Enhancement Of Harmonic Generation Research Articles

Ultrafast Permittivity Engineering Enables Broadband Enhancement and Spatial Emission Control of Harmonic Generation in ZnO

Ultrafast Permittivity Engineering Enables Broadband Enhancement and Spatial Emission Control of Harmonic Generation in ZnO

Second harmonic generation and third harmonic enhancement in silicon by composite metasurface and intense terahertz

Second harmonic generation and third harmonic enhancement in silicon by composite metasurface and intense terahertz

Second harmonic generation enhancement based on quasi-BICs in centrosymmetric materials

In centrosymmetric optical materials, the second-order nonlinear polarization of the bulk electric dipolar contribution is zero. More effective utilization of the contribution of the surface term is one of the key methods to efficiently obtain second-order nonlinear responses on these materials. Herein, a design of densely packed slotted nanopillar arrays based on quasi-bound states in the continuum (quasi-BICs) is proposed. The quasi-BICs are analyzed by using the finite element method as an example of silicon and the second harmonic generation (SHG) process is simulated. In the structure, normal-incidence linearly polarized light excites magnetic dipole-like quasi-BICs with a high quality factor which effectively promotes light-matter interactions. Increasing the nanopillar radius or decreasing the lattice constant within a certain range can cause the distribution of quality factors in k-space of the ky direction to contract toward the Γ point, which leads to a quasi-BIC with higher quality factors at the Γ point. By conjunctively adjusting the nanopillar radius and lattice constant or changing the slot azimuth, the resonance wavelength can be adjusted over a wide range (about several hundred nanometers) or finely (within about one nanometer) while maintaining high quality factors. When the symmetry perturbation introduced by the slot is small, it is calculated that the SHG conversion efficiency is about 10−6∼10−5 at an incident light power density of 1 MW/m2, and the SHG power is about 107∼108 times enhancement compared with the structure without slots. As the slot width decreases, higher SHG conversion efficiency with more significant SHG enhancement can be achieved at a specific slot length. The results provide new insights into the modulation of the resonant wavelength and quality factor of quasi-BICs, as well as the control of second-order nonlinear effects in centrosymmetric materials.

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.

Metallic layered VSe2 saturable absorber based single- and dual-wavelength ultrafast fiber laser

Vanadium selenide (VSe2) is a special two-dimensional (2D) transition metal dichalcogenide (TMD) material with metallic properties similar to graphene, which has been proved to have saturable absorption properties and used in mode-locked fiber lasers. As an excellent saturable absorber (SA) material, VSe2 has advantage of ultrafast carrier recovery time and broadband optical response range. However, the potential application of VSe2 in the field of ultrafast photonics has not been fully developed so far. In this work, the as-prepared VSe2 nanosheets were deposited on tapered fiber by optical deposition to obtain VSe2 SA. By inserting VSe2 SA into an Er-doped fiber laser, the mode-locked pulses with a central wavelength of 1574.4 nm can be obtained. The pulse width of the laser is measured to be ∼680 fs which is narrowest in the reported VSe2 SA-based lasers. In addition, the unique dual-wavelength mode-locked pulse is also obtained by further adjusting intracavity dispersion and polarization. This kind of dual-wavelength pulse is valuable in high order harmonic generation enhancement, terahertz wave generation, dense wavelength division multiplexing, dual-frequency comb and other applications. Our results show that metallic VSe2 is of great potential value in ultrafast fiber laser.

Monolithic PMN-39PT nanograting-assisted second harmonic generation enhancement.

Second harmonic generation plays a vital role in frequency conversion which mutually promotes the laser technology and allows the wavebands extension of new coherent source. The monolithic crystals are supposed to be a superior choice for harmonic generation due to long interaction distance, however, the phase-mismatch brought a sharp reduction in the conversion efficiency. Although birefringent phase-matching and quasi-phase-matching techniques are commonly utilized to fill the phase gap in monolithic crystals, these techniques are limited by the natural refractive index of crystal and the domain engineering, respectively. In recent years, subwavelength structures evolve as a flexible scheme to realize phase matching by engineering the geometry features of crystals. Here, structured nanogratings are designed and fabricated on a monolithic PMN-39PT (Pb(Mg1/3Nb2/3)O3-0.39PbTiO3) substrate, a novel ferroelectric crystal with promising optical prospect, for enhancing second harmonic generation, where birefringent or quasi phase-matching is hard to achieve. The nanograting-assisted second harmonic generation enhancement is observed which is not limited by the availability of thin crystalline films. Meanwhile, a boost in the second harmonic signal synchronously promotes the cascading third harmonic generation. This method may provide an alternative solution for enhanced harmonic generation on monolithic substrates and develop potential nonlinear optical materials for frequency conversion.

Third Harmonic Generation Enhancement and Wavefront Control Using a Local High-Q Metasurface.

High quality factor optical nanostructures provide a great opportunity to enhance nonlinear optical processes such as third harmonic generation. However, the field enhancement in these high quality factor structures is typically accompanied by optical mode nonlocality. As a result, the enhancement of nonlinear processes comes at the cost of their local control as needed for nonlinear wavefront shaping, imaging, and holography. Here we show simultaneous strong enhancement and spatial control over third harmonic generation with a local high-Q metasurface relying on higher-order Mie resonant modes. Our results demonstrate third harmonic generation at an efficiency of up to 3.25 × 10-5, high quality wavefront shaping as illustrated by a third harmonic metalens, and a flatband, angle independent, third harmonic response up to ±11° incident angle. The demonstrated high level of local control and efficient frequency conversion offer promising prospects for realizing novel nonlinear optical devices.

Arbitrary fabrication of complex lithium niobate three-dimensional microstructures for second harmonic generation enhancement.

Lithium niobate (LN) crystal plays important roles in future integrated photonics, but it is still a great challenge to efficiently fabricate three-dimensional micro-/nanostructures on it. Here, a femtosecond laser direct writing-assisted liquid back-etching technology (FsLDW-LBE) is proposed to achieve the three-dimensional (3D) microfabrication of lithium niobate (LN) with high surface quality (Ra = 0.422 nm). Various 3D structures, such as snowflakes, graphic arrays, criss-cross arrays, and helix arrays, have been successfully fabricated on the surface of LN crystals. As an example, a microcone array was fabricated on LN crystals, which showed a strong second harmonic signal enhancement with up to 12 times bigger than the flat lithium niobate. The results indicate that the method provides a new approach for the microfabrication of lithium niobate crystals for nonlinear optics.

Enhancement of high-order harmonic generation in graphene by mid-infrared and terahertz fields

We theoretically investigate high-order harmonic generation (HHG) in graphene under mid-infrared (MIR) and terahertz (THz) fields based on a quantum master equation. Numerical simulations show that MIR-induced HHG in graphene can be enhanced by a factor of 10 for fifth harmonic and a factor of 25 for seventh harmonic under a THz field with a peak strength of 0.5 MV/cm by optimizing the relative angle between the MIR and THz fields. To identify the origin of this enhancement, we compare the fully dynamical calculations with a simple thermodynamic model and a nonequilibrium population model. The analysis shows that the enhancement of the high-order harmonics mainly results from a coherent coupling between MIR- and THz-induced transitions that goes beyond a simple THz-induced population contribution. Published by the American Physical Society 2024

Enhancement of High-Order Harmonic Generation in Low-Density Ti Plasma Plumes Induced by Intense Laser Fields

Enhancement of High-Order Harmonic Generation in Low-Density Ti Plasma Plumes Induced by Intense Laser Fields

Multiple High‐Q Optical Modes in a Polymer‐Lithium Niobate Integrated Metasurface

AbstractWith the development of miniaturization and integration, multifunctional optical devices are necessary. However, its practical realization is a critical challenge due to the lack of simple structures with multiple functionalities. Here, a multimode metasurface is proposed by simply placing polymer nanocubes on the lithium niobate (LN) thin film. The intriguing properties of the integrated structure include high‐quality (Q) factors and different spectral characteristics, associated with quasi‐guide modes (GM) and Mie modes, respectively. The experiment demonstration reveals that Q factors of four modes are larger than 1000 and a second harmonic generation (SHG) enhancement factor of 25.4 is obtained, featuring strong light‐matter interaction. Importantly, the abundant spectral characteristics greatly boost three degrees of freedom, i.e., polarization, incident angle, and slot, to realize multifunctional designs. The results provide a sophisticated platform for developing high‐performance LN metasurfaces with the advantages of simplified fabrication processes and multifunctionality. The strategy can also be extended to other material systems, enabling the flexibility of metasurface‐inspired subwavelength engineering.

2D quasi-layered material with domino structure

Interlayer coupling strength dichotomizes two-dimensional (2D) materials into layered and non-layered types. Traditionally, they can be regarded as atomic layers intrinsically linked via van der Waals (vdW) forces or covalent bonds, oriented orthogonally to their growth plane. In our work, we report a material system that differentiates from layered and non-layered materials, termed quasi-layered domino-structured (QLDS) materials, effectively bridging the gap between these two typical categories. Considering the skewed structure, the force orthogonal to the 2D QLDS-GaTe growth plane constitutes a synergistic blend of vdW forces and covalent bonds, with neither of them being perpendicular to the 2D growth plane. This unique amalgamation results in a force that surpasses that in layered materials, yet is weaker than that in non-layered materials. Therefore, the lattice constant contraction along this unique orientation can be as much as 7.7%, tantalizingly close to the theoretical prediction of 10.8%. Meanwhile, this feature endows remarkable anisotropy, second harmonic generation enhancement with a staggering susceptibility of 394.3 pm V−1. These findings endow further applications arranged in nonlinear optics, sensors, and catalysis.

High-throughput investigation of second harmonic generation enhancement in indium tin oxide films: Effects of Sn doping

The doping effect of the Sn atom in indium tin oxide (ITO) plays a crucial role in influencing the epsilon-near-zero (ENZ) behaviors and the related nonlinear optical properties. A ternary (In1−xSnx)2O3 film is fabricated by high-throughput magnetron sputtering technique. The relationship between Sn doping and second harmonic generation (SHG) enhancement is systematically interpreted through comprehensive characterization of structural and optical properties. Significantly, clear microstructural changes associated with different levels of Sn doping are identified by x-ray diffraction and Raman spectroscopy. These changes directly contribute to shifts in the ENZ wavelength (λENZ). The results indicate that the optimal region for SHG enhancement lies within 7.3–10.6 at. % Sn doping. Moreover, it is demonstrated that λENZ can be adjusted by manipulating the formation of electrically inactive defect clusters via Sn substitution at the 24d sites. This study not only provides valuable insight into the mechanism linking Sn doping and SHG enhancement of ITO but also exemplifies the high-throughput exploration of optical functional materials.

The defect-state-assisted enhancement of high harmonic generation in bulk ZnO

Optical modulation of high harmonic generation (HHG) at ultrashort timescales is of fundamental interest and central importance for emerging photonic applications. Traditionally, this modulation is realized by injecting incoherent electrons into the conduction band, which can only result in the suppression of HHG intensity. In this work, we have proposed and demonstrated an all-optical route to amplify a specific order of high harmonic generation in (11-20)-cut wurtzite zinc oxide (ZnO) based on the pump-probe configuration. Specifically, intensity enhancement is demonstrated by tuning the wavelength of the generation middle-infrared pulse when the wavelength of HHG matches the energy of a specific defect state. The maximum enhancement factor is observed to be 1.8, while the modulation speed varies with different defect states, which are 0.1 ps for the 5th HHG and 1.5 ps for the 4th HHG. This work might enlighten a new path for ultrafast modulation of HHG in solids for the future development of all-optical devices.

High harmonic generation enhanced by magnetic dipole resonance in an amorphous silicon metasurface.

We report on the enhancement of high harmonic generation (HHG) yield in a metasurface consisting of amorphous silicon disks in a periodic array on an insulator substrate. The structure was designed and optimized using the finite-difference time-domain method for the maximum enhancement, which reaches the factor of 20-times compared to the unstructred surface. The local field is enhanced by a broadband magnetic resonance mode allowing to use ultrashort laser pulses with Fourier transform limit down to 40 fs. Due to the anisotropic structure of the metasurface, both the local-field enhancement and the HHG yield show strong polarization anisotropy.

Evolutionary design of two-dimensional material Fabry–Perot structures for enhanced second harmonic generation

Abstract The integration of two-dimensional (2D) materials with resonant photonic structures is seen as a promising direction for enhancing its nonlinear optical response. The design of such heterogeneous resonant structures has often relied on multi-parameter sweeps to determine the optimized dimensions of resonant optical structure that results in good resonance characteristics, often in the absence of the 2D material. Such an approach is computationally intensive and may not necessarily result in efficient generation or collection of nonlinear signals from the designed structure. Here, we report hybrid-genetic optimization (HGA) based design and experimental demonstration of second harmonic generation (SHG) enhancement from Fabry–Perot structures of single and double multilayer gallium selenide (GaSe) flakes with bottom silicon dioxide, and index matched polymethyl methacrylate spacer/encapsulation layers. HGA technique utilized here speeds up the multilayer cavity design by 8.8 and 89-times for the single and double GaSe structures when compared to the full parameter-sweep, with measured SHG enhancement of 128- and 400-times, respectively, when compared to a reference sample composed of GaSe layer of optimized thickness on 300 nm silicon dioxide layer. SHG conversion efficiencies obtained from the HGA structures are 1–2 orders of magnitude higher than previous reports on 2D material integrated resonant metasurfaces or Bragg cavities.

Second harmonic generation enhancement of ITO-based ENZ materials and metasurfaces

Second harmonic generation enhancement of ITO-based ENZ materials and metasurfaces

Third harmonic generation enhancement from silicon-based multilayer guided mode resonance structures under a conical mounting condition

We experimentally demonstrate more than four-orders of magnitude enhancement in third harmonic generation from an amorphous silicon layer as thin as 10 nm deposited above silicon nitride guided mode resonance (GMR) structures under a conical mounting condition using a rectangular aperture as a pupil plane mask for the fundamental excitation. The multilayer GMR structure studied here consists of shallow etched one-dimensional silicon dioxide gratings with a silicon nitride intermediate layer and an amorphous silicon nonlinear medium. Under conical mounting, by restricting the fundamental excitation angles along the grating vector direction, while retaining the angles supported by the objective lens along the grating lines, the resonances are made angle insensitive. The forward detected THG enhancement increases from 2860 in the absence of any pupil plane mask, with a uniform fundamental excitation angular span of 2.3° to 4740 and 1.7 × 104 in the presence of rectangular apertures that selectively reduce the excitation angular span along the grating vector direction to 0.86° and 0.43°, respectively. Conical mounting using rectangular aperture pupil masks to engineer the fundamental excitation is a promising approach to enhance nonlinear optical processes from angle sensitive GMR structures.

Stacked chalcogenide metasurfaces for third harmonic generation in the UV range

We show that an appropriately designed chalcogenide metasurface allows the enhancement of harmonic generation in the UV range, a regime that conventional wisdom deems inaccessible because of absorption. Here we exploit a combination of the photonic band structure that forms when stacking As2S3 metasurfaces, phase-locking, nonlinear dispersion, and improved field localization to enhance third harmonic conversion efficiency. We demonstrate an improvement of two orders of magnitude with respect to the single layer counterpart notwithstanding the fact that the harmonic signal is tuned deep in the absorption range at 285 nm.

Polarization Engineered Second Harmonic Generation Enhancement from Amorphous Silicon - Gallium Nitride Heterogeneous Resonant Metasurface

We experimentally demonstrate second harmonic generation (SHG) enhancement from a heterogeneous resonant metasurface consisting of amorphous silicon sub-wavelength gratings supporting resonances within an underlying gallium nitride (GaN) layer. Electromagnetic design studies used to choose the sub-wavelength grating dimensions, corresponding spectral resonances, its angular sensitivity, electric field and non-linear polarization profiles are discussed. The efficient excitation of second-order nonlinearities within the GaN layer requiring longitudinal fundamental field component and efficient extraction of on-axis SHG using in-plane nonlinear polarization components are simultaneously satisfied for fundamental excitation polarized at 45^o, resulting in excitation of TE and TM-like resonances. Experimental studies on the fabricated structures characterizing the linear and nonlinear SHG properties including power, polarization, and spectral dependence are also discussed. The SHG spectral measurements show 1300-times enhancement for 1460 nm fundamental excitation. The SHG enhancement observed for the higher order resonance at 1460 nm is attributed to the trade-off between the increase in the in-plane to out-of-plane nonlinear polarization ratio, resulting in relative increase in on-axis SHG radiation and the decrease in quality factor of the resonances, which lowers the resonance field strength with increasing guided-mode order.