Broadband Second Harmonic Generation Research Articles

Toward Strong UV-Vis-NIR Second-Harmonic Generation by Dimensionality Engineering of Zinc Thiocyanates.

The precise modulation of the spatial orientations and connection modes of primitives is vital for certain critically important optical functions for nonlinear optical (NLO) materials (specifically, second-harmonic generation (SHG) and optical bandgap); however, we are yet to achieve a sufficient level of control for the designed construction of efficient broadband NLO materials. Exploiting the changes in microscopic polarization that may result from dimensional increase, we propose herein a zero-dimensional (0D)-to-three-dimensional (3D) dimensionality-increase strategy to realize strong broadband SHG responses for the first time. The novel 3D pseudo diamond-like Zn(SCN)2 has been synthesized by removing SHG-inactive [NH4]+ counter cations and H2O molecules that are located between the adjacent discrete [Zn(SCN)4] building blocks within the 0D (NH4)2Zn(SCN)4·3H2O. The 0D-to-3D dimensionality engineering, proceeding from (NH4)2Zn(SCN)4·3H2O to Zn(SCN)2, results in significantly enhanced SHG responses and efficient broadband activity (8 × KH2PO4 @ 1064 nm, 4.18 eV bandgap for the former c.f. 2 × β-BaB2O4 @ 380 nm, 30 × KH2PO4 @ 1064 nm, 2 × KTiOPO4 @ 2100 nm, 4.78 eV bandgap for the latter) from the UV to the NIR regions (SHG@300-1050 nm). Theoretical calculations and crystal structure analyses reveal that the coordination-bond-connected [Zn(SCN)4] building blocks within the diamond-like structure of Zn(SCN)2 are responsible for its giant broadband SHG responses.

Chirped periodically poled lithium-niobate-on-insulator micro-waveguides for broadband second-harmonic generation.

Periodically poled lithium niobate (LN) waveguides based on quasi-phase matching schemes, benefiting from their high nonlinear coefficient (d33) and strong optical confinement, are widely employed for implementing efficient second-harmonic generation (SHG). Here, we report broadband SHG in z-cut chirped periodically poled lithium-niobate-on-insulator (CPPLNOI) ridge micro-waveguides. Nearly 90-nm-wide SHG at the telecom band is achieved, along with an averaged normalized efficiency of 7.5%/(W·cm2). We also demonstrate simultaneous generation of second as well as cascaded third and fourth harmonics under direct pumping of femtosecond pulses. This work would benefit applications for frequency conversion of a wideband coherent light source.

Second Harmonic Generation in Apodized Chirped Periodically Poled Lithium Niobate Loaded Waveguides Based on Bound States in Continuum

With the rapid development of optical communication and quantum information, the demand for efficient and broadband nonlinear frequency conversion has increased. At present, most single-frequency conversion processes in lithium niobate on insulator (LNOI) waveguides suffer from lateral leakage without proper design, leading to an additional increase in propagation loss. Achieving broadband frequency conversion also encounters this problem in that there are no relevant works that have solved this yet. In this paper, we theoretically propose an efficient and flat broadband second harmonic generation (SHG) in silicon nitride loaded apodized chirped periodically poled LNOI waveguides. By using a bound states in the continuum (BICs) mechanism to reduce the propagation loss and utilizing the characteristic that the BICs are insensitive to wavelength, an ultra-low-loss wave band of 80 nm is realized. Then, by employing an apodized chirped design, a flat broadband SHG is achieved. The normalized conversion efficiency (NCE) is approximately 222%W−1cm−2, and the bandwidth is about 100 nm. Moreover, the presented waveguides are simple and can be fabricated without direct etching of lithium niobate, exhibiting excellent fabrication tolerance. Our work may open a new avenue for exploring low-loss and flat broadband nonlinear frequency conversion on various on-chip integrated photonic platforms.

Broadband second-harmonic generation based on orientation-patterned II-VI crystals

Broadband second-harmonic generation (SHG) has important applications in many fields, such as femtosecond laser technology, optical communication, and biomedicine. The broadband SHG has been implemented in some crystals; however, it is not clear for forward and backward broadband quasi-phase-matching (QPM) SHGs in orientation-patterned Ⅱ-Ⅵ crystals. In this paper, the characters of orientation-patterned ZnS (OP-ZnS), orientation-patterned ZnSe (OP-ZnSe), and orientation-patterned CdTe (OP-CdTe) are, respectively, studied, including the forward broadband SHG and backward broadband SHG bandwidths at different temperatures. In addition, the influences of temperature on the forward broadband SHG bandwidth are investigated. The forward broadband QPM SHGs of OP-ZnS, OP-ZnSe, and OP-CdTe are obtained, and the backward broadband QPM SHGs cannot be obtained. The influence of temperature on the forward bandwidth is small.

A bond-free PPLN thin film ridge waveguide

Lithium niobate thin film waveguide is attractive in nonlinear frequency conversion, especially in the second harmonic generation (SHG). However, the conventional fabrication method of lithium niobate thin film waveguide requires expensive bonding equipment and the prepared film is easy to peel off. In this paper, a novel fabrication method of PPLN thin film ridge waveguide with a trapezoidal substrate is presented, based on glue bonding. The PPLN waveguide together with its trapezoidal substrate is surrounded with low refractive glue to modulate the vertical refractive index gradient along the waveguide length, which was proved to be useful for broadband SHG with a theoretical bandwidth above 25 nm by changing the substrate thickness from 3 μm to 17 μm. The proposed structure was verified by using a C-band ASE laser as the pump source, where the SHG laser bandwidth is about 11 nm. The power of SHG is 2.55 μw, and the normalized conversion efficiency is 10.5 %/W∙cm2. This work is beneficial to simplify the fabrication process of lithium niobate thin film ridge waveguide, and has certain promotion significance for photonic chip integration.

Broadband second-harmonic generation in an angle-cut lithium niobate-on-insulator waveguide by a temperature gradient.

Frequency conversion via nonlinear wave mixing is an important technology to broaden the spectral range of lasers, propelling their applications in optical communication, spectroscopy, signal processing, and quantum information. Many applications require not only a high conversion efficiency but also a broad phase matching bandwidth. Here, we demonstrate broadband birefringence phase matching (BPM) second-harmonic generation (SHG) in angle-cut lithium niobate-on-insulator (LNOI) ridge waveguides based on a temperature gradient scheme. The bandwidth and shift of the phase matching spectrum can be effectively tuned by controlling the temperature gradient of the waveguide. Broadband SHG of a telecom C-band femtosecond laser is also demonstrated. The approach may open a new avenue for tunable broadband nonlinear frequency conversion in various integrated photonics platforms.

Hybrid plasmonic–dielectric metal-nanowire coupler for high-efficiency broadband nonlinear frequency conversion

Pursuing nanometer-scale nonlinear converters based on second harmonic generation (SHG) is a stimulating strategy for bio-sensing, on-chip optical circuits, and quantum information processing, but the light-conversion efficiency is still poor in such ultra-small dimensional nanostructures. Herein, we demonstrate a highly enhanced broadband frequency converter through a hybrid plasmonic–dielectric coupler, a ZnTe/ZnO single core–shell nanowire (NW) integrated with silver (Ag) nanoparticles (NPs). The NW dimension has been optimized to allow the engineering of dielectric resonances at both fundamental wave and second harmonic frequencies. Meanwhile, the localized surface plasmon resonances are excited in the regime between the Ag NPs and ZnTe/ZnO dielectric NW, as evidenced by plasmon-enhanced Raman scattering and resonant absorption. These two contributors remarkably enhance local fields and consequently support the strong broadband SHG outputs in this hybrid nanostructure by releasing stringent phase-matching conditions. The proposed nanoscale nonlinear optical converter enables the manipulation of nonlinear light–matter interactions toward the development of on-chip nanophotonic systems.

铌酸锂微纳波导中的二阶非线性光学效应研究进展

<p indent="0mm">Lithium niobate (LiNbO₃, LN) crystal has a large second-order nonlinear coefficient (<italic>d</italic>₃₃=25.2 pm/V@1064 nm), wide transparent window (0.35–5 μm), and stable periodic microdomain structure preparation, which is a good platform for the study and application of second-order nonlinear optical effects. Lithium niobate thin film (LNTF) is regarded as a promising integrated photonics platform due to its excellent linear and nonlinear optical properties. As the basic unit of an integrated optical system, lithium niobate micro/nano waveguide has been studied as a transmission and control device, and it shows excellent second-order nonlinear optical characteristics. The second-order nonlinearity plays an important role in modern optics, including second-harmonic generation (SHG), sum- and difference-frequency generation, parametric down conversion, and parametric oscillation. Efficient and compact wavelength converters based on second-order nonlinearity are key components for a wide range of applications, including entangled photon sources, optical parametric oscillators, and optical parametric amplifiers. The second-order nonlinear polarization intensity is proportional to the square of the electric field intensity. Micro/nano optical waveguides can improve the light intensity in the device through the local characteristics of the spatial light field, to improve the conversion efficiency of the nonlinear processes. And significantly enhanced electric field strength makes the normalized nonlinear conversion efficiency of LNTF waveguides exceed that of the reverse proton<bold> </bold>exchange lithium niobate waveguides (frequency conversion efficiency 150% W^–1 cm^–2@1550 nm) by one order of magnitude. The nonlinear conversion efficiency of LNTF micro/nano waveguides can be further improved through mode phase matching (MPM) or quasi-phase matching (QPM) to optimize the spatial overlap between the eigenmodes involved in the nonlinear process. The detailed theory, fabrication and application were demonstrated in the manuscript as follows: (1) The theory of second harmonic generation. As an example of second-order nonlinear process, the factors affecting the conversion efficiency of second harmonic generation were analyzed, and can be summarized as nonlinear coefficient, mode special overlap, mode area and phase-matching condition. (2) The fabrication of periodically poled lithium niobate waveguides and periodically poled technics. Based on the micro fabrication processes such as electron beam lithography, dry etching and chemico-mechanical polishing, the propagation loss could be reduced to <sc>0.027 dB/cm.</sc> With the combination of low loss waveguides and the electrode polarization process, periodically poled lithium niobate microstructures and the detailed fabrication processes were discussed in the manuscript. (3) Efficient second harmonic generation based on MPM and QPM. It was reported that the normalized efficiency can reach 1000% W^–1 cm^–2, and we described broadband and tunable SHG in detail. (4) Spontaneous parametric down conversion. With the development of quantum information technology and its application in the fields of secure communication and precision measurement, quantum photon sources with high speed, high brightness and high purity have attracted more and more attention. Due to the strong optical confinement, the micro/nano waveguides reduce the pump power and improve the quality of generated photon pairs, which is helpful to realize the integrated optical path of quantum information processing. In summary, this paper reviews the recent development of second-order nonlinear optical effects in LNTF micro/nano waveguides. Firstly, the theory of second harmonic conversion is introduced, and then the fabrication and periodically poled techniques of LNTF micro/nano waveguides are discussed. As an example, the efficient SHG and parametric down conversion of LNTF waveguides were detailedly demonstrated. The processes of mode phase matching and quasi-phase matching technics, tunable SHG and wideband frequency doubling effect were emphatically investigated.

High-efficiency broadband second-harmonic-generation of YCa4O(BO3)3 crystal

High-efficiency broadband second-harmonic-generation (SHG) of YCa4O(BO3)3 (YCOB) crystal was demonstrated for the first time. The theoretical calculation predicted that the retracing point wavelength for type-I SHG of YCOB crystal was at around 1650 nm, which was proved by the followed phase-matching experiment. With a tunable femtosecond laser as the light source, the type-I SHG experiments of YCOB crystal were performed in the range of 1550–1700 nm. Compared with other broadband SHG crystals, YCOB crystal presented the highest optical conversion efficiency of 58%, the largest spectral bandwidth conversion ratio of 65%, and the broadest wavelength acceptance bandwidth of 118.8 nm·cm1/2.

Broadband second-harmonic generation in step-chirped periodically poled lithium niobate waveguides.

Periodically poled lithium niobate (PPLN) structures on a chip enable efficient second-order nonlinear optical effects, benefiting from the tight light confinement and the utilization of d33. Here, we report a broadband second-harmonic (SH) generation in a step-chirped PPLN waveguide on X-cut lithium niobate on insulator (LNOI). The high fidelity of the poling period is demonstrated over the whole length of 7 mm using a non-destructive technique of piezoresponse force microscopy. The SH signal was continuously observed in the step-chirped PPLN waveguides while scanning the wavelength of the pump laser from 1550 nm to 1660 nm. The SH conversion efficiency was measured to be 9.6 % W-1 cm-2 at 1642 nm. This work will benefit wavelength conversions of light sources with wideband spectra.

Investigation of Mid-Infrared Broadband Second-Harmonic Generation in Non-Oxide Nonlinear Optic Crystals

The mid-infrared (mid-IR) continuum generation based on broadband second harmonic generation (SHG) (or difference frequency generation) is of great interest in a wide range of applications such as free space communications, environmental monitoring, thermal imaging, high-sensitivity metrology, gas sensing, and molecular fingerprint spectroscopy. The second-order nonlinear optic (NLO) crystals have been spotlighted as a material platform for converting the wavelengths of existing lasers into the mid-IR spectral region or for realizing tunable lasers. In particular, the spectral coverage could be extended to ~19 µm with non-oxide NLO crystals. In this paper, we theoretically and numerically investigated the broadband SHG properties of non-oxide mid-IR crystals in three categories: chalcopyrite semiconductors, defect chalcopyrite, and orthorhombic ternary chalcogenides. The technique is based on group velocity matching between interacting waves in addition to birefringent phase matching. We will describe broadband SHG characteristics in terms of beam propagation directions, spectral positions of resonance, effective nonlinearities, spatial walk-offs between interacting beams, and spectral bandwidths. The results will show that the spectral bandwidths of the fundamental wave allowed for broadband SHG to reach several hundreds of nm. The corresponding SH spectral range spans from 1758.58 to 4737.18 nm in the non-oxide crystals considered in this study. Such broadband SHG using short pulse trains can potentially be applied to frequency up-conversion imaging in the mid-IR region, in information transmission, and in nonlinear optical signal processing.

Broadband second-harmonic generation from artificial optical nonlinearity.

In this Letter, we present a mechanism for effectively broadening the bandwidth of second-harmonic generation (SHG) with the metamaterial-based artificial optical nonlinearity. As the nonlinear response of the artificial nonlinearity arising from the magnetoelectric coupling constructed by the meta-molecule (MM) structure, the broadband second-order nonlinearity can be built by simply combining the MMs with different geometrical sizes together. The physical model and the numerical simulation fully support the artificial generation and modulation of the broadband second harmonics. Our work suggests a new route for realizing the on-chip custom-designed nonlinear optical devices with broadband operation.

Three-dimensional nonlinear photonic crystal in naturally grown potassium\u2013tantalate\u2013niobate perovskite ferroelectrics

Since quasi-phase-matching of nonlinear optics was proposed in 1962, nonlinear photonic crystals were rapidly developed by ferroelectric domain inversion induced by electric or light poling. The three-dimensional (3D) periodical rotation of ferroelectric domains may add feasible modulation to the nonlinear coefficients and break the rigid requirements for the incident light and polarization direction in traditional quasi-phase-matching media. However, 3D rotating ferroelectric domains are difficult to fabricate by the direct external poling technique. Here, we show a natural potassium–tantalate–niobate (KTN) perovskite nonlinear photonic crystal with spontaneous Rubik’s cube-like domain structures near the Curie temperature of 40 °C. The KTN crystal contains 3D ferroelectric polarization distributions corresponding to the reconfigured second-order susceptibilities, which can provide rich reciprocal vectors to compensate for the phase mismatch along an arbitrary direction and polarization of incident light. Bragg diffraction and broadband second-harmonic generation are also presented. This natural nonlinear photonic crystal directly meets the 3D quasi-phase-matching condition without external poling and establishes a promising platform for all-optical nonlinear beam shaping and enables new optoelectronic applications for perovskite ferroelectrics.

Broadband second-harmonic generation in a tapered PPLN waveguide

We demonstrate a period poled tapered lithium niobate waveguide and study second harmonic generation (SHG) in this device for the purpose of broadening the quasi-phase matching (QPM) acceptance bandwidth. The finite-difference beam-propagation method is used to simulate the guided modes and calculate the effective indices. The simulation results show that by tapering the width of the cross section linearly, the phase mismatch between a specific input wavelength and its SHG signal can be varied along the propagation length. Ideal SHG phase-matching conditions for a wide range of input wavelengths in communication band from 1 542.5 nm to 1 553.5 nm can be satisfied in different positions of the waveguide.

Broadband second-harmonic and sum-frequency generation with a long-wave infrared laser in AgGaGe5Se12.

Using an 8 µm long-wave infrared laser as the fundamental wave, we achieved second-harmonic generation (SHG) and sum-frequency generation simultaneously in AgGaGe5Se12 and obtained a 4 µm laser output. Among them, SHG was achieved in the 173 nm spectral range of the fundamental wave, which was consistent with theoretical calculations. The average power of the obtained 4 µm laser was 41 mW, corresponding to an optical-to-optical conversion efficiency of 3.2%. The measured temperature acceptance bandwidth (LδT) (FWHM) was 50 K·cm; the angular acceptance bandwidth (Lδθ) (FWHM) was 13.3 mrad·cm; and the average absorption coefficient in the wavelength range of 0.86-11.30 µm was 0.07cm-1. In addition, the spectral acceptance bandwidth (Lδλ) of fundamental wave in AgGaGe5Se12 SHG and the spectral gain bandwidth of frequency downconversion in AgGaGe5Se12 were calculated. In view of the small absorption coefficient, the large temperature acceptance bandwidth, and the large spectral gain bandwidth, we conclude that AgGaGe5Se12 is a suitable nonlinear crystal for high-power short/mid/long-wave infrared lasers and frequency conversions of nanosecond-femtosecond infrared lasers. These results are conducive to the further development of AgGaGe5Se12 lasers.

Effects of Interlayer Coupling and Band Offset on Second Harmonic Generation in Vertical MoS2/MoS2(1-x)Se2x Structures.

Noncentrosymmetric monolayers (MLs) of transition metal dichalcogenides (TMDCs) and their 3R-type vertical stacks provide an ideal platform for studying atomic-scale nonlinear light-matter interaction in terms of second harmonic generation (SHG). Unlike the case of MLs, SHG from artificial stacks can be nontrivially affected by interlayer coupling and band offset between the constituent MLs, where the latter occurs for band-gap-engineered vertical heterostructures (VHs). In order to study these effects, we produced different sets of 3R-type homobilayers (homo-BLs) and heterobilayers (hetero-BLs) composed of MoS2 and its ternary alloy MoS2(1-x)Se2x. We first investigated the impact of interlayer coupling on the SHG response across the A- and B-exciton resonances in the MoS2 homo-BLs. The coupling strength was varied by preparing (i) decoupled BLs (SiO2 intercalated), (ii) weakly coupled BLs (dry transferred), and (iii) strongly coupled BLs (postannealed) and monitored by photoluminescence, Raman, and reflectance difference spectroscopy, and atomic force microscopy. Unlike the decoupled BL, SHG in the coupled BLs cannot be explained by the simple square law in thickness due to coupling-induced band modification. The impact of exciton-resonance offset on SHG was also investigated in the hetero-BLs by controlling the Se concentration in MoS2xSe2(x-1). Although these VHs can significantly broaden the spectral range for efficient SHG by vertically superposing distinct resonances of the constituent MLs, coherent reinforcement of SHG cannot be achieved basically because of the π/2 phase difference between the on-resonance SHG field in one ML and the off-resonance SHG field in the other ML. Upon postannealing, however, the overlapping resonance regime exhibited unexpectedly high SHG enhancement. This may arise from the formation of the strong resonance when the VHs approach ideal 3R-type hetero-BLs. Our approach may be utilized for fully exploiting the TMDC VHs for highly efficient broadband SHG applications.

Robust, efficient, and broadband SHG of ultrashort pulses in composite crystals.

We experimentally demonstrate efficient second-harmonic generation (SHG) of tunable ultrashort pulses of 100 femtoseconds, using a novel method based on composite segmented periodically poled (CSPP) design. The scheme was borrowed from the nuclear magnetic resonance (NMR) composite pulses (CP) of Shaka and Pines. Using CSPP, a broadband and efficient conversion over a bandwidth of 35nm in very short interaction length was achieved. In addition, CSPP showed robustness to temperature changes up to 90°C. Two CSPP schemes with 15 and 31 segments and periodically poled design were implemented on Mg-doped LiNbO3 crystal. The CSPP performance was shown to be superior in all aspects. The experimental results are compared to numerical simulation with excellent agreement.

Ultra-Broadband Second-Harmonic Generation in ZnO Nano-Tetrapod With Over-One-Octave Bandwidth

Broadband nonlinear optical frequency conversion has attracted considerable interest in many applications, such as optical communication, frequency comb generation, and so on. In this letter, we report on the ultra-broadband second-harmonic generation (SHG) from the zinc oxide nano-tetrapod with less stringent phase-matching requirement. Using a super-continuum source together with an optical parametric oscillator as the excitation light, a broadband SHG with over-one-octave bandwidth spanning from the ultraviolet to near-infrared (375–1100 nm) is readily obtained. The SHG dependence of pump polarization and pump power is also characterized systematically. This nanoscale ultra-broadband optical converter may open a new way for various applications ranging from imaging to on-chip all-optical signal processing operations.

Adaptive pumping for spectral control of broadband second-harmonic generation.

Second-harmonic generation (SHG) is always a significant frequency conversion process in nonlinear optics for many great applications but can be limited when broadband spectral laser sources are involved, e.g.,femtosecond pulses. The conversion efficiency can be high, but the spectral control is hard because of the phase-matching (PM) limitation. Recently, a random quasi-phase-matching (QPM) scheme was proposed to make use of highly nonlinear materials that are difficult to be phase matched under traditional configurations. The spectral control is even harder in anisotropic random materials, and the coherence is completely lost. Here, we proposed an approach to solve this problem by coherent light control via feedback-based wavefront shaping. We utilized this method for spectral control of broadband SHG, which can be efficient even in strongly scattering media. Randomly selected wavelengths in the broadband spectra were enhanced with a good selectivity, and the direction was also controlled in a three-dimensional (3D) configuration. This technique paves the way for convenient spatial and spectral control of both linear and nonlinear emissions and a local enhancement of their conversion efficiency, indicating great progress in both random and ultrafast nonlinear optics.

Broadband SHG based on TIR-QPM in a multi-tapered slab – a comparative study with two isotropic semiconductor materials

In this paper, we have done a comparative analysis on the performance of broadband second harmonic generation (SHG) using the concept of Total-Internal-Reflection-Quasi-Phase-Matching in near-infrared (NIR) region when the isotropic multi-tapered semiconductor slab is made of Zinc Telluride (ZnTe) and Cadmium Telluride (CdTe) semiconductors. MATLAB simulation has been carried out to obtain the conversion efficiency and 3db bandwidth when the slab is incident with a broadband fundamental laser radiation and the phenomenon of total internal reflection (TIR) takes place within the slab of 10 mm length. We have also considered the absorption losses, reflection losses and Goos-Hänchen (GH) shift in this process. The effects of variation in temperature, variation of the tapering angles of the slab which is made of semiconductor has been studied for second harmonic radiations in both CdTe and ZnTe crystals. Optimizing these parameters, we can design a wider broadband frequency converter with acceptable peak efficiency.