Nonlinear Metasurfaces Research Articles

All-optical polarization tuning based on an intensity-dependent nonlinear metasurface

Active control of light polarization at the nanoscale is essential for integrated photonic devices. Here, an all-optical approach is proposed to tune the polarization state of near-infrared light using a nonlinear metasurface. Based on the large intensity-dependent refractive index change of epsilon-near-zero (ENZ) materials, a phase difference between two orthogonal electric fields at ENZ wavelength can be continuously tuned in a range larger than 0.61π by varying the incident light power. The polarization state of the reflected light can thus be actively tuned from linear to circular state via an all-optical approach. Notably, abundant polarization states can be obtained by altering the polarization angle of incident light. The proposed all-optical approach is promising for tunable photonic functionalities of practical applications.

Topological metasurface: from passive toward active and beyond

Metasurfaces are subwavelength structured thin films consisting of arrays of units that allow the control of polarization, phase, and amplitude of light over a subwavelength thickness. Recent developments in topological photonics have greatly broadened the horizon in designing metasurfaces for novel functional applications. In this review, we summarize recent progress in the research field of topological metasurfaces, first from the perspectives of passive and active in the classical regime, and then in the quantum regime. More specifically, we begin by examining the passive topological phenomena in two-dimensional photonic systems, including both time-reversal broken systems and time-reversal preserved systems. Subsequently, we discuss the cutting-edge studies of active topological metasurfaces, including nonlinear topological metasurfaces and reconfigurable topological metasurfaces. After overviewing topological metasurfaces in the classical regime, we show how they could provide a new platform for quantum information and quantum many-body physics. Finally, we conclude and describe some challenges and future directions of this fast-evolving field.

Nonlinear photonics with metasurfaces

Nonlinear optics is a well-established field of research that traditionally relies on the interaction of light with macroscopic nonlinear media over distances significantly greater than the wavelength of light. However, the recently emerged field of optical metasurfaces provides a novel platform for studying nonlinear phenomena in planar geometries. Nonlinear optical metasurfaces introduce new functionalities to the field of nonlinear optics extending them beyond perturbative regimes of harmonic generation and parametric frequency conversion, being driven by mode-matching, resonances, and relaxed phase-matching conditions. Here we review the very recent advances in the rapidly developing field of nonlinear metasurface photonics, emphasizing multi-frequency and cascading effects, asymmetric and chiral frequency conversion, nonperturbative nonlinear regimes, and nonlinear quantum photonics, empowered by the physics of Mie resonances and optical bound states in the continuum.

Inverse Design of Nonlinear Polaritonic Metasurfaces for Second Harmonic Generation

Enabling strong nonlinear optical phenomena requires carefully designed photonic devices to maximize light–matter interactions. In recent years, topology optimization has become an increasingly popular tool to optimize photonic devices, due to its efficiency in dealing with extremely large parameter spaces. The focus has largely been on two-dimensional linear optical devices, particularly in integrated photonic settings, with a limited number of studies extending topology optimization to nonlinear effects in dielectric structures. Here, we apply topology optimization to metal–multiple quantum well–metal structures supporting intersubband transitions. In past years, the combination of photonic engineering and material design has enabled extremely efficient ultrathin second harmonic generating metasurfaces, based on L- and T-shaped resonators. Topology optimization enables novel designs that exceed the state-of-the-art nonlinear metasurfaces to date, with the promise of further improvement. The same approach may be extended to other frequency mixing phenomena, such as sum-frequency or difference-frequency generation.

Photon pair generation from lithium niobate metasurface with tunable spatial entanglement [Invited

The two-photon state with spatial entanglement is an essential resource for testing fundamental laws of quantum mechanics and various quantum applications. Its creation typically relies on spontaneous parametric downconversion in bulky nonlinear crystals where the tunability of spatial entanglement is limited. Here, we predict that ultrathin nonlinear lithium niobate metasurfaces can generate and diversely tune spatially entangled photon pairs. The spatial properties of photons including the emission pattern, rate, and degree of spatial entanglement are analyzed theoretically with the coupled mode theory and Schmidt decomposition method. We show that by leveraging the strong angular dispersion of the metasurface, the degree of spatial entanglement quantified by the Schmidt number can be decreased or increased by changing the pump laser wavelength and a Gaussian beam size. This flexibility can facilitate diverse quantum applications of entangled photon states generated from nonlinear metasurfaces.

Coherent all-optical steering of upconverted light by a nonlinear metasurface

In recent years a strong drive towards the miniaturization of nonlinear optics has been motivated by the functionalities it could empower in integrated devices. Among these, the upconversion of near-infrared photons to the visible and their manipulation is fundamental to downscale optical information. We propose a dual-beam scheme whereby a pulse at the telecom frequency ω (1550 nm wavelength) is mixed with its frequency-doubled replica at 2ω. When the two pump pulses are superimposed on a nonlinear, all-dielectric metasurface two coherent frequency-tripling pathways are excited: third-harmonic generation (THG, ω+ω+ω) and sum-frequency generation (SFG, ω+2ω). Their coherent superposition at 3ω produces interference, which we enable by filtering the k-space with the metasurface diffraction. The steering of the emission among diffraction orders, is sensitive to the relative phase between the two pumps. Therefore, by exploiting the phase as a tuning knob, the upconverted signal can be switched between diffraction orders with an efficiency >90%. The proposed approach can be envisioned as an all-optical method to reroute upconverted telecom photons.

Nonlocal and cascaded effects in nonlinear graphene nanoplasmonics.

The ability of plasmons to focus light on nanometer length scales opens a wide range of enticing applications in optics and photonics, among which the enhancement of nonlinear light-matter interactions for all-optical modulation and spectral diversification emerges as a prominent theme. However, the subwavelength plasmonic near-field enhancement in good plasmonic materials such as noble metals is hindered by large ohmic losses, while conventional phase-matching of fields in bulk nonlinear crystals is not suitable for realizing nonlinear optical phenomena on the nanoscale. In contrast, anharmonic electron motion of free charge carriers in highly-doped graphene, which supports long-lived, highly-confined, and actively-tunable plasmons, renders the carbon monolayer an excellent platform for both plasmonics and nonlinear optics. Here we theoretically explore the enhancement in nonlinear response that can be achieved by interfacing multiple graphene nanostructures in close proximity to trigger nonlocal effects associated with large gradients in the electromagnetic near field. Focusing on second- and third-harmonic generation, we introduce a semianalytical formalism to describe interacting graphene nanoribbons with independent width, location, and electrical doping, so as to realize configurations in which plasmonic resonances may simultaneously enhance both the fundamental optical excitation frequency and harmonic intermediary and/or output frequencies. Our findings reveal the importance of both passive and active tuning in the design of atomically-thin nanostructures for nonlinear optical applications, and in particular emphasize the role played by nonlocal effects in generating an even-ordered nonlinear response that may contribute to other nonlinear optical processes through a cascaded interaction. We anticipate that our findings can aid in the design of actively-tunable nonlinear plasmonic resonators and metasurfaces.

Nonreciprocal transmission of electromagnetic waves with nonlinear active plasmonic metasurfaces

Nonreciprocity is important for optical information processing, full-duplex communications, and protection of sensitive laser equipment from unwanted reflections. However, it is very challenging to obtain strong nonreciprocal response in optical frequencies, especially when nanoscale configurations are considered. In this work, we solve this problem by demonstrating a compact bifacial plasmonic metasurface that acts as an ultrathin nonreciprocal transmission filter at near-infrared frequencies. The proposed nanostructure is simple to be practically implemented, since it is composed of two silver nanostripes with different dimensions placed on both sides of an ultrathin active dielectric spacing layer. The introduced gain leads to an exceptional point formation in the linear operation regime, where unidirectional perfect transmission due to loss compensation is achieved from the presented non-Hermitian parity-time symmetric nanoscale system. The demonstrated plasmonic metasurface breaks the Lorentz reciprocity law at the nanoscale when its nonlinear response is considered, mainly due to its spatially asymmetric geometry combined with enhanced nonlinearity. Strong and broadband nonreciprocity with unity transmission contrast from opposite directions is realized under relatively low-input laser intensity values. Furthermore, asymmetric nonlinear third-harmonic generation with a pronounced contrast is also illustrated by the same nonreciprocal metasurface design. The findings of this work can lead to the realization of various self-induced nonreciprocal nanophotonic configurations, such as integrated ultrafast switches, ultrathin protective coatings, and asymmetric directional imaging devices.

THz Radiation Efficiency Enhancement from Metal-ITO Nonlinear Metasurfaces.

Strong single-cycle THz emission has been demonstrated from nonlinear plasmonic metasurfaces, when excited by femtosecond laser pulses. In order to invoke a higher nonlinear response, such metasurfaces have been coupled to thin indium-tin-oxide (ITO) films, which exhibit an epsilon-near zero (ENZ) behavior in the excitation wavelength range and enhance the nonlinear conversion. However, the THz conductivity of the ITO film also reduces the radiation efficiency of the meta-atoms constituting the metasurface. To overcome this, we etch the ITO layer around the plasmonic meta-atoms, which allows harnessing of the enhanced localized fields due to the ENZ behavior of the remaining ITO film, while improving the THz radiation efficiency. We report an increase of more than 1 order of magnitude in the emitted THz spectral power density, while the energy conversion efficiency approaches 10-6. This simple yet very effective fabrication scheme provides important progress toward increasing the range of applications of nonlinear plasmonic metasurface THz emitters.

Giant Second Harmonic Generation from Membrane Metasurfaces.

Metasurfaces have emerged as a fascinating framework for nonlinear optics, which have advantages of a compact footprint and unprecedented flexibility in manipulating light. But their nonlinear responses are generally limited by the short interaction lengths with light. Therefore, further enhancement is highly desired for building high-efficiency nonlinear devices. Here, we experimentally demonstrate a record high second harmonic generation (SHG) efficiency of 2.0 × 10-4 using lithium niobate (LN) membrane metasurfaces. Benefiting from the large refractive index contrast in the vertical direction and high fabrication quality, distinct spectral resonances and tight field confinements in the LN layer were achieved. Strong SHG peaks resulting from pump resonances of the metasurfaces were observed. Our nonlinear efficiency is more than 2 orders of magnitude larger than previously reported LN metasurfaces. The results inspire a way to improve the efficiency of nonlinear metasurfaces for ultracompact nonlinear light sources in applications of nonlinear holography, Li-Fi, beam shaping, etc.

Anomalous wavefront control via nonlinear acoustic metasurface through second-harmonic tailoring and demultiplexing

We propose a nonlinear acoustic metasurface concept by exploiting the nonlinearity of locally resonant unit cells formed by curved beams. The analytical model is established to explore the nonlinear phenomenon, specifically the second-harmonic generation (SHG) of the nonlinear unit cell, and validated through numerical and experimental studies. By tailoring the phase gradient of the unit cells, nonlinear acoustic metasurfaces are developed to demultiplex different frequency components and achieve anomalous wavefront control of SHG in the transmitted region. To this end, we numerically demonstrate wave steering, wave focusing, and self-bending propagation. Our results show that the proposed nonlinear metasurface provides an effective and efficient platform to achieve significant SHG and separate different harmonic components for wavefront control of individual harmonics. Overall, this study offers an outlook to harness nonlinear effects for acoustic wavefront tailoring and develops potential toward advanced technologies to manipulate acoustic waves.

Terahertz Pulse Generation with Binary Phase Control in Nonlinear InAs Metasurface.

The effect of terahertz (THz) pulse generation has revolutionized broadband coherent spectroscopy and imaging at THz frequencies. However, THz pulses typically lack spatial structure, whereas structured beams are becoming essential for advanced spectroscopy applications. Nonlinear optical metasurfaces with nanoscale THz emitters can provide a solution by defining the beam structure at the generation stage. We develop a nonlinear InAs metasurface consisting of nanoscale optical resonators for simultaneous generation and structuring of THz beams. We find that THz pulse generation in the resonators is governed by optical rectification. It is more efficient than in ZnTe crystals, and it allows us to control the pulse polarity and amplitude, offering a platform for realizing binary-phase THz metasurfaces. To illustrate this capability, we demonstrate an InAs metalens, which simultaneously generates and focuses THz pulses. The control of spatiotemporal structure using nanoscale emitters opens doors for THz beam engineering and advanced spectroscopy and imaging applications.

Chiral Third-Harmonic Metasurface for Multiplexed Holograms.

Chiral nonlinear metasurfaces could natively synergize nonlinear wavefront manipulation and circular dichroism, offering enhanced capacity for multifunctional and multiplexed nonlinear metasurfaces. However, it is still quite challenging to simultaneously enable strong chiral response, precise wavefront control, high nonlinear conversion efficiency, and independent functions on spins and chirality. Here, we propose and experimentally demonstrate multiplexed third-harmonic (TH) holograms with four channels based on a chiral Au-ZnO hybrid metasurface. Specifically, the left- and right-handed circularly polarized (LCP and RCP) components of the TH holographic images can be designed independently under the excitation of an LCP (or RCP) fundamental beam. In addition, the TH conversion efficiency is measured to be as large as 10-5, which is 8.6 times stronger than that of a bare ZnO film with the same thickness. Thus, our work provides a promising platform for realizing efficient and multifunctional nonlinear nanodevices.

Nonlinear Chiroptical Holography with Pancharatnam–Berry Phase Controlled Plasmonic Metasurface

AbstractMetasurface optical holography represents an important technique for developing ultrathin diffractive optical elements. Among various designs, the metasurface devices with strong chiroptical responses offer a new degree of freedom to manipulate light fields. However, in a linear optical regime, it is usually complicated to realize strong chiroptical properties with metasurfaces. Here, nonlinear chiroptical holography using the Pancharatnam–Berry phase controlled achiral metasurface is reported. The metasurface consists of mirror symmetry breaking plasmonic meta‐atoms. Under the pumping of a fundamental wave, the achiral meta‐atoms radiate second harmonic waves with strong circular dichroism and spin dependent Pancharatnam–Berry phase. Both the amplitude and phase of the second harmonic waves can be independently and simultaneously controlled at the subwavelength scale. As a proof of concept, the spin selective nonlinear chiroptical holography is experimentally demonstrated through the second harmonic process on gold plasmonic metasurfaces. The proposed nonlinear metasurface with Pancharatnam–Berry phase and chiroptical properties open new avenues for multifunctional wavefront engineering and optical information processing.

Dual‐Band Chiral Nonlinear Metasurface Supported by Quasibound States in the Continuum

AbstractThis paper presents an all‐dielectric chiral metasurface composed of an array of two‐layer distorted square structures with nanoholes. This metasurface can simultaneously generate dual‐band opposite chiral responses, which can be attributed to the bound states in the continuum (BICs) and the distorted chiral structure. By combining the BICs with chirality, a dual‐band chiral nonlinear metasurface and a chiral‐sensing method are proposed. The simulated results show that the third harmonic generation (THG) conversion efficiency can reach the order of 10−4 for two peaks with a peak‐pump intensity of approximately 5.3 GW cm−2 in the near‐infrared region. Moreover, the third‐harmonic circular dichroism for each peak can reach up to 0.99 and ‐0.94, respectively. Furthermore, it is theoretically demonstrated that this metasurface can be used for chiral sensing with high sensitivities. These results provide new insights for linear and nonlinear spin‐dependent applications.

Continuous amplitude control of second harmonic waves from the metasurfaces through interference paths

Nonlinear plasmonic metasurfaces represent a promising platform for generating and controlling the multiple degrees of freedom of harmonic waves at the subwavelength scale. Among various functionalities, the amplitude control of the harmonic waves is usually achieved by varying the fundamental frequency and the pumping power. However, these kinds of methods lack the ability to control the energy distributions of the nonlinear waves at different diffraction orders. Here, we report the continuous intensity control of the harmonic waves from the plasmonic metasurfaces through interference paths. The metasurfaces consist of geometric phase controlled gold meta-atoms with threefold rotational symmetry. By controlling the relative phase of two neighboring metasurface paths, the intensity of the diffracted second harmonic waves can be artificially modulated. Our findings suggest that the conventional interference technique represents a powerful route for controlling the radiation of the nonlinear waves from sub-wavelength meta-atoms and may have great applications in developing ultra-compact nonlinear optical sources.

Control of second-harmonic generation in all-dielectric intersubband metasurfaces by controlling the polarity of χ(2).

All-dielectric metasurfaces have recently led to a paradigm shift in nonlinear optics as they allow for circumventing the phase matching constraints of bulk crystals and offer high nonlinear conversion efficiencies when normalized by the light-matter interaction volume. Unlike bulk crystals, in all-dielectric metasurfaces nonlinear conversion efficiencies primarily rely on the material nonlinearity, field enhancements, and the modal overlaps, therefore most efforts to date have only focused on utilizing these degrees of freedom. In this work, we demonstrate that for second-harmonic generation in all-dielectric metasurfaces, an additional degree of freedom is the control of the polarity of the nonlinear susceptibility. We demonstrate that semiconductor heterostructures that support resonant nonlinearities based on quantum-engineered intersubband transitions provide this new degree of freedom. We can flip and control the polarity of the nonlinear susceptibility of the dielectric medium along the growth direction and couple it to the Mie-type photonic modes. Here we demonstrate that engineering the χ(2) polarity in the meta-atom enables the control of the second-harmonic radiation pattern and conversion efficiency. Our results therefore open a new direction for engineering and optimizing second-harmonic generation using all-dielectric intersubband nonlinear metasurfaces.

Inverse design of broadband, strongly-coupled plexcitonic nonlinear metasurfaces

Hybrid photonic structures of plasmonic metasurfaces coupled to atomically thin semiconductors have emerged as a versatile platform for strong light–matter interaction, supporting both strong coupling and parametric nonlinearities. However, designing optimized nonlinear hybrid metasurfaces is a complex task, as the multiple parameters’ contribution to the nonlinear response is elusive. Here we present a simple yet powerful strategy for maximizing the nonlinear response of the hybrid structures based on evolutionary inverse design of the metasurface’s near-field enhancement around the excitonic frequency. We show that the strong coupling greatly enhances the nonlinear signal, and that its magnitude is mainly determined by the Rabi splitting, making it robust to geometrical variations of the metasurface. Furthermore, the large Rabi splitting attained by these hybrid structures enables broadband operation over the frequencies of the hybridized modes. Our results constitute a significant step toward achieving flexible nonlinear control, which can benefit applications in nonlinear frequency conversion, all-optical switching, and phase-controlled nonlinear metasurfaces.

Resonant metasurfaces for generating complex quantum states.

Quantum state engineering, the cornerstone of quantum photonic technologies, mainly relies on spontaneous parametric downconversion and four-wave mixing, where one or two pump photons spontaneously decay into a photon pair. Both of these nonlinear effects require momentum conservation for the participating photons, which strongly limits the versatility of the resulting quantum states. Nonlinear metasurfaces have subwavelength thickness and allow the relaxation of this constraint; when combined with resonances, they greatly expand the possibilities of quantum state engineering. Here, we generated entangled photons via spontaneous parametric downconversion in semiconductor metasurfaces with high-quality factor, quasi-bound state in the continuum resonances. By enhancing the quantum vacuum field, our metasurfaces boost the emission of nondegenerate entangled photons within multiple narrow resonance bands and over a wide spectral range. A single resonance or several resonances in the same sample, pumped at multiple wavelengths, can generate multifrequency quantum states, including cluster states. These features reveal metasurfaces as versatile sources of complex states for quantum information.

Second‐Harmonic Generation in Strained Silicon Metasurfaces

Dielectric metasurfaces supporting Mie resonances can allow significantly boosted and tailored nonlinear light–matter interactions at the nanoscale. However, nonlinear dielectric metasurfaces typically only have odd‐order nonlinearities, unless resorting to material systems such as GaAs, GaP, or LiNbO3, each with unique challenges in device fabrication and integration. As the most widely adopted constituent material of metasurfaces, silicon (Si) does not possess an intrinsic second‐order nonlinear susceptibility. Herein, second‐harmonic generation (SHG) in a Si metasurface strained by a silicon nitride (SiN x ) cladding layer is demonstrated. Utilizing the stress caused by the SiN x layer to break the inversion symmetry of the bulk Si crystal, greatly enhanced SHG in the strained Si metasurface compared with that from an unpatterned Si film with the SiN x cladding layer, with an experimentally measured conversion efficiency as high as 4.2 × 10−5 W−1, is observed. Experiments are further performed and it is concluded that the enhanced SHG is most likely due to the applied stress instead of charged defects in the SiN x cladding. This work opens a new route to realizing dielectric metasurfaces with second‐order nonlinearity in a complementary metal–oxide–semiconductor (CMOS)‐compatible platform.