Nonlinear Devices Research Articles

Lithium niobate on insulator – fundamental opto-electronic properties and photonic device prospects

Abstract Lithium niobate on insulator (LNOI) combines a variety of optoelectronic properties and can meet practical performance requirements that are uncommon in optoelectronic materials. This review introduces the fundamentals and the photonic device concepts that arise from the LNOI materials platform. Firstly, the nonlinear optical response of LNOI is presented, including birefringent phase matching (BPM), modal phase matching (MPM), and quasi-phase matching (QPM). The tunable properties are also introduced, including electro-optical (EO), thermo-optical (TO), and acousto-optical (AO) effects. The structures of nonlinear optical devices, such as ridge waveguides (including periodically polarized inversion waveguides), Mach–Zehnder interferometer (MZI) modulators and micro-resonators (such as disks and rings) are demonstrated. Finally, the future of LNOI devices is discussed. In the already mature and developed optoelectronic material systems, it is rare to find one particular material system supporting so many basic optical components, photonic devices and optoelectronic devices as LNOI does in the field of integrated photonic chips.

High-efficiency nonlinear frequency conversion enabled by optimizing the ferroelectric domain structure in x-cut LNOI ridge waveguide

Abstract Photonic devices based on ferroelectric domain engineering in thin film lithium niobate are key components for both classical and quantum information processing. Periodic poling of ridge waveguide can avoid the selective etching effect of lithium niobate, however, the fabrication of high-quality ferroelectric domain is still a challenge. In this work, we optimized the applied electric field distribution, and rectangular inverted domain structure was obtained in the ridge waveguide which is beneficial for efficient nonlinear frequency conversions. Second harmonic confocal microscope, piezoresponse force microscopy, and chemical selective etching were used to characterize the inverted domain in the ridge waveguide. In addition, the performance of nonlinear frequency conversion of the periodically poled nano-waveguide was investigated through second harmonic generation, and the normalized conversion efficiency was measured to be 1,720 % W−1 cm−2, which is close to 60 % that of the theoretical value. The fabrication technique described in this work will pave the way for the development of high-efficiency, low-loss lithium niobate nonlinear photonic devices.

On the displacement control performance of base-isolated structures incorporating nonlinear negative stiffness device

Low-frequency dominant far-field harmonic-like long period ground motions (FGMs) excitations have the potential to amplify the seismic response of base-isolated structures (BIS) and may result in isolator displacements exceeding their maximum limits. The application of negative stiffness devices (NSD) in isolated structures primarily focuses on SDOF systems, which fails to capture the displacement response of the superstructure on the isolation story. To address this issue, this study proposes the application of NSD to a 2DOF system in a BIS, with root mean square value as the metric for displacement transmissibility. Firstly, the displacement transmissibility of base-isolated structures with negative stiffness devices (BIS-NSD) and BIS is derived using the triple-harmonic balance (T-HB) method and the single-harmonic balance (S-HB) method, respectively. Subsequently, the applicability of the T-HB method and the S-HB method in obtaining analytical solution for the displacement transmissibility of BIS-NSD and BIS is revealed and validated through numerical solution. Parameters are selected based on fixed-point theorem for comparative analysis of the displacement and acceleration transmissibility between BIS-NSD and BIS. Finally, a comparative analysis between BIS-NSD and BIS under FGMs confirms the application advantages of NSD. The results indicate that compared to BIS, BIS-NSD significantly reduces the displacement transmissibility of the superstructure and the isolation story in the low-frequency range. As the primary resonance frequency decreases, NSD widens the vibration bandwidth of BIS. BIS-NSD effectively mitigates the increase in displacement caused by low-frequency ground motions. The acceleration transmissibility demonstrates that, without sacrificing the acceleration of the superstructure, it effectively controls the displacement of the isolation story.

Broadband and ascendant nonlinear optical properties of the wide bandgap material GaN nanowires

Gallium nitride (GaN) nanowire, as a type of wide bandgap nanomaterial, has attracted considerable interest because of its outstanding physicochemical properties and applications in energy storage and photoelectric devices. In this study, we prepared GaN nanowires via a facile chemical vapor deposition method and investigated their nonlinear absorption responses ranging from ultraviolet to near-infrared in the z-scan technology under irradiation by picosecond laser pulses. The experiment revealed that GaN nanowires exhibit remarkable nonlinear absorption characteristics attributed to their wide bandgap and nanostructure, including saturable absorption and reverse saturable absorption. When compared to bulk GaN crystals, the nanowires provide a richer and more potent set of nonlinear optical effects. Furthermore, we conducted an analysis of the corresponding electronic transition processes associated with photon absorption. Under high peak power density laser excitation, two-photon absorption or three-photon absorption dominate, with maximum modulation depths of 73.6%, 74.9%, 63.1% and 64.3% at 266 nm, 355 nm, 532 nm, and 1064 nm, respectively, corresponding to absorption coefficients of 0.22 cm/GW, 0.28 cm/GW, 0.08 cm/GW, and 2.82 ×10−4 cm3/GW2. At lower peak energy densities, GaN nanowires demonstrate rare and excellent saturation absorption characteristics at wavelength of 355 nm due to interband transitions, while saturable absorption is also observed at 532 nm and 1064 nm due to band tail absorption. The modulation depths are 85.2%, 41.9%, and 13.7% for 355 nm, 532 nm, and 1064 nm, corresponding to saturation intensities of 3.39 GW/cm2, 5.58 GW/cm2 and 14.13 GW/cm2. This indicates that GaN nanowires can be utilized as broadband optical limiters and high-performance pulse laser modulating devices, particularly for scarce ultraviolet optical limiters, and saturable absorbers for ultraviolet and visible lasers. Furthermore, our study demonstrates the application potential of wide bandgap nanomaterials in nonlinear optical devices.

Nonlinear self-calibrated spectrometer with single GeSe-InSe heterojunction device.

Computational spectrometry is an emerging field that uses photodetection in conjunction with numerical algorithms for spectroscopic measurements. Compact single photodetectors made from layered materials are particularly attractive since they eliminate the need for bulky mechanical and optical components used in traditional spectrometers and can easily be engineered as heterostructures to optimize device performance. However, such photodetectors are typically nonlinear devices, which adds complexity to extracting optical spectra from their response. Here, we train an artificial neural network to recover the full nonlinear spectral photoresponse of a single GeSe-InSe p-n heterojunction device. The device has a spectral range of 400 to 1100 nm, a small footprint of ~25 × 25 square micrometers, and a mean reconstruction error of 2 × 10-4 for the power spectrum at 0.35 nanometers. Using our device, we demonstrate a solution to metamerism, an apparent matching of colors with different power spectral distributions, which is a fundamental problem in optical imaging.

Twist-Angle-Controlled Nonlinear Circular Dichroism on Gold-Crystal Hybrid Metasurfaces.

Optical chirality, which plays important roles in liquid crystal display and biological and chemical detection, has been attracting scientists' attention due to its potential applications in optical information processing. Usually, the chiral optical response of natural molecules is very weak. However, the emergence of metasurfaces offers a promising solution to solve this issue. By judiciously designing the geometry of meta-atoms, we have realized strong optical circular dichroism (CD) in both linear and nonlinear optical regimes. However, tuning of the CD with a metasurface remains challenging. Here, we propose the twist-angle-controlled nonlinear CD effect by using the second-harmonic generation process on a gold-crystal hybrid metasurface. The CD effect of the second-harmonic waves can be tuned well by controlling the twist angle between the two constituent materials. The proposed hybrid metasurface may open new avenues for developing ultracompact and multifunctional nonlinear optical devices.

Integrated and DC-powered superconducting microcomb

Frequency combs, specialized laser sources emitting multiple equidistant frequency lines, have revolutionized science and technology with unprecedented precision and versatility. Recently, integrated frequency combs are emerging as scalable solutions for on-chip photonics. Here, we demonstrate a fully integrated superconducting microcomb that is easy to manufacture, simple to operate, and consumes ultra-low power. Our turnkey apparatus comprises a basic nonlinear superconducting device, a Josephson junction, directly coupled to a superconducting microstrip resonator. We showcase coherent comb generation through self-started mode-locking. Therefore, comb emission is initiated solely by activating a DC bias source, with power consumption as low as tens of picowatts. The resulting comb spectrum resides in the microwave domain and spans multiple octaves. The linewidths of all comb lines can be narrowed down to 1 Hz through a unique coherent injection-locking technique. Our work represents a critical step towards fully integrated microwave photonics and offers the potential for integrated quantum processors.

Phase Composition of HiVac-VPE Lithium Niobate Optical Waveguides Identified by Spectroscopic Investigations.

High-index contrast lithium niobate waveguides, fabricated by the High Vacuum Vapor-phase Proton Exchange (HiVac-VPE) technique, are very promising for increasing both the optical nonlinear and electro-optical efficiencies of photonic integrated devices. So as to play this role effectively, it is mandatory to know the crystallographic phase composition of waveguides and the position of protonated layers for appropriate tailoring and optimization based on the intended applications. In addition, the estimation of structural disorder and electro-optical properties of the waveguides are also of high interest. Benefiting from Raman spectroscopy, IR reflection, IR absorption, and UV-VIS absorption, the HxLi1-xNbO3 phase compositions, as well as the structural disorder in waveguides, were determined. Based on experimental data on the shift of the fundamental absorption edge, we have quantitatively estimated the electro-optic coefficient r13 in as-exchanged waveguides. The electro-optical properties of the waveguides have been found to be depending on the phase composition. The obtained results allow for reconsidering the proton exchange fabricating process of photonic nonlinear devices and electro-optic modulators based on high-index contrast channel waveguides on the LiNbO3 platform.

Luminescence and two-photon absorption assisted optical limiting properties of Ag-doped CdWO4 nanorods

The emerging demand for the fabrication of nonlinear optical materials with high limits of optical power is obvious in nonlinear optics due to their wide application in photonic devices. We report the linear and third-order nonlinear optical properties of Ag-doped CdWO4 nanorods and their dependence on Ag-doping concentration. CdWO4 nanorods with different Ag concentrations were synthesized by the chemical precipitation method and characterized by UV–Vis absorption, X-ray diffraction (XRD), Raman, Photoluminescence and its lifetime studies, X-ray Photoelectron spectroscopy and Transmission Electron Microscopy (TEM). The introduction of Ag ions has led to an increased redshift in the CdWO4 absorption spectra extended into longer wavelength bands, thus enhancing optical absorption within the visible range. The XRD pattern showed that the nanorods crystallized in a monoclinic wolframite structure. The incorporation of Ag in CdWO4 decreases the luminescence emission intensity due to surface quenching effect. Luminescence lifetime measurement reveals the longer decay lifetime for Ag-doped CdWO4 nanorods due to the reduction of density of defects and deep trap state. The nonlinear optical behaviour of the nanorods was investigated by an Open aperture Z-scan technique at 532 nm using pulsed wave Nd: YAG laser. Experimental results showed that reverse saturable absorption is responsible for the observed nonlinearity in the nanorods. The addition of Ag can significantly improve the nonlinear absorption coefficient and optical limiting effects of CdWO4 which can be used as a potential material in nonlinear optical devices.

Interfacial Second-Harmonic Generation via Superposition of Symmetries in a Double-Resonance-Enhanced Plasmonic Nanocavity.

Second-harmonic generation (SHG) has rapidly advanced with the miniaturization of on-chip devices and has found many applications, including optical frequency conversion, nonlinear imaging, and quantum technology. However, owing to the obvious phase-matching constraints involved in nonlinear optical interactions in bulk crystals and the decrease in the length and strength of nonlinear interactions in nanophotonic and surface/interface systems, improving the SHG efficiency and manipulating its optical properties at the nanoscale are challenging tasks. Herein, a monocrystalline silver microplate and nanocube-coupled nanocavity with double-resonance plasmonic modes and an ultrasmall gap were constructed, resulting in efficiently enhanced SHG. In particular, the SHG from the silver microplate (111) is polarization-dependent, and the anisotropy of the SHG in the plasmonic nanocavity can be further controlled via the superposition of symmetries at the interface and plasmonic waveguide-cavity modes. The interfacial SHG provides technology for developing lattice surface atomic arrangement and nanostructure rapid characterization, nonlinear light sources, and on-chip nonlinear nanophotonic devices.

Studies on the synthesis, growth, and characterization of 2-cyanopyridinium salicylate single crystals for nonlinear optical applications

By employing methanol as the solvent in slow solvent evaporation method, a new nonlinear optical organic single crystal of 2-cyanopyridinium salicylate (2-CPSC) was grown. The lattice parameters of the 2-CPSC crystals were found out to be a = 7.7764(9) Å, b = 12.3938(17) Å, c = 12.3685(18) Å, and β = 94.44º using single crystal X-ray diffraction (SCXRD) analysis. The confirmation of crystalline nature was done by powder XRD analysis. The 2-CPSC crystal's chemical composition and functional groups were confirmed by Fourier transform infrared (FTIR) spectral analysis. The optical study was done by ultraviolet-visible-near infrared (UV–Vis-NIR) spectral analysis showing a cutoff wavelength of 338 nm. Studies on the grown 2-CPSC crystal's dielectric and Vicker's microhardness were also conducted. The linear dependence of photocurrent with the applied electric field was revealed for the grown crystals. The 2-CPSC crystal's third-order nonlinearity was investigated by the single-beam Z-scan technique using a continuous He-Ne laser. The open aperture Z-scan reveals the two-photo absorption mechanism and the closed aperture Z-scan study reveals the positive nonlinearity of the 2-CPSC crystals with third order susceptibility value of χ3=2.6763×10−6(esu). The density functional theory (DFT) method of B3LYP level with the 6–31++G(d,p) basis set was used for different quantum chemical calculations like geometry optimization, natural bond orbital (NBO) analysis, mulliken atomic charge, and molecular electrostatic potential (MEP). The higher nonlinearity of the 2-CPSC can be a potential alternative for commercially available potassium dihydrogen phosphate (KDP) and candidate for its application in nonlinear optical devices like optical limiting and optical switching.

Enhanced second harmonic generation from supercavity mode and magnetic resonance in dumbbell-shaped silicon nanoblock

Abstract Electromagnetic multipole resonance can be excited by dielectric nanostructures of appropriate size to effectively promote light-matter interaction. The interactions between light and nanostructures have the capability to enhance the electromagnetic field in the near field, thereby improving the nonlinear effect of nanostructures. We illustrate that the supercavity mode and magnetic dipole resonance are activated by a single dumbbell-shaped silicon nanoblock (DS-SiNB), to trap the near-field electromagnetic field energy. Enhanced second harmonic generation is achieved by exploiting the localized electromagnetic field at the surface of the nanostructure. Numerical simulations reveal that magnetic quadrupole (MQ) and total electric dipole (TED) can be coupled to the same radiation channel by adjusting continuously the aspect ratio Lout/Ly (the outer edge length to the length of DS-SiNB) of the nanoblock. When the aspect ratio Lout/Ly = 1, the supercavity mode formed by the interference of MQ and TED is excited at λ1 = 1124 nm. And, the strong magnetic resonance mode formed by the coupling of two magnetic dipoles (MD) in the same direction is also excited at λ2 = 1124 nm. Supercavity mode and strong magnetic dipole resonance can effectively capture electromagnetic fields on the surface of nanostructures to attain enhanced second harmonic generation (SHG). Our study presents a novel approach to enhance the nonlinear optical effect of a single silicon nanostructure, which can lead to the development of more efficient nonlinear optical devices.

Extraordinary Enhancement of Nonlinear Optical Interaction in NbOBr2 Microcavities.

2D materials are burgeoning as promising candidates for investigating nonlinear optical effects due to high nonlinear susceptibilities, broadband optical response, and tunable nonlinearity. However, most 2D materials suffer from poor nonlinear conversion efficiencies, resulting from reduced light-matter interactions and lack of phase matching at atomic thicknesses. Herein, a new 2D nonlinear material, niobium oxide dibromide (NbOBr2) is reported, featuring strong and anisotropic optical nonlinearities with scalable nonlinear intensity. Furthermore, Fabry-Pérot (F-P) microcavities are constructed by coupling NbOBr2 with air holes in silicon. Remarkable enhancement factors of ≈630 times in second harmonic generation (SHG) and 210 times in third harmonic generation (THG) are achieved on cavity at the resonance wavelength of 1500nm. Notably, the cavity enhancement effect exhibits strong anisotropic feature tunable with pump wavelength, owing to the robust optical birefringence of NbOBr2. The ratio of the enhancement factor along the b- and c-axis of NbOBr2 reaches 2.43 and 5.27 for SHG and THG at 1500nm pump, respectively, which leads to an extraordinarily high SHG anisotropic ratio of 17.82 and a 10° rotation of THG polarization. The research presents a feasible and practical strategy for developing high-efficiency and low-power-pumped on-chip nonlinear optical devices with tunable anisotropy.

Ultra-sensitive current bistability and light switching in a resonant tunneling superlattice transistor

Bistability in the current–voltage characteristics of semiconductor superlattices and quantum cascade laser structures has the potential for wide-ranging applications, particularly in sensing systems. However, the interdependency of applied bias and current injection in conventional two-terminal structures has led to complications in analysis and rendered the bistability phenomenon difficult to implement in practical applications. Here, we report a new kind of electronic bistability coupled to optical switching in a resonant tunneling bipolar superlattice transistor. This bistability manifests as sharp discontinuities in the collector current with extremely small variations of the applied voltage, which arise from unstable tunneling transmission across the hetero-barrier between the two-dimensional electron gas (2DEG) at the edge of the transistor base and the collector superlattice structure. The electronic transitions between high and low quantum mechanical transmissions are demonstrated to be caused by self-consistent variations of the internal electric field at the heterointerface between the 2DEG and the superlattice. They are also present in the base current of the three-terminal device and result in sharp switching of near-infrared spontaneous light emission output from an interband radiative recombination process with a peak emission wavelength of 1.58 μm. A comprehensive quantum mechanical theoretical model accounting for the self-consistent bistable tunneling transmission is in quantitative agreement with the experimental data. The measured peak transconductance sensitivity value of 6000 mS can be used in the highly sensitive detector and non-linear device applications.

Intense second-harmonic generation in two-dimensional PtSe2

Abstract Platinum diselenide (PtSe2), classified as a noble metal dichalcogenide, has garnered substantial interest owing to its layer-dependent band structure, remarkable air-stability, and high charge-carrier mobilities. These properties make it highly promising for a wide array of applications in next-generation electronic and optoelectronic devices, as well as sensors. Additionally, two-dimensional (2D) PtSe2 demonstrates significant potential as a saturable absorber due to its exceptional nonlinear optical response across an ultrabroad spectra range, presenting exciting opportunities in ultrafast and nonlinear photonics. In this work, we explore the second-order nonlinear optical characteristics of 2D PtSe2 by analyzing its second-harmonic generation (SHG) excited by a pulsed laser at 1064 nm. Our investigation unveils a layer-dependent SHG response in PtSe2, with prominent SHG intensity observed in few-layer PtSe2. The distinct six-fold polarization dependence pattern observed in the SHG intensity reflects the inherent threefold rotational symmetry inherent to the PtSe2 crystal structure. Remarkably, the SHG intensity of 4-layer PtSe2 surpasses that of mechanically exfoliated monolayer molybdenum disulfide (MoS2) by approximately two orders of magnitude (60-fold), underscoring its exceptional second-order nonlinear optical response. Combined with its ultrahigh air-stability, these distinctive nonlinear optical characteristics position two-dimensional PtSe2 as a promising candidate for ultrathin nonlinear nanophotonic devices.

Interfacial second harmonic generation switching with 2D monolayer/VO2 heterostructure

To establish a facile nonlinear optical switching mechanism activated by thermal field, that is compatible with on-chip integration, we develop a physical model to quantify the interfacial second harmonic generation (SHG) of 2D monolayer/3D phase-changing material heterostructure. Our results show that heat-induced phase transition of VO2 can realize temperature-reversible interfacial SHG switching, with an ON-OFF ratio of about 3 and a low temperature threshold of about 60 °C. Experimental results can be well addressed by quantitative calculations based on the physical model. This work constitutes substantial insights into interfacial SHG switching, which will benefit design and construction of on-chip nonlinear optical devices based on 2D monolayers.

The growth aspects and experimental techniques for the characterization of amino acid L-histidine hybrid crystals for nonlinear optical device applications

The development of crystal growth and measurement methods opens new possibilities for studying materials with remarkable nonlinear optical features. The development of bulk crystals is a constant concern to be beneficial for device applications. This study focuses on the development of nonlinear optical crystals of l-histidine complexes, characterization approaches, and prospective applications. The solution growth approach, a straightforward, inexpensive, and low-temperature growth technique, was adopted broadly. Recent studies show that l-histidine derivatives have potential optical, SHG, thermal, dielectric, and mechanical properties, making them an excellent choice for nonlinear optical devices. In this work, structural, spectroscopic, chemical composition, linear and nonlinear optical analyses, thermal, and dielectric characterizations of l-histidine derivatives were conducted. Most of the l-histidine complexes were found to be crystallized in orthorhombic and monoclinic crystal systems with P212121 and P21 space groups. The crystalline perfections of the samples were analyzed by the HR-XRD method. The energy-dispersive X-ray (EDX) spectroscopic technique was applied to evaluate the chemical content of the compounds. FT-IR and FT-Raman techniques were used to recognize the molecular vibrations and functional groups of the l-histidine derivatives. The UV-visible and photoconductivity studies were done to examine the optical behaviors of the developed crystals. Most of the crystals were found to have excellent optical transparency and wide bandgaps. It has been observed that l-histidine hydro-fluoride dehydrate and l-histidine tetrafluoroborate are found to have the highest second harmonic generation (SHG) efficiencies. The dielectric analyses were utilized to study the dielectric constant and dielectric loss variations with the applied frequency. According to the thermal analyses, most of the crystals were found to have substantial thermal stabilities suitable for device applications.

Novel third order nonlinear optical stilbazolium crystal replaced with 3-methoxy benzaldehyde as donor for optical device applications

A novel organic nonlinear optical stilbazolium group single crystal of 1-methyl-2-[2-(3-methoxystyryl)]-pyridinium iodide (subsequently referred to as MSMI) was grown by the solution growth technique using the method of slow evaporation at ambient temperature. The Single-crystal XRD investigation indicates that the MSMI crystal belongs to a monoclinic crystal system with a centrosymmetric space group. CHN elemental analyser confirms the weight percentage of carbon (C = 51.00 %) hydrogen (H = 4.55 %) and nitrogen (N = 3.94 %) in the MSMI crystal structure. The presence of 16 hydrogen atoms and 15 carbon atoms in the MSMI was affirmed by the Nuclear Magnetic Resonance (NMR) spectroscopic analysis. Fourier Transform Infrared (FTIR) studies confirmed the fundamental vibrations for different functional groups found in the MSMI crystal. The Hirsfeld surface analysis figured out the hydrogen bond interaction and π…π interaction which supports the stability of the crystal structure. The crystal is found to exhibit transmittance of wavelength above 400 nm and has a band gap of 3.05 eV ascertained from UV–Vis-NIR spectroscopic analysis. Photoluminescence (PL) studies reveal that the title crystal has an emission wavelength of 572 nm. The surface characteristics of the title crystal were examined by Atomic Force Microscopy (AFM), and etching studies. The value of Meyer's number is n = 1.8 which is determined by the Vickers microhardness studies. The value of the third-order nonlinear refractive index (n2) is 4.662×10−8 cm2/W, the nonlinear absorption coefficient (β) is 1.305×10−3 cm/W, nonlinear susceptibility (χ(3)) is 9.297×10−5 esu and the optical limiting threshold is 11.43 J/cm2 was ascertained form the Z-scan technique. The results indicate that the MSMI crystal is a potential optical limiter and has promising applications in nonlinear optical devices.

High-throughput quantum photonic devices emitting indistinguishable photons in the telecom C-band.

Single indistinguishable photons at telecom C-band wavelengths are essential for quantum networks and the future quantum internet. However, high-throughput technology for single-photon generation at 1550 nm remained a missing building block to overcome present limitations in quantum communication and information technologies. Here, we demonstrate the high-throughput fabrication of quantum-photonic integrated devices operating at C-band wavelengths based on epitaxial semiconductor quantum dots. Our technique enables the deterministic integration of single pre-selected quantum emitters into microcavities based on circular Bragg gratings. Respective devices feature the triggered generation of single photons with ultra-high purity and record-high photon indistinguishability. Further improvements in yield and coherence properties will pave the way for implementing single-photon non-linear devices and advanced quantum networks at telecom wavelengths.

Artificial Domain Patterning in Ultrathin Ferroelectric Films via Modifying the Surface Electrostatic Boundary Conditions.

Nanoscale spatially controlled modulation of the properties of ferroelectrics via artificial domain pattering is crucial to their emerging optoelectronics applications. New patterning strategies to achieve high precision and efficiency and to link the resultant domain structures with device functionalities are being sought. Here, we present an epitaxial heterostructure of SrRuO3/PbTiO3/SrRuO3, wherein the domain configuration is delicately determined by the charge screening conditions in the SrRuO3 layer and the substrate strains. Chemical etching of the top SrRuO3 layer leads to a transition from in-plane a domains to out-of-plane c domains, accompanied by a giant (>105) modification in the second harmonic generation response. The modulation effect, coupled with the plasmonic resonance effect from SrRuO3, enables a highly flexible design of nonlinear optical devices, as demonstrated by a simulated split-ring resonator metasurface. This domain patterning strategy may be extended to more thin-film ferroelectric systems with domain stabilities amenable to electrostatic boundary conditions.