Journal
ACS PHOTONICS
Volume 3, Issue 8, Pages 1477-1481Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsphotonics.6b00034
Keywords
nonlinear optics; metasurfaces; plasmonic enhancement; intoferometry; optical control
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Funding
- Office of Science, U.S. Department of Energy [DE-FG02-01ER45916]
- National Science Foundation Research Experience for Undergraduates program of the Vanderbilt Institute of Nanoscale Science and Engineering [DMR-1263182]
- National Science Foundation under the American Recovery and Reinvestment Act [ARI-R2 DMR-0963361]
- Laboratory Directed Research and Development Program of Oak Ridge National Laboratory [DE-AC05-00OR22725]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1263182] Funding Source: National Science Foundation
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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. 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.
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