The Interplay of Symmetry and Scattering Phase in Second Harmonic Generation from Gold Nanoantennas

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Title: The Interplay of Symmetry and Scattering Phase in Second Harmonic Generation from Gold Nanoantennas
Authors: Gennaro, SD
Rahmani, M
Giannini, V
Aouani, H
Sidiropoulos, TP
Navarro-Cía, M
Maier, SA
Oulton, RF
Item Type: Journal Article
Abstract: Nonlinear phenomena are central to modern photonics but, being inherently weak, typically require gradual accumulation over several millimeters. For example, second harmonic generation (SHG) is typically achieved in thick transparent nonlinear crystals by phase-matching energy exchange between light at initial, ω, and final, 2ω, frequencies. Recently, metamaterials imbued with artificial nonlinearity from their constituent nanoantennas have generated excitement by opening the possibility of wavelength-scale nonlinear optics. However, the selection rules of SHG typically prevent dipole emission from simple nanoantennas, which has led to much discussion concerning the best geometries, for example, those breaking centro-symmetry or incorporating resonances at multiple harmonics. In this work, we explore the use of both nanoantenna symmetry and multiple harmonics to control the strength, polarization and radiation pattern of SHG from a variety of antenna configurations incorporating simple resonant elements tuned to light at both ω and 2ω. We use a microscopic description of the scattering strength and phases of these constituent particles, determined by their relative positions, to accurately predict the SHG radiation observed in our experiments. We find that the 2ω particles radiate dipolar SHG by near-field coupling to the ω particle, which radiates SHG as a quadrupole. Consequently, strong linearly polarized dipolar SHG is only possible for noncentro-symmetric antennas that also minimize interference between their dipolar and quadrupolar responses. Metamaterials with such intra-antenna phase and polarization control could enable compact nonlinear photonic nanotechnologies.
Issue Date: 19-Jul-2016
Date of Acceptance: 17-Jul-2016
ISSN: 1530-6992
Publisher: American Chemical Society
Start Page: 5278
End Page: 5285
Journal / Book Title: Nano Letters
Volume: 16
Issue: 8
Copyright Statement: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Nano Letters, © 2016 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Sponsor/Funder: Engineering & Physical Science Research Council (E
Funder's Grant Number: EP/M013812/1
Keywords: Nonlinear optics
second harmonic generation
Nanoscience & Nanotechnology
MD Multidisciplinary
Publication Status: Published
Appears in Collections:Condensed Matter Theory
Experimental Solid State
Faculty of Natural Sciences

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