing and sum- and difference-frequency generation, in a wide variety of dielectric materials.
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [4] ;  [3]
  1. Vanderbilt Univ., Nashville, TN (United States). Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Computational Sciences and Engineering Division
  2. Vanderbilt Univ., Nashville, TN (United States). Dept. of Physics and Astronomy; Univ. of Virginia, Charlottesville, VA (United States). Dept. of Physics
  3. Vanderbilt Univ., Nashville, TN (United States). Dept. of Physics and Astronomy
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Computational Sciences and Engineering Division
Publication Date:
Grant/Contract Number:
AC05-00OR22725; FG02-01ER45916
Type:
Accepted Manuscript
Journal Name:
ACS Photonics
Additional Journal Information:
Journal Volume: 3; Journal Issue: 8; Journal ID: ISSN 2330-4022
Publisher:
American Chemical Society (ACS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; interferometry; metasurfaces; nonlinear optics; optical control; plasmonic enhancement
OSTI Identifier:
1364273

Davidson, Roderick B., Yanchenko, Anna, Ziegler, Jed I., Avanesyan, Sergey M., Lawrie, Benjamin J., and Haglund, Richard F.. Ultrafast Plasmonic Control of Second Harmonic Generation. United States: N. p., Web. doi:10.1021/acsphotonics.6b00034.
Davidson, Roderick B., Yanchenko, Anna, Ziegler, Jed I., Avanesyan, Sergey M., Lawrie, Benjamin J., & Haglund, Richard F.. Ultrafast Plasmonic Control of Second Harmonic Generation. United States. doi:10.1021/acsphotonics.6b00034.
Davidson, Roderick B., Yanchenko, Anna, Ziegler, Jed I., Avanesyan, Sergey M., Lawrie, Benjamin J., and Haglund, Richard F.. 2016. "Ultrafast Plasmonic Control of Second Harmonic Generation". United States. doi:10.1021/acsphotonics.6b00034. https://www.osti.gov/servlets/purl/1364273.
@article{osti_1364273,
title = {Ultrafast Plasmonic Control of Second Harmonic Generation},
author = {Davidson, Roderick B. and Yanchenko, Anna and Ziegler, Jed I. and Avanesyan, Sergey M. and Lawrie, Benjamin J. and Haglund, Richard F.},
abstractNote = {Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast control pulse is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an even-order nonlinear optical response. The temporal evolution of the plasmonic near-field is characterized with ~100 as resolution using a novel nonlinear interferometric technique. The serrated nanogap is a unique platform in which to investigate optically controlled, plasmonically enhanced harmonic generation in dielectric materials on an ultrafast time scale. Lastly, this metamaterial geometry can also be readily extended to all-optical control of other nonlinear phenomena, such as four-wave mixing and sum- and difference-frequency generation, in a wide variety of dielectric materials.},
doi = {10.1021/acsphotonics.6b00034},
journal = {ACS Photonics},
number = 8,
volume = 3,
place = {United States},
year = {2016},
month = {6}
}