Nonlinear optical phenomena in nanostructured materials have been challenging our perceptions of nonlinear optical processes that have been explored since the invention of lasers. For example, the ability to control optical field confinement, enhancement, and scattering almost independently allows nonlinear frequency conversion efficiencies to be enhanced by many orders of magnitude compared to bulk materials. Also, the subwavelength length scale renders phase matching issues irrelevant. Compared with plasmonic nanostructures, dielectric resonator metamaterials show great promise for enhanced nonlinear optical processes due to their larger mode volumes. Here, we present, for the first time, resonantly enhanced second-harmonic generation (SHG) using gallium arsenide (GaAs) based dielectric metasurfaces. Using arrays of cylindrical resonators we observe SHG enhancement factors as large as 10(4) relative to unpatterned GaAs. At the magnetic dipole resonance, we measure an absolute nonlinear conversion efficiency of ∼2 × 10(-5) with ∼3.4 GW/cm(2) pump intensity. The polarization properties of the SHG reveal that both bulk and surface nonlinearities play important roles in the observed nonlinear process.

Resonantly Enhanced Second-Harmonic Generation Using III-V Semiconductor All-Dielectric Metasurfaces.

The fact that nanoparticles and nanomaterials have fundamental properties different both from their constituent atoms or molecules and from their bulk counterparts has stimulated great interest, both theoretical and practical, in nanoparticles and nanoparticle-based assemblies (functional materials), with the result that these structures have become the subject of explosive research over the last twenty years or so. A great deal of progress in this field has relied on the use of lasers. In this paper, the directions followed and results obtained in laser nanotechnology research are reviewed. The parameters, properties, and applications of nanoparticles are discussed, along with the physical and chemical methods for their fabrication and investigation. Nanofabrication applications of and fundamental physical principles behind laser ablation and laser nanolithography are discussed in detail. The applications of laser radiation are shown to range from fabricating, melting, and evaporating nanoparticles to changing their shape, structure, size, and size distribution, through studying their dynamics and forming them into periodic arrays and various structures and assemblies. The historical development of research on nanoparticles and nanomaterials and the application of laser nanotechnology in various fields are briefly reviewed.

https://iopscience.iop.org/article/10.3367/UFNe.0183.201307a.0673/pdf

Laser applications in nanotechnology: nanofabrication using laser ablation and laser nanolithography

This review provides a comprehensive description of nonlinear optical (NLO) properties of gold nanoparticles, which can be used in biological applications The main focus is placed on two-photon absorption (2PA) and two-photon excited photoluminescence (2PEL) - the processes crucial for multiphoton microscopy, which allows deeper imaging of the material and causes less damage to the biological samples in comparison to conventional (one-photon) microscopy We present the basics of 2PA measurement techniques and a summary of recent achievements in the understanding of multiphoton excitation and the resulting photoluminescence in gold nanoparticles, both plasmonic ones and small nanoclusters with molecule-like properties The examples of 2PA applications in bioimaging are also presented, with a comment on future challenges and applications

Two-photon absorption and photoluminescence of colloidal gold nanoparticles and nanoclusters

This Letter reports the shape-dependent third-order nonlinear optical properties of anisotropic gold nanoparticles. We characterized the nonlinear absorption coefficients of nanorods, nanostars, and nanoshells using femtosecond Z-scan measurements. By comparing nanoparticle solutions with a similar linear extinction at the laser excitation wavelength, we separated shape effects from that of the localized surface plasmon wavelength. We found that the nonlinear response depended on particle shape. Using pump-probe spectroscopy, we measured the ultrafast transient response of nanoparticles, which supported the strong saturable absorption observed in nanorods and weak nonlinear response in nanoshells. We found that the magnitude of saturable absorption as well as the ultrafast spectral responses of nanoparticles were affected by the linear absorption of the nanoparticles.

Shape-Dependent Nonlinear Optical Properties of Anisotropic Gold Nanoparticles.

High-performance multiphoton-pumped lasers based on cesium lead halide perovskite nanostructures are promising for nonlinear optics and practical frequency upconversion devices in integrated photonics. However, the performance of such lasers is highly dependent on the quality of the material and cavity, which makes their fabrication challenging. Herein, we demonstrate that cesium lead halide perovskite triangular nanorods fabricated via vapor methods can serve as gain media and effective cavities for multiphoton-pumped lasers. We observed blue-shifts of the lasing modes in the excitation fluence-dependent lasing spectra at increased excitation powers, which fits well with the dynamics of Burstein–Moss shifts caused by the band filling effect. Moreover, efficient multiphoton lasing in CsPbBr3 nanorods can be realized in a wide excitation wavelength range (700–1,400 nm). The dynamics of multiphoton lasing were investigated by time-resolved photoluminescence spectroscopy, which indicated that an electron–hole plasma is responsible for the multiphoton-pumped lasing. This work could lead to new opportunities and applications for cesium lead halide perovskite nanostructures in frequency upconversion lasing devices and optical interconnect systems.

Cesium lead halide perovskite triangular nanorods as high-gain medium and effective cavities for multiphoton-pumped lasing

We report a systematic study of the size-related nonlinear optical properties of triangular Au particles. The triangular Au nanoparticle arrays of four sizes (37 nm, 70 nm, 140 nm and 190 nm) were fabricated on quartz substrates using nanosphere lithography. By performing the Z-scan method with femtosecond laser (800 nm, 50 fs), the optical nonlinearities of Au nanoparticle arrays were determined. The results showed a size-related competition between two mechanisms of ground-state bleaching and two-photon absorption. As the size increased, the nonlinear absorption changed from two-photon absorption to saturated absorption, while the nonlinear refraction changed from self-defocusing to self-focusing. These size-tunable nonlinearities make it possible to optimize the one- and two-photon figures of merit, W and T, for all-optical switching.

Size-related third-order optical nonlinearities of Au nanoparticle arrays.

We report the two-photon absorption induced lasing performance in a single CdS microwire under the excitation of a femtosecond pulse laser with a wavelength of 800 nm. Sharp lasing peaks are centered at 523 nm with an average linewidth of 0.4 nm, indicating a high quality factor of 1300. The lasing emission is highly dependent on the polarization direction of the excitation light and the optimized lasing threshold is estimated to be 3.3 mJ/cm2 as the polarization direction is parallel to the microwire axis. Furthermore, the polarization-dependent lasing effect is confirmed by performing the finite-difference time-domain method.

Two-photon pumped lasing in a single CdS microwire

Optimization of metal-enhanced fluorescence by different concentrations of gold-silica core–shell nanoparticles

The invention discloses an efficient and nonlinear light polarization modulator based on a metasurface and a two-dimensional material and a preparation method thereof. The efficient and nonlinear light polarization modulator comprises a metal nanopore array located in a lower layer and the single-layer two-dimensional material located in an upper layer. A focused ion beam etching method is utilized to process a complete metal nano film so as to obtain a triangular nanopore array. The single-layer two-dimensional material is transferred to the surface of the nanopore array by adopting a hydrofluoric acid corrosion method so as to obtain the single-layer two-dimensional material and metal nanopore array compounded metasurface. By utilizing the compounded metasurface, second harmonic polarization direction for emergence can be modulated. Circularly polarized base-frequency incident light can produce oppositely and circularly polarized and frequency-multiplied emergent light, linearly polarized base-frequency incident light with a polarizing angle of theta can produce linearly polarized base-frequency emergent light with a polarizing angle of 2theta. In addition, compared with a traditional metal metasurface, the conversion efficiency is improved by about two magnitude orders. The efficient and nonlinear light polarization modulator is small in size, simple in structure and high in integration level.

Efficient and nonlinear light polarization modulator based on metasurface and two-dimensional material and preparation method thereof

We report surface second harmonic generation (SHG) in a single ZnTe nanowire. The SHG has a high efficiency of 5×10^(−6) and low divergence angle of 4°. Special polarization dependence is also observed in the experiment.

/pdf/laterally-emitted-surface-second-harmonic-generation-in-a-1ubcakcapi.pdf

Laterally Emitted Surface Second Harmonic Generation in a Single ZnTe Nanowire

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