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Second-Harmonic Generation Optical Rotation Solely Attributable to Chirality in Plasmonic Metasurfaces.

Authors
  • Collins, Joel T1
  • Hooper, David C1
  • Mark, Andrew G2
  • Kuppe, Christian1
  • Valev, Ventsislav K1
  • 1 Centre for Photonics and Photonic Materials, and Centre for Nanoscience and Nanotechnology, Department of Physics , University of Bath , Bath , BA2 7AY , United Kingdom. , (United Kingdom)
  • 2 Max Planck Institute for Intelligent Systems , Heisenbergstraße 3 , 70569 Stuttgart , Germany. , (Germany)
Type
Published Article
Journal
ACS Nano
Publisher
American Chemical Society
Publication Date
Jun 26, 2018
Volume
12
Issue
6
Pages
5445–5451
Identifiers
DOI: 10.1021/acsnano.8b00601
PMID: 29852066
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

Chiral plasmonic nanostructures, those lacking mirror symmetry, can be designed to manipulate the polarization of incident light resulting in chiroptical (chiral optical) effects such as circular dichroism (CD) and optical rotation (OR). Due to high symmetry sensitivity, corresponding effects in second-harmonic generation (SHG-CD and SHG-OR) are typically much stronger in comparison. These nonlinear effects have long been used for chiral molecular analysis and characterization; however both linear and nonlinear optical rotation can occur even in achiral structures, if the structure is birefringent due to anisotropy. Crucially, chiroptical effects resulting from anisotropy typically exhibit a strong dependence on structural orientation. Here we report a large second-harmonic generation optical rotation of ±45°, due to intrinsic chirality in a highly anisotropic helical metamaterial. The SHG intensity is found to strongly relate to the structural anisotropy; however, the angle of SHG-OR is invariant under sample rotation. We show that by tuning the geometry of anisotropic nanostructures, the interaction between anisotropy, chirality, and experimental geometry can allow even greater control over the chiroptical properties of plasmonic metamaterials.

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