Enhancement Of Second Harmonic Generation Research Articles

Unusual Thermo-Enhanced Second Harmonic Generation in Organic Configurationally-Locked Polyene Crystals.

To modulate nonlinear optical (NLO) effects of crystalline material holds great application potential in the photoelectronic and optical fields. Organic configurationally-locked polyene represents an exciting NLO family with large second harmonic generation (SHG) effects, whereas it is a huge blank to switch and modulate their NLO property through external stimuli. For the first time, here present unusual thermo-enhanced SHG activities are presented in a polyene-based NLO compound, 2-{3-[2-(4-pyrrolidinphenyl)vinyl]-5,5-dimethylcyclohex-2-enylidene}malononitrile (1), giving a record-high magnitude of SHG enhancement up to ≈170% during its isomorphic phase transition. Theoretical analysis discloses this behavior stems from the reduced degree of torsion in the π-conjugated structures in 1, as verified by dihedral angles between its pyrrolidine and phenyl planes. As the first study on thermo-enhanced SHG properties of organic crystals, this work affords a new avenue of modulating physical properties to fabricate high-performance photoelectronic and optical devices.

Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS2: Insight from First-Principles Exciton-State Coupling Formalism and Calculations.

Excitons are vital in the photophysics of materials, especially in low-dimensional systems. The conceptual and quantitative understanding of excitonic effects in nonlinear optical (NLO) processes is more challenging compared to linear ones. Here, we present an ab initio approach to second-order NLO responses, incorporating excitonic effects, that employs an exciton-state coupling formalism and allows for a detailed analysis of the role of individual excitonic states. Taking monolayer h-BN and MoS2 as two prototype 2D materials, we calculate their second harmonic generation (SHG) susceptibility and shift current conductivity tensor. We find strong excitonic enhancement in the NLO responses requires that the resonant excitons are not only optically bright themselves but also able to couple strongly to other bright excitons. Our results explain the occurrence of two strong peaks in the SHG of monolayer h-BN and why the A and B excitons of MoS2 unexpectedly exhibit minimal excitonic enhancement in both SHG and shift current generation.

Enhancing Resonant Second-Harmonic Generation in Bilayer WSe2 by Layer-Dependent Exciton-Polaron Effect.

Two-dimensional (2D) materials serve as exceptional platforms for controlled second-harmonic generation (SHG). Current approaches to SHG control often depend on nonresonant conditions or symmetry breaking via single-gate control. Here, we employ dual-gate bilayer WSe2 to demonstrate an SHG enhancement concept that leverages strong exciton resonance and a layer-dependent exciton-polaron effect. By selectively localizing injected holes within one layer, we induce exciton-polaron states in the hole-filled layer while maintaining normal exciton states in the charge-neutral layer. The distinct resonant conditions of these layers effectively break interlayer inversion symmetry, thereby promoting resonant SHG. This method achieves a remarkable 40-fold enhancement of SHG at minimal electric field, equivalent to conditions near the dielectric-breakdown threshold but using only ∼3% of the critical breakdown field. Our results highlight SHG sensitivity to carrier density and type, offering a new tool for manipulating SHG and probing quantum states in 2D excitonic systems.

Enhancement of second-harmonic generation in a lithium niobate metasurface by exploring the bound states in the continuum.

The nonlinear lithium niobate (LiNbO3), characterized by transparency across a broad spectral range from ultraviolet to mid-infrared, stands out as an ideal material for second-harmonic generation (SHG). The concept of bound states in the continuum (BIC) represents a non-radiative mode embedded within the radiation continuum, offering the capability to confine the electromagnetic field within the nanostructure. Here, we propose the design of a LiNbO3 metasurface utilizing the BIC mechanism to enhance SHG at fundamental wavelengths above 2 µm, which injects new thoughts into the field of integrated optics and on-chip photonics. Notably, we rigorously accounted for the influence of the side-wall angle θ and the corner rounding radius R of the LiNbO3 metasurface, which arises from fabrication tolerances. Considering those influences in the simulation, we achieved a quasi-BIC (q-BIC) with a quality factor (Q-factor) up to 1.44 × 105. Moreover, by considering the depleted pump model, the absolute efficiency of SHG reached 4.09% with a corresponding normalized efficiency of 8.19 × 10-10m2/W under a radiation intensity of 5 kW/cm2. Our research aims to establish a predictive framework through numerical simulations, specifically addressing realistic fabrication problems. This approach is intended to optimize the parameters for LiNbO3 metasurface fabrication, ensuring that the subsequent experiment efforts are efficient. Our findings provide an approach to predicting the optical response in actual structures and inspire new applications in photonics.

Strain-induced ferroelectric phase transition and second-harmonic generation enhancement in NbOCl2 monolayer

Strain-induced ferroelectric phase transition and second-harmonic generation enhancement in NbOCl2 monolayer

Substrate Interference and Strain in the Second-Harmonic Generation from MoSe2 Monolayers.

Nonlinear optical materials of atomic thickness, such as non-centrosymmetric 2H transition metal dichalcogenide monolayers, have a second-order nonlinear susceptibility (χ(2)) whose intensity can be tuned by strain. However, whether χ(2) is enhanced or reduced by tensile strain is a subject of conflicting reports. Here, we grow high-quality MoSe2 monolayers under controlled biaxial strain created by two different substrates and study their linear and nonlinear optical responses with a combination of experimental and theoretical approaches. Up to a 15-fold overall enhancement in second-harmonic generation (SHG) intensity is observed from MoSe2 monolayers grown on SiO2 when compared to its value on a Si3N4 substrate. By considering an interference contribution from different dielectrics and their thicknesses, a factor of 2 enhancement of χ(2) was attributed to the biaxial strain: substrate interference and strain are independent handles to engineer the SHG strength of non-centrosymmetric 2D materials.

Above-Room-Temperature Ferroelectricity and Giant Second Harmonic Generation in 1D vdW NbOI3.

The realization of spontaneous ferroelectricity down to the one-dimensional (1D) limit is both fundamentally intriguing and practically appealing for high-density ferroelectric and nonlinear photonics. However, the 1D vdW ferroelectric materials are not discovered experimentally yet. Here, the first 1D vdW ferroelectric compound NbOI3 with a high Curie temperature TC>450K and giant second harmonic generation (SHG) is reported. The 1D crystalline chain structure of the NbOI3 is revealed by cryo-electron microscopy, whereas the 1D ferroelectric order originated from the Nb displacement along the Nb-O chain (b-axis) is confirmed via obvious electrical and ferroelectric hysteresis loops. Impressively, NbOI3 exhibits a giant SHG susceptibility up to 1572pmV-1 at a fundamental wavelength of 810nm, and a further enhanced SHG susceptibility of 5582pmV-1 under the applied hydrostatic pressure of 2.06GPa. Combing in situ pressure-dependent X-ray diffraction, Raman spectra measurements, and first-principles calculations, it is demonstrated that the O atoms shift along the Nb─O atomic chain under compression, which can lead to the increased Baur distortion of [NbO2I4] octahedra, and hence induces the enhancement of SHG. This work provides a 1D vdW ferroelectric system for developing novel ferroelectronic and photonic devices.

Second-harmonic radiation by on-chip integrable mirror-symmetric nanodimers with sub-nanometric plasmonic gap

Abstract Second-harmonic generation (SHG) facilitated by plasmonic nanostructures has drawn considerable attention, owing to its efficient frequency up-conversion at the nanoscale and potential applications in on-chip integration and nanophotonic devices. Herein, we present a nanodimer array fabricated by nanoimprinting, composed of nanofinger-pair symmetrically leaning at an off-angle with a well-defined sub-nanometric gap. Commonly, geometric symmetry would suppress the far-field SHG due to the near-field cancelling of symmetric surface SH polarization. However, we find that the light-induced surface SH polarization distribution along the wave-vector of incidence could be influenced by the off-angle, which is consistent to the requirement of SH polarization symmetry-breaking in symmetric metallic nanocavity. A dramatic enhancement of far-field SHG is achieved by tuning the off-angle of nanofinger-pair, even approaching up to over 4 orders of magnitude for an optimal value. The demonstration of SHG enhancement on our well-defined plasmonic nanodimer provides a new way of on-chip integration to activate high-efficient SH radiation, which might be potential for applications in novel nonlinear optical nanodevices with remarkable efficiency and sensitivity.

Revealing Enhanced Optical Nonlinearity and Robust Ferromagnetism in Atomically Sharp Stacking Binary-Ternary Magnetic Heterostructures.

Two-dimensional (2D) materials provide a versatile platform for the integration of diverse crystals, enabling the formation of heterostructures with intriguing functionalities. Coherently growing 2D heterostructures are highly desirable for property manipulation due to their strong interfacial interaction. In this work, we propose a general synthesis approach and provide insight into well-designed 2D binary-ternary magnetic heterostructures. Atomically sharp interfaces were achieved in typical lateral and vertical Cr1+mSe2(001)/CuCr2Se4(111) heterostructures owing to their similar lattice arrangement, with the observation of a significant enhancement of optical second-harmonic generation. Further magnetism measurements revealed a Curie temperature up to 360 K and thickness- and temperature-dependent magnetism in this heterostructure. Additionally, we synthesized three analogous 2D magnetic heterostructures in Fe-Cr-S, Co-Cr-S, and Cu-Cr-S systems, demonstrating the ubiquitous nature of the coherent heteroepitaxy. Our work involves the development of an innovative platform for investigating the underlying physics and potential applications of 2D binary-ternary heterostructures as well as the fabrication of associated functional devices.

Observation of Anapole Resonances in Lithium Niobate Metasurfaces with Significantly Enhanced Second Harmonic Generation

AbstractBenefiting from their large second‐order nonlinear coefficients and high integration capabilities, crystalline lithium niobate (LN) films have shown great application prospects in the field of nonlinear metasurfaces. It is necessary to endow LN metasurfaces with optical resonances to further boost nonlinear optical responses. Among these optical resonances, anapole resonances carried by LN metasurfaces have been predicted to efficiently enhance second harmonic generations (SHG) but have never been experimentally realized. Anapole resonance requires ideal nanostructures to have steep sidewalls and a high filling ratio, but the intrinsic hardness and inert chemical properties of LN materials pose great challenges for the fabrication of LN nanostructures. Here, a multi‐gas component dry‐etching technique is proposed to prepare various LN nanostructures, achieving typical LN nanopillar arrays with a sidewall angle of ≈85° at a depth of 300 nm and a filling ratio of 52%. Importantly, nanostructured LN metasurfaces are designed and fabricated to experimentally realize anapole resonances at a fundamental wavelength of ≈800 nm, demonstrating a ≈30‐fold enhancement in second harmonic generation compared with bare LN films. The work provides promising strategies for the versatile fabrication of LN nanostructures and their applications in nonlinear meta‐optics.

Stacking Faults Enabled Second Harmonic Generation in Centrosymmetric van der Waals RhI3.

Second harmonic generation (SHG) in van der Waals (vdW) materials has garnered significant attention due to its potential for integrated nonlinear optical and optoelectronic applications. Stacking faults in vdW materials are a typical kind of planar defect that introduces a degree of freedom to modulate the crystal symmetry and resultant SHG response. However, the physical origin and tunability of stacking-fault-governed SHG in vdW materials remain unclear. Here, taking the intrinsically centrosymmetric vdW RhI3 as an example, we theoretically reveal the origin of stacking-fault-governed SHG response, where the SHG response comes from the energetically favorable AC̅ stacking fault of which the electrical transitions along the high-symmetry paths Γ-M and Γ-K in the Brillion zone play the dominant role at 810 nm. Such a stacking-fault-governed SHG response is further confirmed via structural characterizations and SHG measurements. Furthermore, by applying hydrostatic pressure on RhI3, the correlation between structural evolution and SHG response is revealed with SHG enhancement up to 6.9 times, where the decreased electronic transition energies and higher momentum matrix elements due to the stronger interlayer interactions upon compression magnify the SHG susceptibility. This study develops a promising foundation for nonlinear nano-optics applications through the strategic design of stacking faults.

Combining ultrahigh index with exceptional nonlinearity in resonant transition metal dichalcogenide nanodisks

Second-order nonlinearity in solids gives rise to a plethora of unique physical phenomena ranging from piezoelectricity and optical rectification to optical parametric amplification, spontaneous parametric down-conversion and the generation of entangled photon pairs. Monolayer transition metal dichalcogenides, such as MoS2, exhibit one of the highest known second-order nonlinear coefficients. However, the monolayer nature of these materials prevents the fabrication of resonant objects exclusively from the material itself, necessitating the use of external structures to achieve the optical enhancement of nonlinear processes. Here we exploit the 3R phase of a molybdenum disulfide multilayer for resonant nonlinear nanophotonics. The lack of inversion symmetry—even in the bulk of the material—provides a combination of massive second-order susceptibility, extremely high and anisotropic refractive index in the near-infrared region (n > 4.5) and low absorption losses, making 3R-MoS2 highly attractive for nonlinear nanophotonics. We demonstrate this by fabricating 3R-MoS2 nanodisks of various radii, which support resonant anapole states, and observing substantial (>100-fold) enhancement of second-harmonic generation in a single resonant nanodisk compared with an unpatterned flake of the same thickness. The enhancement is maximized at the spectral overlap between the anapole state of the disk and the material resonance of the second-order susceptibility. Our approach unveils a powerful tool for enhancing the entire spectrum of optical second-order nonlinear processes in nanostructured van der Waals materials, thereby paving the way for nonlinear and quantum high-index transition metal dichalcogenide nanophotonics.

Manipulation of Chiral Nonlinear Optical Effect by Light-Matter Strong Coupling.

Light-matter strong coupling (LMSC) is an intriguing state in which light and matter are hybridized inside a cavity. It is increasingly recognized as an excellent way to control material properties without any chemical modification. Here, we show that the LMSC is a powerful state for manipulating chiral nonlinear optical (NLO) effects through the investigation of second harmonic generation (SHG) circular dichroism. At the upper polariton band in LMSC, in addition to the enhancement of SHG by more than 1 order of magnitude, the responsivity to the handedness of circularly polarized light was largely modified, where sign inversion and increase of the dissymmetry factor were achieved. Quarter waveplate rotation analysis revealed that the LMSC clearly influenced the coefficients associated with chirality in the NLO process and also contributed to the enhancement of nonlinear magnetic dipole interactions. This study demonstrated that LMSC serves as a great platform for controlling chiral and magneto-optics.

Shape unrestricted topological corner state based on Kekulé modulation and enhanced nonlinear harmonic generation.

Topological corner states have been extensively utilized as a nanocavity to increase nonlinear harmonic generation due to their high Q-factor and robustness. However, the previous topological corner states based nanocavities and nonlinear harmonic generation have to comply with particular spatial symmetries of underlying lattices, hindering their practical application. In this work, we design a photonic nanocavity based on shape unrestricted topological corner state by applying Kekulé modulation to a honeycomb photonic crystal. The boundaries of such shape unrestricted topological corner state are liberated from running along specific lattice directions, thus topological corner states with arbitrary shapes and high Q-factor are excited. We demonstrate enhancement of second (SHG) and third harmonic generation (THG) from the topological corner states, which are also not influenced by the geometry shape of corner. The liberation from the shape restriction of corner state and nonlinear harmonic generation are robust to lattice defects. We believe that the shape unrestricted topological corner state may also find a way to improve other nonlinear optical progress, providing great flexibility for the development of photonic integrated devices.

Symmetry-breaking-induced off-resonance second-harmonic generation enhancement in asymmetric plasmonic nanoparticle dimers.

The linear and nonlinear optical properties of metallic nanoparticles have attracted considerable experimental and theoretical research interest. To date, most researchers have focused primarily on exploiting their plasmon excitation enhanced near-field and far-field responses and related applications in sensing, imaging, energy harvesting, conversion, and storage. Among numerous plasmonic structures, nanoparticle dimers, being a structurally simple and easy-to-prepare system, hold significant importance in the field of nanoplasmonics. In highly symmetric plasmonic nanostructures, although the odd-order optical nonlinearity of the near-surface region will be improved because of the enhanced near-fields, even-order nonlinear processes such as second-harmonic generation (SHG) will still be quenched and thus optically forbidden. Under this premise, it is imperative to introduce structural symmetry breaking to realize plasmon-enhanced even-order optical nonlinearity. Here, we fabricate a series of nanoparticle dimers each composed of two gold nanospheres with different diameters and subsequently investigate their structural asymmetry dependent linear and nonlinear optical properties. We find that the SHG intensities of gold nanosphere dimers are significantly enhanced by structural asymmetry under off-resonance excitation while the plasmonic near-field enhancement mainly affects SHG under on-resonance excitation. Our results reveal that symmetry breaking will play an indispensable role when designing novel coupled plasmonic nanostructures with enhanced nonlinear optical properties.

230-fold Enhancement of second-harmonic generation by coupled double resonances in a dolmen-type gold metasurface

Optical metasurfaces, artificial planar nanostructures composed of subwavelength meta-atoms, have attracted significant attention due to their ability to tailor optical nanoscale properties, making them a versatile platform for shaping light in both linear and nonlinear regimes. This paper reports on the realization of second harmonic generation (SHG) enhancement based on a dolmen-type gold metasurface containing two resonances. Nonlinear scattering theory is employed to numerically investigate the SHG enhancement phenomenon in the resonant metasurface. The periodic dolmen-type gold metasurface introduces a diffraction coupling effect between Fano resonance and surface lattice resonance (SLR), providing strong local-field enhancement and significantly enhancing the nonlinear effect. We analyze the influence of the coupling between Fano resonance and SLR on the SHG intensity and achieve a 230-fold enhancement in SHG intensity compared to the single resonance case by adjusting the periodicity of the metasurface. The SHG-enhanced gold metasurface may find applications in sensing, imaging, optical computing, and integrated nonlinear optics.

Boosted Second Harmonic Generation and Cascaded Sum Frequency Generation from a Surface Crystallized Glass Ceramic Microcavity.

The development of novel materials and structures for efficient second-order nonlinear micro/nano devices remains a significant challenge. In this study, the remarkable enhancement of second-harmonic generation (SHG) and cascaded sum frequency generation in whispering gallery mode microspheres made of surface-crystallized glass with a 6-µm Ba2TiSi2O8 crystal layer are demonstrated. Attributed to the core-shell design, the Ba2TiSi2O8 located on the surface can be efficiently coupled with whispering gallery modes, resulting in a highly efficient micron-scale cavity-enhanced second-order optical nonlinearity. Greatly enhanced SHG of the microcavity is observed, which is up to 80 times stronger than that of a non-resonant sample. Furthermore, owing to the wavelength non-selectivity of random quasi-phase matching, ultra-wideband SHG with a strong response ranging from 860 to 1600nm and high-contrast polarization characteristics is demonstrated. The glass-ceramic-based microsphere cavity also boosts the cascading optical nonlinearity, manifested by a two-magnitude enhancement of cascaded sum frequency generation. This work delineates an efficient strategy for boosting nonlinear optical response in glass ceramics, which will open up new opportunities for applications in photonics and optical communications.

Dielectric metasurface evolution from bulk to monolayer by strong coupling of quasi-BICs for second harmonic boosting

2D materials are promising candidates as nonlinear optical components for on-chip devices due to their ultrathin structure. In general, their nonlinear optical responses are inherently weak due to the short interaction thickness with light. Recently, there has been great interest in using quasi-bound states in the continuum (q-BICs) of dielectric metasurfaces, which are able to achieve remarkable optical near-field enhancement for elevating the second harmonic generation (SHG) emission from 2D materials. However, most studies focus on the design of combining bulk dielectric metasurfaces with unpatterned 2D materials, which suffer considerable radiation loss and limit near-field enhancement by high-quality q-BIC resonances. Here, we investigate the dielectric metasurface evolution from bulk silicon to monolayer molybdenum disulfide (MoS2), and discover the critical role of meta-atom thickness design on enhancing near-field effects of two q-BIC modes. We further introduce the strong-coupling of the two q-BIC modes by oblique incidence manipulation, and enhance the localized optical field on monolayer MoS2 dramatically. In the ultraviolet and visible regions, the MoS2 SHG enhancement factor of our design is 105 times higher than that of conventional bulk metasurfaces, leading to an extremely high nonlinear conversion efficiency of 5.8%. Our research will provide an important theoretical guide for the design of high-performance nonlinear devices based on 2D materials.

Giant enhancement of second harmonic generation via merging bound states in the continuum for vacuum ultraviolet radiation

Vacuum ultraviolet (VUV) light plays a crucial role in various scientific and technological fields, such as nanolithography and biomedical treatments. However, the inherent nonlinear optical coefficient of nonlinear optical crystals is typically very low, and increasing the action length is often necessary to improve the nonlinear conversion efficiency. This makes it challenging for these materials to achieve high-density optoelectronic integration at the micro-/nano-scale. In this study, we propose a design for generating coherent VUV radiation close to 175 nm using second harmonic generation (SHG) with an absolute efficiency exceeding 1.2‰ mW−1. This is achieved by merging multiple bound state in the continuum modes in a free-standing photonic crystal slab. Even with fabrication imperfections at a level lower than 10% disorder, the SHG efficiency of the samples remains robust, maintaining an efficiency of at least 2‰. This research provides a beneficial platform for generating efficient VUV light in the nanoscale.

High-Q quasi-bound states in the continuum in C2-symmetric metasurface with enhanced second harmonic generation in two-dimensional materials

Quasi-bound states in the continuum (Quasi-BIC) possess a high quality-factor (Q-factor) that can amplify local electromagnetic fields and nonlinear effects such as second harmonic generation (SHG). In this paper, we propose a silicon metasurface with C2 symmetry. By tuning the structural parameters without breaking the C2 symmetry, three symmetric protected BICs (SP-BICs) are transformed into sharp quasi-BICs dominated by different modes in the nearinfrared spectrum. The quasi-BICs exhibit Q-factors as high as 10370 in C2 symmetric metasurface. Numerical simulations reveal that the toroidal dipole (TD) and magnetic dipole (MD) enhance intercellular coupling and local electromagnetic fields, laying the foundation for generating metasurface with high Q-factor. Furthermore, the longitudinal radiative component of electric quadrupole (EQ) outside the facet promotes enhanced light interaction with the 2D material. Leveraging the robust local electromagnetic fields and radiation characteristics of these quasi-BICs, we have achieved substantial SHG enhancement across multiple wavelengths under continuous wave (CW) operation. The SHG from 2D GaSe flake reaches 14189-fold enhancement. Our results not only offer insights into designing metasurface structures with high Q-factors but also explore the methods of enhancing the interaction between metasurface and 2D materials. The proposed nanostructure has numerous potential applications in nonlinear optics, optoelectronics and signal processing.