We demonstrate a novel scheme to dramatically enhance both the second- and third-harmonic generation in a graphene-insulator-graphene metasurface. The key underlying feature of our approach is the existence of a double-resonance phenomenon, namely the metasurface is designed to possess fundamental plasmon resonances at both the fundamental frequency and the higher harmonic. In particular, this dual resonant field enhancement at the two optical frequencies, combined with a favorable spatial overlap of the optical near-fields, lead to the increase of the generated higher harmonic by several orders of magnitude. Remarkably, we demonstrate that by tuning the Fermi energy of the graphene gratings the dual-resonance property can be locked-in over a broad spectral range of ~20 THz, and equally important, the enhanced nonlinear frequency generation process can be readily switched in the same device between the second and third harmonic. This new type of graphene metasurface could open up new avenues towards the development of novel ultra-compact and multi-frequency active photonic nanodevices.
Described experimental conditions, reproducibility and optimization for the nonlinear optical effects (SHG, THG) for the diagnostic of functionalization of vertically aligned mesoporous silica thin films activated by silver and copper ions. The samples synthesis procedure are described in details. The dependence sof the seonc dhamroni genriaotn (SHG) and third harmonic genriaotn (THG) verus the fundamental energy density are presetned. The diffences between the SHG and THG energy power dependences are observed.
A comprehensive study of second and third harmonic conversion efficiency, angular and temperature tolerance, and long-term stability in LBO crystals using a 10-J-class laser
We demonstrate phase-matched second-harmonic generation (SHG) from three-dimensional metamaterials consisting of stacked metasurfaces. To achieve phase matching, we utilize a novel mechanism based on phase engineering of the metasurfaces at the interacting wavelengths, facilitating phase-matched SHG in the unconventional backward direction. By stacking up to five metasurfaces, we obtain the expected factor of 25 enhancement in SHG efficiency. Our results motivate further investigations to achieve higher conversion efficiencies also with more complex wavefronts.
Second harmonic generation (SHG) is a coherent nonlinear phenomenon that plays an important role in laser color conversion. Lithium niobate (LN), which features both a large band gap and outstanding second-order nonlinearities, acts as an important optical material for nonlinear frequency conversion covering a wide spectral range from ultraviolet to mid-infrared. Here we experimentally demonstrate LN metasurfaces with controllable SHG properties. Distinct enhancements for the SHG efficiency are observed at Mie-resonances. And by changing the geometric parameters thus the resonances of the meta…
We report on nonlinear frequency conversion from the telecom range via second harmonic generation (SHG) and third harmonic generation (THG) in suspended gallium nitride slab photonic crystal (PhC) cavities on silicon, under continuous-wave resonant excitation. Optimized two-dimensional PhC cavities with augmented far-field coupling have been characterized with quality factors as high as 4.4$\times10^{4}$, approaching the computed theoretical values. The strong enhancement in light confinement has enabled efficient SHG, achieving normalized conversion efficiency of 2.4$\times10^{-3}$ $W^{-1}$, …
Plasmonic resonances in metallic nanostructures have been shown to drastically enhance local electromagnetic fields, and thereby increase the efficiency of nonlinear optical phenomena, such as second harmonic generation (SHG). While it has been experimentally observed that enhanced fields can significantly boost SHG, to date it proved difficult to probe electrical and magnetic resonances in one and the same nanostructure. This however is necessary to directly compare relative contributions of electrical and magnetic components of SHG enhancement. In this paper we report an experimental study o…
Optical harmonic generation on excitons is found in ZnSe/BeTe quantum wells with type-II band alignment. Two experimental approaches with spectrally-broad femtosecond laser pulses and spectrally-narrow picosecond pulses are used for spectroscopic studies by means of second and third harmonic generation (SHG and THG). The SHG signal is symmetry-forbidden for light propagation along the structure's growth axis, which is the [001] crystal axis, but can be induced by an external magnetic field. The THG signal is detected at zero magnetic field and its intensity is field independent. A group theory…
The nonlinear process of second harmonic generation (SHG) in monolayer (1L) transition metal dichalcogenides (TMD), like $WS_2$, strongly depends on the polarization state of the excitation light. Combining plasmonic nanostructures with $1L-WS_2$ by transferring it onto a plasmonic nanoantenna array, a hybrid metasurface is realized impacting the polarization dependency of its SHG. Here, we investigate how plasmonic dipole resonances affect the process of SHG in plasmonic-TMD hybrid metasurfaces by nonlinear spectroscopy. We show, that the polarization dependency is affected by the lattice str…
Silicon-based nonlinear metasurfaces were implemented only with third-order nonlinearity due to the crystal centrosymmetry and the efficiencies are considerably low, which hinders their practical applications with low-power lasers. Here, we propose to integrate a two-dimensional GaSe flake onto a silicon metasurface to assist high-efficiency second-order nonlinear processes, including second-harmonic generation (SHG) and sum-frequency generation (SFG). By resonantly pumping the integrated GaSe-metasurface, which supports a Fano resonance, the obtained SHG is about two orders of magnitude stron…
We investigate experimentally Third Harmonic Generation (THG) from plasmonic metasurfaces consisting of two-dimensional rectangular lattices of centrosymmetric gold nano-bars. By varying the incidence angle and the lattice period, we show how Surface Lattice Resonances (SLRs) at the involved wavelengths are the major contributors in determining the magnitude of the nonlinear effects. A further boost on THG is observed when we excite together more than one SLR, either at the same or at different frequencies. When such multiple resonances take place, interesting phenomena are observed, such as m…
The nonlinear processes of frequency conversion like second harmonic generation (SHG) usually obey certain selection rules, resulting from the preservation of different kind of physical quantities, e.g., the angular momentum. For SHG created by monolayer of transition-metal dichalcogenides (TMDCs) like WS2, the valley-exciton locked selection rule predicts an SHG signal in the cross-polarization state. By combining plasmonic nanostructures with a monolayer of TMDC, a hybrid metasurface is realized which affects this nonlinear process due to an additional polarization conversion process. Here, …
Nonlinear metasurfaces offer new paradigm for boosting optical effect beyond limitations of conventional materials. In this work, we present an alternative way to produce pronounced third-harmonic generation (THG) based on nonlinear field resonances rather than linear field enhancement, which is a typical strategy for achieving strong nonlinear response. By designing and studying a nonlinear plasmonic-graphene metasurface at terahertz regime with hybrid guided modes and bound states in the continuum modes, it is found that a THG with a narrow bandwidth can be observed, thanks to the strong res…
The mid-wave infrared (MWIR) spectral region (3-5 μm) is important to a vast variety of applications in imaging, sensing, spectroscopy, surgery, and optical communications. Efficient third-harmonic generation (THG), converting light from the MWIR range into the near-infrared, a region with mature optical detection and manipulation technologies, offers the opportunity to mitigate a commonly recognized limitation of current MWIR systems. In this work, we present the possibility of boosting THG in the MWIR through a metasurface design. Specifically, we demonstrate a 30-fold enhancement in a highl…
Enhanced third-harmonic generation and degenerate four-wave mixing in an all-dielectric metasurfaces via Brillouin zone folding-induced bound states in the continuum
Parametric oscillation is a fundamental concept that underlies nonlinear wave-matter interactions, leading to generation or amplification of new frequency components. Using a temporal modulation generated by the heterodyne interference of a control direct current (dc) electric field and an optical field, we resonantly drive large-amplitude oscillations of amorphous silicon meta-atoms - nanoscale building blocks of an optical metasurface. We observed gigantically enhanced second harmonic generation (SHG) with an electric-field-controlled on off ratio over 10000 and an ultra-high modulation dept…
To date, second-harmonic generation (SHG) at nanoscale has been concentrated on employing high-refractive-index nanostructures, owing to the strong field confinement at deep subwavelength scales based on optically resonant effects. However, low-index nanostructures generally exhibit weaker resonant effects and lower field confinement. To address this issue, by harnessing the large nonlinearity of LiNbO$\mathrm{_3}$, we propose a novel approach to employ guided resonances and bound states in the continuum (BICs) with a LiNbO$\mathrm{_3}$ metasurface consisting of a LiNbO$\mathrm{_3}$ disk array…
We investigate optical second-harmonic generation (SHG) from metasurfaces where noncentrosymmetric V-shaped gold nanoparticles are ordered into regular array configurations. In contrast to expectations, a substantial enhancement of the SHG signal is observed when the number density of the particles in the array is reduced. More specifically, by halving the number density, we obtain over five-fold enhancement in SHG intensity. This striking result is attributed to favorable interparticle interactions mediated by the lattice, where surface-lattice resonances lead to spectral narrowing of the pla…
The emerging all-dielectric platform exhibits high-quality ($Q$) resonances governed by the physics of bound states in the continuum (BIC) that drives highly efficient nonlinear optical processes. Here we demonstrate the robust enhancement of third-(THG) and fifth-harmonic generation (FHG) from all-dielectric metasurfaces composed of four silicon nanodisks. Through the symmetry breaking, the genuine BIC transforms into the high-$Q$ quasi-BIC resonance with tight field confinement for record high THG efficiency of $3.9\times10^{-4}$ W$^{-2}$ and FHG efficiency of $4.8\times10^{-10}$ W$^{-4}$ us…
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…
Electro-optically tunable second-harmonic generation in lithium niobate metasurfaces boosted by Brillouin zone folding induced bound states in the continuum
Highly Efficient Second/Third Harmonic Generation in van der Waals Layered Material AgScP2S6 with Anisotropic Polarization and Temperature Dependence
The Ohio State University（俄亥俄州立大学）；the University of Texas at Dallas（德克萨斯大学达拉斯分校）；ELI ALPS, ELI-HU Non-Profit Ltd.（ELI ALPS，匈牙利ELI非营利有限公司）；Materials and Manufacturing Directorate, Airforce Research Laboratory（空军研究实验室材料与制造管理局）；Azimuth Corporation（Azimuth公司）；Core4ce LLC（Core4ce有限责任公司）
Hybrid dielectric metasurfaces have emerged as a promising approach to enhancing near field confinement and thus achieving high optical nonlinearity using low loss dielectrics. Additional flexibility in design and fabrication of hybrid metasurfaces allows dynamic control of light, which is value-added for a wider range of applications. Here, we demonstrate a tunable and efficient third harmonic generation (THG) via hybrid metasurfaces with phase change material Ge2Sb2Te5 (GST) deposited on top of amorphous silicon nanostructutes. Fano resonance is excited to confine the incident light inside t…
Resonant metasurfaces are an attractive platform for enhancing the non-linear optical processes, such as second harmonic generation (SHG), since they can generate very large local electromagnetic fields while relaxing the phase-matching requirements. Here, we take this platform a step closer to the practical applications by demonstrating visible range, continuous wave (CW) SHG. We do so by combining the attractive material properties of gallium phosphide with engineered, high quality-factor photonic modes enabled by bound states in the continuum. For the optimum case, we obtain efficiencies ar…
The nonlinear responses of different materials provide useful mechanisms for optical switching, low noise amplification, and harmonic frequency generation. However, the nonlinear processes usually have an extremely weak nature and require high input power to be excited. To alleviate this severe limitation, we propose new designs of ultrathin nonlinear metasurfaces composed of patterned graphene micro-ribbons to significantly enhance third harmonic generation (THG) at far-infrared and terahertz (THz) frequencies. The incident wave is tightly confined and significantly boosted along the surface …
Breaking inversion symmetry in solids plays a central role in nonlinear optics because it can change material properties, such as producing even-order nonlinear optical (NLO) effects. Although a centrosymmetric diamond has been developed as a photonic platform, including waveguides and light sources, the NLO effects in bulk diamonds are limited to the third-order. Thus, exploiting more powerful second-order NLO effects, such as second harmonic generation (SHG), are still challenging. Here we explore symmetry-breaking-induced second-order NLO effects in bulk diamonds using the color center, nit…
Terahertz frequency upconversion by coherently driving charge dynamics in the InSb/CdTe heterostructure
Tsinghua University（清华大学）；Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Peking University（北京大学）；ShanghaiTech University（上海科技大学）；University of Chinese Academy of Sciences（中国科学院大学）
A ~545 mW single-frequency tunable 520 nm green laser has been demonstrated using a periodically-poled potassium titanyl phosphate (PPKTP) bulk crystal based on single-pass third-harmonic generation (THG) of a 1560 nm laser via single-pass second-harmonic generation (SHG) followed by single-pass sum-frequency generation (SFG). In single-pass SHG, two cascaded periodically-poled magnesium-oxide-doped lithium niobate (PPMgO:LN) crystals were used, and ~3.5 W 780.25 nm doubled laser output is produced, corresponding to maximum doubling efficiency of 26.8%. The system can provide a pump source (52…
Bianisotropy is a powerful concept enabling asymmetric optical response, including asymmetric reflection, absorption, optical forces, light trapping, and lasing. The physical origin of these asymmetric effects can be understood from magnetoelectric coupling and asymmetrical field enhancement. Here, we theoretically propose highly asymmetric second-harmonic generation (SHG) in bianisotropic AlGaAs metasurfaces. We show that around four orders of magnitude second-harmonic power difference for the forward and backward illuminations can be obtained by altering geometrical parameters that coincide …
Nonlinear optics in whispering-gallery-mode (WGM) microresonators have attracted much attention. Owing to strong confinement of the light in a small volume, a WGM microresonator can dramatically boost the strength of light field, giving rise to enhancement of the nonlinear interactions of light with the resonator material. Here, we demonstrate highly efficient second harmonic generation (SHG) and third harmonic generation (THG) in an on-chip monocrystalline lithium niobate (LN) microresonator. Benefitting from a cyclic phase matching scheme for the transverse-electric WGMs, nonlinear wavelengt…
Tensor-driven geometric phase in nonlinear AlGaAs metasurfaces
Université Paris Cité（巴黎西岱大学）；CNRS（法国国家科学研究中心）；Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院）；Centre de Nanosciences et de Nanotechnologies, Université Paris-Saclay（巴黎萨克雷大学纳米科学和纳米技术研究中心）；University of Brescia（布雷西亚大学）
Polarization-Sensitive Third Harmonic Generation in resonant silicon nitride Metasurfaces for deep-UV Emission
Universitat Politècnica de Catalunya（加泰罗尼亚理工大学）；Università degli Studi di Brescia（布雷西亚大学）；DTU Nanolab, National Center for Nanofabrication and Characterization（丹麦技术大学纳米实验室，国家纳米加工与表征中心）；DTU Electro, Department of Electrical and Photonics Engineering（丹麦技术大学电气与光子工程系）
We study optical harmonic generation on the 1S exciton-polariton in the semiconductor ZnSe. Intense and spectrally narrow exciton resonances are found in optical second (SHG), third (THG), and fourth (FHG) harmonic generation spectra. The resonances are shifted to higher energy by 3.2 meV from the exciton energy in the linear reflectivity spectrum. Additional resonances are observed in the THG and FHG spectra and assigned to combinations of incident and backscattered photons in the crystal. Rotational anisotropy diagrams are measured and further information on the origin of the optical harmoni…
Strong light-matter coupling within electromagnetic environments provides a promising path to modify and control chemical and physical processes. The origin of the enhancement of nonlinear optical processes such as second-harmonic and third-harmonic generation (SHG and THG) due to strong light-matter coupling is attributed to distinct physical effects which questions the relevance of strong coupling in these processes. In this work, we leverage a first-principles approach to investigate the origins of the experimentally observed enhancement of resonant SHG and THG under strong light-matter cou…
Lead halide perovskites (MAPbX3) have emerged as promising materials for photovoltaic and optoelectronic devices. However, their exceptional nonlinear properties have not been fully exploited in nanophotonics yet. Herein we fabricate MAPbX3 perovskite metasurfaces and explore their internal nonlinear processes. While both of third-order harmonic generation (THG) and three-photon luminescence are generated, the latter one is less affected by the material loss and has been significantly enhanced by a factor of 60. The corresponding simulation reveals that the improvement is caused by the resonan…
Resonant structures in modern nanophotonics are non-Hermitian (leaky and lossy), and support quasinormal modes. Moreover, contemporary cavities frequently include 2D materials to exploit and resonantly enhance their nonlinear properties or provide tunability. Such materials add further modeling complexity due to their infinitesimally thin nature and strong dispersion. Here, a formalism for efficiently analyzing third harmonic generation (THG) in nanoparticles and metasurfaces incorporating 2D materials is proposed. It is based on numerically calculating the quasinormal modes in the nanostructu…
The enhanced electric field at plasmonic resonances in nanoscale antennas can lead to efficient harmonic generation, especially when the plasmonic geometry is asymmetric on either inter-particle or intra-particle levels. The planar Archimedean nanospiral offers a unique geometrical asymmetry for second-harmonic generation (SHG) because the SHG results neither from arranging centrosymmetric nanoparticles in asymmetric groupings, nor from non-centrosymmetric nanoparticles that retain a local axis of symmetry. Here we report forward SHG from planar arrays of Archimedean nanospirals using 15 fs pu…
A key concept underlying the specific functionalities of metasurfaces, i.e. arrays of subwavelength nanoparticles, is the use of constituent components to shape the wavefront of the light, on-demand. Metasurfaces are versatile and novel platforms to manipulate the scattering, colour, phase or the intensity of the light. Currently, one of the typical approaches for designing a metasurface is to optimize one or two variables, among a vast number of fixed parameters, such as various materials' properties and coupling effects, as well as the geometrical parameters. Ideally, it would require a mult…
We report the first observation of nonlinear harmonic generation and sum frequency generation (SFG) coupled with stimulated Raman scattering (SRS) via the second-order (χ^{(2)}) and the third-order (χ^{(3)}) nonlinearities in a silica microbottle resonator. The visible light emission due to third harmonic generation (THG) was observed in both the output of a tapered fiber and the optical microscope images, which can be used to identify the axial mode profiles. SFG enabled by three- and four-wave mixing processes between the pump light and the light generated via SRS was also observed. Second H…
Femtosecond all-optical polarization manipulation of harmonic generation in an anisotropic strongly coupled plasmon-epsilon-near-zero metasurface
Key Laboratory for Physical Electronics and Devices of the Ministry of Education and Shaanxi Key Lab of Information Photonic Technique, School of Electronic Science and Engineering, Xi’an Jiaotong University（教育部光电技术与器件重点实验室、陕西省信息光子技术重点实验室，西安交通大学电子科学与工程学院）
