Nonlinear Metasurfaces Research Articles

Global Selection Rules and Giant Enhanced Harmonic Generations in LiNbO3 Nonlinear Meta‐Optics

AbstractNonlinear optical metasurfaces provide nanoscale‐level control of harmonic waves, making them highly promising platforms for both fundamental research and applications in nonlinear optics. However, the traditional selection rules theory, which has long served as a guiding principle for nonlinear meta‐optics, is local and neglects the significance of meta‐atomic lattice symmetry. In addition, achieving high‐efficiency harmonic generation along with nonlinear optical Pancharatnam‐Berry (PB) phase control remains challenging. To this end, a novel global selection rule jointly determined by the symmetries of both meta‐atom and lattice is proposed. Nonlinear metasurfaces designed based on this theory enable frequency conversions forbidden by previous local selection rules. A more comprehensive relationship between the nonlinear PB phase and the meta‐atomic rotation angle is revealed. Moreover, an efficient nonlinear PB metasurface platform for second harmonic generations is first demonstrated using LiNbO3 thin films with aligned crystal orientations in a hybrid design. The normalized conversion efficiency reaches approximately two orders of magnitude higher than that of existing nonlinear PB metasurfaces working in the near‐infrared band. These findings not only shed light on the underlying mechanisms of nonlinear light‐matter interactions, but also open up exciting possibilities in terahertz, entangled photon pairs, and high harmonic generations.

Electro-optically Modulated Nonlinear Metasurfaces.

Electrically reconfigurable nonlinear metasurfaces provide dynamic control over nonlinear phenomena such as second-harmonic generation (SHG), unlocking novel applications in signal processing, light switching, and sensing. Previous methods, like electric-field-induced SHG in plasmonic metasurfaces and Stark-tuned nonlinearities in quantum well metasurfaces, face limitations due to weak SHG responses from metals and mid-infrared constraints of quantum wells, respectively. Addressing the need for efficient SHG control in the visible and near-infrared ranges, we present a novel approach using the electro-optic (EO) effect to modulate SHG. By leveraging the exceptional EO and SHG properties of lithium niobate (LN), we integrate the EO effect with SHG within a metasurface framework for the first time. Our LN metasurface achieves an 11.3% modulation depth in SHG amplitude under a ±50 V alternating voltage. These results open new avenues for reconfigurable photonic applications. including tunable nonlinear light sources, quantum optics, and nonlinear information processing.

Nonlinear, Active, and Time-Varying Metasurfaces for Wireless Communications: A perspective and opportunities

Nonlinear, Active, and Time-Varying Metasurfaces for Wireless Communications: A perspective and opportunities

Broadband infrared imaging governed by guided-mode resonance in dielectric metasurfaces

Nonlinear metasurfaces have experienced rapid growth recently due to their potential in various applications, including infrared imaging and spectroscopy. However, due to the low conversion efficiencies of metasurfaces, several strategies have been adopted to enhance their performances, including employing resonances at signal or nonlinear emission wavelengths. This strategy results in a narrow operational band of the nonlinear metasurfaces, which has bottlenecked many applications, including nonlinear holography, image encoding, and nonlinear metalenses. Here, we overcome this issue by introducing a new nonlinear imaging platform utilizing a pump beam to enhance signal conversion through four-wave mixing (FWM), whereby the metasurface is resonant at the pump wavelength rather than the signal or nonlinear emissions. As a result, we demonstrate broadband nonlinear imaging for arbitrary objects using metasurfaces. A silicon disk-on-slab metasurface is introduced with an excitable guided-mode resonance at the pump wavelength. This enabled direct conversion of a broad IR image ranging from >1000 to 4000 nm into visible. Importantly, adopting FWM substantially reduces the dependence on high-power signal inputs or resonant features at the signal beam of nonlinear imaging by utilizing the quadratic relationship between the pump beam intensity and the signal conversion efficiency. Our results, therefore, unlock the potential for broadband infrared imaging capabilities with metasurfaces, making a promising advancement for next-generation all-optical infrared imaging techniques with chip-scale photonic devices.

A synthetic moving-envelope metasurface antenna for independent control of arbitrary harmonic orders

Flexible frequency controls are crucial in many photonic and electronic applications, ranging from communications systems, spectroscopy, and metrology to quantum information processing. However, the state-of-the-art solutions based on nonlinear bulk media, electro-optic effect, and nonlinear metasurfaces incur very limited spectral controllability, and merely a couple of harmonic orders can be independently manipulated. Here, we theoretically propose and experimentally demonstrate synthetic moving-envelope metasurface antennas capable of simultaneously generating arbitrary harmonic orders and independently manipulating their wave properties in a software-defined manner. As proof-of-principle examples, we demonstrate unidirectional frequency transition, frequency comb generation, arbitrary harmonic orders independent control, and their applications in frequency-division multiplexing communications. All these complicated functionalities are achieved by the 1-bit spatiotemporally ON-OFF switching of meta-atoms of the waveguide-integrated metasurface antenna. Our proposed synthetic metasurface antenna solution greatly expands the frontiers of wave engineering and information manipulation, showing promising potential in wireless communications, spectroscopy, metrology, and quantum science.

Gold saturable metasurface for building a wavelength-tunable optical spiking neuron.

Plasmonic resonant metasurfaces have found many applications in nonlinear optics, such as harmonic generation, all-optical modulation, saturable absorption, etc. A saturable absorber, as a key device for pulsing emission, plays an important role in building passively Q-switched or mode-locked fiber lasers. Recently, excitable fiber lasers have attracted much attention in the area of neuromorphic photonics. In this work, a plasmonic metasurface consisting of periodic gold nanorods resonant near 1550 nm is designed and fabricated, which exhibits saturable absorption with a modulation depth of about 2.6%. The saturable metasurface is, for the first time, utilized in an excitable erbium-doped polarization-maintaining fiber laser, acting as a crucial nonlinear term for the dynamics of the optical spiking neuron. Compared to biological neurons, the artificial optical neuron possesses shorter a refractory period, faster pulse encoding capability, and changeable firing rate as a function of cavity length (up to 20 kHz in our experiment). In addition, the optical neuron is tunable in emission wavelength within the range from 1526.3 nm to 1568.2 nm, beneficial to wavelength-division multiplexing in photonic neural networks. The trial of the nonlinear plasmonic metasurface for an excitable laser could inspire new perspectives in constructing optical neurons and extend applications of metasurfaces from conventional nonlinear optics to neuromorphic computing.

Electrically tunable third-harmonic generation using intersubband polaritonic metasurfaces

Nonlinear intersubband polaritonic metasurfaces, which integrate giant nonlinear responses derived from intersubband transitions of multiple quantum wells (MQWs) with plasmonic nanoresonators, not only facilitate efficient frequency conversion at pump intensities on the order of few tens of kW cm-2 but also enable electrical modulation of nonlinear responses at the individual meta-atom level and dynamic beam manipulation. The electrical modulation characteristics of the magnitude and phase of the nonlinear optical response are realized through Stark tuning of the resonant intersubband nonlinearity. In this study, we report, for the first time, experimental implementations of electrical modulation characteristics of mid-infrared third-harmonic generation (THG) using an intersubband polaritonic metasurface based on MQW with electrically tunable third-order nonlinear response. Experimentally, we achieved a 450% modulation depth of the THG signal, 86% suppression of zero-order THG diffraction tuning based on local phase tuning exceeding 180 degrees, and THG beam steering using phase gradients. Our work proposes a new route for electrically tunable flat nonlinear optical elements with versatile functionalities.

Second harmonic generation in monolithic gallium phosphide metasurfaces

Abstract Gallium phosphide (GaP) offers unique opportunities for nonlinear and quantum nanophotonics due to its wide optical transparency range, high second-order nonlinear susceptibility, and the possibility to tailor the nonlinear response by a suitable choice of crystal orientation. However, the availability of single crystalline thin films of GaP on low index substrates, as typically required for nonlinear dielectric metasurfaces, is limited. Here we designed and experimentally realized monolithic GaP metasurfaces for enhanced and tailored second harmonic generation (SHG). We fabricated the metasurfaces from bulk (110) GaP wafers using electron-beam lithography and an optimized inductively coupled plasma etching process without a hard mask. SHG measurements showed a high NIR-to-visible conversion efficiency reaching up to 10−5, at the same level as typical values for thin-film-based metasurface designs based on III–V semiconductors. Furthermore, using nonlinear back-focal plane imaging, we showed that a significant fraction of the second harmonic was emitted into the zeroth diffraction order along the optical axis. Our results demonstrate that monolithic GaP metasurfaces are a simple and broadly accessible alternative to corresponding thin film designs for many applications in nonlinear nanophotonics.

Intersubband polaritonic metasurfaces for high-contrast ultra-fast power limiting and optical switching

Nonlinear intersubband polaritonic metasurfaces support one of the strongest known ultrafast nonlinear responses in the mid-infrared frequency range across all condensed matter systems. Beyond harmonic generation and frequency mixing, these nonlinearities can be leveraged for ultrafast optical switching and power limiting, based on tailored transitions from strong to weak polaritonic coupling. Here, we demonstrate synergistic optimization of materials and photonic nanostructures to achieve large reflection contrast in ultrafast polaritonic metasurface limiters. The devices are based on optimized semiconductor heterostructure materials that minimize the intersubband transition linewidth and reduce absorption in optically-saturated nanoresonators, achieving a record-high reflection contrast of 54% experimentally. We also discuss opportunities to further boost the metrics of performance of this class of ultrafast limiters, showing that reflection contrast as high as 94% may be realistically achieved using all-dielectric intersubband polaritonic metasurfaces.

Intrinsic nonlinear geometric phase in SHG from zincblende crystal symmetry media

Abstract We demonstrate that AlGaAs thin films and metasurfaces generate a distinct intrinsic nonlinear geometric phase in their second harmonic signals, differing significantly from previous studies on nonlinear dielectric, plasmonic, or hybrid metasurfaces. Unlike conventional observations, our study reveals that the second harmonic phase remains unaffected by the linear optical response at both pump and harmonic wavelengths, introducing a novel realm of achievable phase functions yet to be explored. Furthermore, we explore the interplay between this intrinsic nonlinear geometric phase and the geometric phase induced by rotations of nanoresonators within metasurface arrangements. Our findings extend the capabilities of nonlinear wavefront shaping metasurfaces, exploiting phase manipulation to uncover unique phenomena exclusive to the nonlinear regime.

Nanoscale optical nonreciprocity with nonlinear metasurfaces

Optical nonreciprocity is manifested as a difference in the transmission of light for the opposite directions of excitation. Nonreciprocal optics is traditionally realized with relatively bulky components such as optical isolators based on the Faraday rotation, hindering the miniaturization and integration of optical systems. Here we demonstrate free-space nonreciprocal transmission through a metasurface comprised of a two-dimensional array of nanoresonators made of silicon hybridized with vanadium dioxide (VO2). This effect arises from the magneto-electric coupling between Mie modes supported by the resonator. Nonreciprocal response of the nanoresonators occurs without the need for external bias; instead, reciprocity is broken by the incident light triggering the VO2 phase transition for only one direction of incidence. Nonreciprocal transmission is broadband covering over 100 nm in the telecommunication range in the vicinity of λ = 1.5 µm. Each nanoresonator unit cell occupies only ~0.1 λ3 in volume, with the metasurface thickness measuring about half-a-micron. Our self-biased nanoresonators exhibit nonreciprocity down to very low levels of intensity on the order of 150 W/cm2 or a µW per nanoresonator. We estimate picosecond-scale transmission fall times and sub-microsecond scale transmission rise. Our demonstration brings low-power, broadband and bias-free optical nonreciprocity to the nanoscale.

Nonlinear metasurface engineering with disordered gold nanorods on ITO: a cost-effective approach to broadband response, polarization-independence, and weak nonlinear index dispersion.

The strong coupling of epsilon-near-zero materials with nanoantennas has demonstrated enhanced nonlinear optical responses, yet practical challenges persist. Here, we propose an alternative: an ultrathin metasurface featuring broadband response with a weakly dispersive nonlinear index, achieved through a simple implementation. Our metasurface, comprising a disordered gold nanorod array on indium tin oxide, exhibits polarization-independent behavior and a large average nonlinear refractive index of 5 cm2/GW across a broad wavelength range (1000-1300 nm). Enhanced performance is attributed to the weak coupling between gold nanorods and indium tin oxide, offering a cost-effective method for nonlinear optical metasurfaces and a flexible design in nanophotonic applications.

Inverse design of nonlinear metasurfaces for sum frequency generation

Abstract Sum frequency generation (SFG) has multiple applications, from optical sources to imaging, where efficient conversion requires either long interaction distances or large field concentrations in a quadratic nonlinear material. Metasurfaces provide an essential avenue to enhanced SFG due to resonance with extreme field enhancements with an integrated ultrathin platform. In this work, we formulate a general theoretical framework for multi-objective topology optimization of nanopatterned metasurfaces that facilitate high-efficiency SFG and simultaneously select the emitted direction and tailor the metasurface polarization response. Based on this framework, we present novel metasurface designs showcasing ultimate flexibility in transforming the outgoing nonlinearly generated light for applications spanning from imaging to polarimetry. For example, one of our metasurfaces produces highly polarized and directional SFG emission with an efficiency of over 0.2 cm2 GW−1 in a 10 nm signal operating bandwidth.

Tunable third harmonic generation based on high-Q polarization-controlled hybrid phase-change metasurface

Abstract Dielectric metasurfaces have made significant advancements in the past decade for enhancing light–matter interaction at the nanoscale. Particularly, bound states in the continuum (BICs) based on dielectric metasurfaces have been employed to enhance nonlinear harmonic generation. However, conventional nonlinear metasurfaces are typically fixed in their operating wavelength after fabrication. In this work, we numerically demonstrate tunable third harmonic generation (THG) by integrating a dielectric metasurface with the phase-change material Ge2Sb2Te5 (GST). The hybrid phase-change metasurface can support two BICs with different electromagnetic origins, which are transformed into two high-Q quasi-BICs through the introduction of structural asymmetry. The two quasi-BICs are selectively excited by controlling the polarization of incident light, and their wavelengths are tunable due to the phase transition of GST. Notably, the efficiency of THG is significantly enhanced at the fundamental wavelengths corresponding to the two quasi-BICs, and the operating wavelength for THG enhancement can be dynamically tuned through the GST phase transition. Furthermore, the wavelength of THG enhancement can be further tuned by manipulating the polarization of pump light. Additionally, a high-Q analog of electromagnetically induced transparency is numerically achieved through the interaction between a low-Q Mie resonance and a quasi-BIC mode, which also improves the THG efficiency. The high-Q polarization-controlled hybrid phase-change metasurface holds promise for applications in dynamically tunable nonlinear optical devices.

Magnetic modes for enhancing second harmonic generation at ultraviolet frequencies

Enhancing nonlinear frequency conversions at ultraviolet (UV) frequencies holds immense significance in contemporary physics and nanophotonics. In this work, we have theoretically demonstrated a highly efficient UV second-harmonic generation (SHG) in the Al nanorod−LiNbO3 (LN)−Al film nanostructure by two orders of magnitude higher compared to the conventional LiNbO3 nanostructure in this range. This result is acquired by designing a simple Al nanoparticle-Al film plasmonic system that generates magnetic resonances at near-UV frequencies to confine light to the LN, which can highly enhance the electromagnetic field and lead to strong interactions with the large nonlinear susceptibility. Our research provides profound insights into the pivotal role of plasmon-induced magnetic resonance (PIMR) modes in UV-SHG processes, thereby opening up new avenues for the development of nanoscale UV nanosources and nonlinear metasurface applications at subwavelength scale.

Engineering Quantum Light Sources with Flat Optics.

Quantum light sources are essential building blocks for many quantum technologies, enabling secure communication, powerful computing, and precise sensing and imaging. Recent advancements have witnessed a significant shift toward the utilization of "flat" optics with thickness at subwavelength scales for the development of quantum light sources. This approach offers notable advantages over conventional bulky counterparts, including compactness, scalability, and improved efficiency, along with added functionalities. This review focuses on the recent advances in leveraging flat optics to generate quantum light sources. Specifically, the generation of entangled photon pairs through spontaneous parametric down-conversion in nonlinear metasurfaces, and single photon emission from quantum emitters including quantum dots and color centers in 3D and 2D materials are explored. The review covers theoretical principles, fabrication techniques, and properties of these sources, with particular emphasis on the enhanced generation and engineering of quantum light sources using optical resonances supported by nanostructures. The diverse application range of these sources is discussed and the current challenges and perspectives in the field arehighlighted.

Scattering matrix for chiral harmonic generation and frequency mixing in nonlinear metasurfaces

We generalize the concept of optical scattering matrix (S-matrix) to characterize harmonic generation and frequency mixing in planar metasurfaces in the limit of undepleted pump approximation. We show that the symmetry properties of such nonlinear S-matrix are determined by the metasurface symmetries at the macroscopic and microscopic scale. We demonstrate that for description of degenerate frequency mixing processes such as optical harmonic generation, the multidimensional S-matrix can be replaced with a reduced two-dimensional S-matrix. We show that for metasurfaces possessing specific point group symmetries, the selection rules determining the transformation of the reduced nonlinear S-matrix are simplified substantially and can be expressed in a compact form. We apply the developed approach to analyze chiral harmonic generation in nonlinear metasurfaces with various symmetries including rotational, inversion, in-plane mirror, and out-of-plane mirror symmetries. For each of those symmetries, we confirm the results of the developed analysis by full-wave numerical calculations. We believe our results provide a new paradigm for engineering nonlinear optical properties of metasurfaces which may find applications in active and nonlinear optics, biosensing, and quantum information processing.

Spin Unlocked Vortex Beam Generation on Nonlinear Chiroptical Metasurfaces.

Optical vortices with spin and orbital angular momentum (SAM and OAM) states offer multiple degrees of freedom for manipulating optical fields and thus enable great potentials in optical information processing. Recently, the optical metasurface has become an important platform for vortex beam generation and steering. However, the strong spin-orbit interaction on such metasurfaces usually leads to spin locked OAM generation, which limits the complete control of the angular momentum state of light. Here, we propose to solve this constraint using geometric phase controlled nonlinear chiroptical metasurfaces. The metasurface consists of two types of plasmonic meta-atoms which have opposite handedness and exhibit a strong spin-dependent circular dichroism effect. By encoding specific phase singularities and phase gradients to different channels, we experimentally demonstrate the spin unlocked second harmonic beam steering. The proposed nonlinear chiroptical metasurfaces may have important applications in developing multifunctional nonlinear optical devices.

Time-Dependent Ultrafast Quadratic Nonlinearity in an Epsilon-Near-Zero Platform.

Ultrafast nonlinearity, which results in modulation of the linear optical response, is a basis for the development of time-varying media, in particular those operating in the epsilon-near-zero (ENZ) regime. Here, we demonstrate that the intraband excitation of hot electrons in the ENZ film results in a second-harmonic resonance shift of ∼10 THz (40 nm) and second-harmonic generation (SHG) intensity changes of >100% with only minor (<1%) changes in linear transmission. The modulation is 10-fold enhanced by a plasmonic metasurface coupled to a film, allowing for ultrafast modulation of circularly polarized SHG. The effect is described by the plasma frequency renormalization in the ENZ material and the modification of the electron damping, with a possible influence of the hot-electron dynamics on the quadratic susceptibility. The results elucidate the nature of the second-order nonlinearity in ENZ materials and pave the way to the rational engineering of active nonlinear metamaterials and metasurfaces for time-varying applications.

Degenerate spontaneous parametric down-conversion in nonlinear metasurfaces.

We propose a simple scheme of degenerate spontaneous parametric down-conversion (SPDC) in nonlinear metasurfaces or photonic crystal slabs with quasi-guided modes. It employs a band crossing between even- and odd-parity quasi-guided mode bands inside the light cone (above the light line) and a selection rule in the conversion efficiency of the SPDC. The efficiency can be evaluated fully classically via the inverse process of noncollinear second-harmonic generation (SHG). As a toy model, we study the SPDC and SHG in a monolayer of noncentrosymmetric spheres and confirm that the scenario works well to enhance the SPDC.