Abstract

Abstract The emergence of metamaterials (MMs) has led to groundbreaking photo-physical phenomena, which arise from their novel structure-dependent properties. Consisting of “meta-atom” building blocks, MMs can be organized into subwavelength metal/dielectric structures using bottom-up or top-down nanofabrication techniques. Optical metal metasurfaces are a class of MMs with macroscopic lateral dimensions but composed of one to few subwavelength layers of precisely oriented metal-based elements over a large surface area. In this review, we focus on gold metasurfaces, highlighting their fabrication methods, morphological characterization, as well as linear and nonlinear optical properties. We then review our recent work on fabricating and characterizing self-assembled gold metasurface. An interesting characteristics of the gold metasurfaces is their wide range of linear refractive indices, varying from n 0 ~ 0.5 in the visible to n 0 ~ 4 in the short wavelength infrared spectral region. Third-order nonlinearities are characterized by the Z-scan technique at wavelengths on- and off-plasmonic resonance of the gold metasurface. Experimental results on the relationship between the third-order nonlinearity of the self-assembled gold metasurface as a function of the linear response are presented for the first time. We conclude by discussing the potential applications and future outlook of self-assembled plasmonic metasurfaces.

Highlights

  • Metamaterials are a class of engineered materials comprised of meta-atom building blocks organized into arrays of subwavelength metal and/or dielectric components

  • We focus on gold metasurfaces, highlighting their fabrication methods, morphological characterization, as well as linear and nonlinear optical properties

  • Second-order nonlinearities are typically studied through second harmonic generation (SHG), but this has been previously reviewed in [4, 10, 25, 34]

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Summary

Introduction

Metamaterials are a class of engineered materials comprised of meta-atom building blocks organized into arrays of subwavelength metal and/or dielectric components. We will instead focus on third-order NLO properties, which can be investigated by third harmonic generation (THG) spectroscopy, four wave-mixing (FWM), optical Kerr effect, or intensity-dependent spatial or spectral phase modulation methods [3, 35, 36]. 726 A.S.L. Gomes et al.: Linear and third-order nonlinear optical properties the generated emission can be at the same pump wavelength (degenerate FWM) or different wavelengths The NLR can be described in terms of an intensity-dependent refractive index, n(I) This formulation is useful for instantaneous (~fs) responses of the NLO Kerr effect. 5, we discuss new results on the feasibility of evaluating the third-order optical properties of a self-assembled gold metasurface from its linear response. We briefly explain examples of metasurface fabrication techniques, as well as morphological characterization methods

Lithography
Block copolymers
Evaporative methods
Langmuir-Blodgett
Langmuir-Schaefer
Layer-by-layer assembly
Patterned surfaces
F ield assisted assembly
Linear optical and NLO characterization of plasmonic metasurfaces
Optical characterization
NLO characterization
On-resonance studies
O n- and off-resonance nonlinear optics in self-assembled gold metasurfaces
Off-resonance studies
Conclusion and outlook
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