Harmonic Generation Efficiency Research Articles

Polarization-controlled third harmonic generation by quasi-bound states in the continuum in silicon nanopillar metasurfaces

All-dielectric metasurfaces have received widespread attention due to their low intrinsic loss compared to the metallic counterparts. However, relatively high radiation loss and low quality (Q) factor of the dielectric nanostructures may significantly degrade their nonlinear optical efficiency. Here, we demonstrate that silicon-nanopillar-based metasurfaces supporting quasi bound states in the continuum (BICs) can greatly enhance the efficiency of third harmonic generation (THG). We show that symmetry-protected BICs form at the Γ-point of doubly degenerate band or nondegenerate band can be selectively transformed into quasi BIC through symmetry breaking of our silicon metasurfaces. Benefiting from the high Q and resonance enhancement by the quasi BICs, the THG conversion efficiencies of the silicon metasurface reaches 4.3 × 10-4 with a peak pump intensity of 1.3 GW/cm2, which can be four orders higher than that of a silicon planar film with the same thickness. In addition, the THG intensity is polarization-dependent for the single quasi BIC while it is polarization-independent for the doublet quasi BIC. Our results provide a new strategy for the design of high-efficiency silicon-based optical nonlinear devices.

Structural, optical, second harmonic, and mechanical studies on zinc chloride added alpha-glycine crystals

The slow evaporation solution method was employed to synthesize and crystallize zinc chloride doped α-glycine (ZCAG) single crystals. The single crystal X-ray diffraction studies of pure α-glycine single crystals revealed that the structure belong to primitive monoclinic lattice. Powder X-ray diffraction studies of ZCAG showed the well-defined sharp peaks and formation of centrosymmetric structure with space group P21/n. The increase in lattice volume of ZCAG suggested that the access of zinc chloride into the α-glycine crystal and the entry of zinc chloride to the α-glycine crystal was also established from the energy-dispersive X-ray analysis. Fourier transform infrared spectrum of ZCAG revealed that the functional groups of α-glycine was not transformed due to the introduction of zinc chloride into the lattice. The optical transparency of ZCAG was observed in the UV-visible region, and it exhibited a superior transmittance in the visible region. Energy bandgap value was determined and found to changes while increasing the dopant concentration. An emission peak was observed in the violet region from the photoluminescence spectra. The centrosymmetric ZCAG exhibited second harmonic generation efficiency of 1.44 times higher than standard potassium dihydrogen phosphate, possibly due to local non-centrosymmetry in the lattice, which is further augmented by lattice distortion induced by the dopant. Low dielectric constant and loss of the grown ZCAG crystals showed the remarkable application of non-linear optical. The Meyer index indicates that the grown ZCAG are categorized as soft materials.

Strong enhancement of third harmonic generation from a Tamm plasmon multilayer structure with WS2.

Improving the conversion efficiency is particularly important for the generation and applications of harmonic waves in optical microstructures. Herein, we propose to enhance the efficiency of third harmonic generation by integrating a monolayer WS2 with the metal/dielectric/photonic crystal multilayer structure. The numerical simulations show that the multilayer structure enables to generate the Tamm plasmon mode between the metal film and photonic crystal around the telecommunication wavelength, which is consistent with the experimental result. By measuring with a self-built nonlinear optical micro-spectroscopy system, we find that the third harmonic signal can be reinforced by 16-fold through inserting the monolayer WS2 in the dielectric spacer. This work will provide a new way for improving nonlinear optical response, especially THG in multilayer photonic microstructures.

Enhanced Photon-Pair Generation Based on Thin-Film Lithium Niobate Doubly Resonant Photonic Crystal Cavity

In this work, a doubly resonant photonic crystal (PhC) cavity is proposed to enhance second harmonic generation (SHG) efficiency and photon pair generation rate (PGR). Through the exploration of geometry parameters, a band-edge mode within the light cone is identified as the first harmonic (FH) mode, and a band-edge mode outside the light cone is designated as the second harmonic (SH). Subsequently, by increasing the layers of the core region, a heterostructure PhC cavity is designed. The results showcase a doubly resonant PhC cavity achieving a 133/W SHG efficiency and a photon pair generation rate of 3.7 × 108/s. The exceptional conversion efficiency is attributed to the high quality factors Q observed in the FH and SH modes with values of approximately 280,000 and 2100, respectively. The remarkably high Q factors compensate for nonlinear efficiency degradation caused by detuning, simultaneously making the manufacturing process easier and more feasible. This work is anticipated to provide valuable insights into efficient nonlinear conversion and photon pair generation rates.

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.

Effect of Laser Beam Amplitude Profile on Second Harmonic Generation Efficiency

Effect of Laser Beam Amplitude Profile on Second Harmonic Generation Efficiency

Meta-structure enhanced second harmonic S0 waves for material microstructural changes monitoring

Cumulative second harmonic Lamb waves in nonlinear media feature increasing amplitudes with propagation distance, conducive to the monitoring of material microstructural changes in structures. The phenomenon can be readily generated by zero-order symmetric (S0) mode waves in the low-frequency range. However, in a practical piezoelectric-transducer-activated system, both S0 and A0 (zero-order antisymmetric) mode Lamb waves are inevitably excited, while only the former is responsible for cumulative effects. The generation efficiency of the cumulative second harmonics is then affected by the presence of the A0 waves. To tackle the problem, this study develops a metamaterial structure, referred to as a meta-structure, to tactically enhance the cumulative second harmonic S0 Lamb waves by converting the A0 mode components into S0 mode waves. Topology optimization is conducted to design the meta-structure, which is surface-mounted onto the structure under inspection, to achieve high-efficiency A0-to-S0 wave mode conversion. Through tuning the parameters and constraints of the optimization, the designed single-sided meta-structure breaks the structural symmetry in the thickness direction, while facilitating its practical implementation. Typical scenarios with different meta-structure materials are discussed. Numerical simulations demonstrate that the strain amplitudes of the fundamental S0 mode waves can be increased by 60% with the deployment of the meta-structure, alongside an enhancement of the second harmonic S0 mode waves at different sensing distances. Finally, the designed meta-structure is fabricated via 3D printing technique and tested experimentally on an aluminum plate subjected to thermal aging treatment for monitoring the heating-induced microstructural changes inside the structure. Experimental results confirm an increase in the wave amplitudes of the linear S0 mode waves with the assistance of the meta-structure. The developed system improves the sensitivity of nonlinear Lamb wave-based monitoring methods in characterizing material microstructural changes, which shows great promise for detecting incipient damage in practical structural health monitoring applications.

Growth, mechanical, thermal, electrical, linear, and nonlinear optical studies of urea resorcinol single crystals for NLO applications

Urea Resorcinol (UR) was synthesized and grown using the slow cooling technique to form a possible organic nonlinear optical crystal. Single crystal X-ray diffraction analysis was used to determine the shape and lattice characteristics of the generated UR crystals. The crystallinity was verified using a high-resolution X-ray diffraction examination. The emission and transparency of the formed crystal were revealed by optical studies including photoluminescence and UV–visible-NIR spectrum analyses. Through the use of an optical microscope and the Vickers microhardness tester, its mechanical behavior was investigated and the density of its etch pits was estimated. The investigations were also conducted on the UR crystal's microphysical properties, including its dielectric tensor, dielectric loss, and thermal analysis. An Nd:YAG laser was used to quantify the laser-induced surface damage and the results were connected to the grown crystal's specific heat capacity. By using the Kurtz and Perry technique, the efficiency of second harmonic generation was determined for different UR crystal particle sizes that have good phase matchability, and its SHG output was compared to urea.

Giant enhancement of third harmonic generation via guided mode resonances in notched silicon waveguides

We report a giant enhancement of the third harmonic generation (THG) at 343 nm by periodically notched silicon waveguide arrays supporting guided mode resonances (GMRs) at 1030 nm. Maximum efficiency of the third harmonic generation η = 7.71 × 10−5 is achieved with a peak pump power density of 5.31 GW/cm2. The enhancement factor of the THG from the GMR metasurface reaches up to 1.3 × 107 compared to a flat silicon film with the same thickness. This observation demonstrates a promising approach to design high-efficiency nonlinear optical metasurfaces.

Exploring the physicochemical properties of a new mixed halide 1D hybrid material Zn(C2H8N2)Br1.41Cl0.59 with a non-centrosymmetric structure: Promising material for nonlinear applications

Colorless crystals of a new mixed halide hybrid material, Zn(C2H8N2)Br1.41Cl0.59, were synthesized by the slow evaporation method at room temperature. The crystal structure, thermal behavior, and optical analysis were analyzed to characterize this complex. The crystal structure study revealed that this compound adopts the orthorhombic system and crystallizes in the non-centrosymmetric space group Ima2. Its one-dimensional structure is built from infinite wavy chains of [Zn(C2H8N2)Br1.41Cl0.59]n propagating along the crystallographic a-axis, which are interconnected through NH···Br/Cl hydrogen bonds. Thermogravimetric analysis indicated that this complex remains stable up 251 °C, decomposing in a single step to yield zinc oxide (ZnO) as final product. Differential scanning calorimetry (DSC) revealed an endothermic peak at 195 °C, indicating that the title compound undergoes a phase transition at this temperature. Additionally, the material's suitability for optical application was assessed through UV–Visible absorption and non-linear optical (NLO) techniques. The determined band gap energy of 4.5 eV suggests that this new complex can be classified as a semiconductor material closely resembling an insulator. Furthermore, the second harmonic generation (SHG) efficiency of the grown crystal was analyzed using the Kurtz-Perry powder technique. The IR and Raman spectra confirm the results obtained from X-ray single-crystal structural analyses.

Optical, electrical and thermal investigations on brucinium di-hydrogen citrate tri-hydrate single crystal: An optimistic tool for microelectronics, OPO and OLED applications

Highly capable nonlinear optical brucinium di-hydrogen citrate tri-hydrate (BDHCTH) single crystal under organic material category has been grown-up successfully by slow evaporation method. Optical, electrical, and thermal investigations were made on title crystal to discover the suitability of fabrication of an optical as well as electrical device for the first time. Crystal structure analysis confirms that, the BDHCTH crystal belongs to triclinic crystal system with non-centro symmetric space group P1. The SLDT value of BDHCTH crystal was found to be 4.22 GW/cm2. Second harmonic generation efficiency of the BDHCTH compound is 1.08 times superior to the reference sample KDP. An attribution of single and sharp peak with lesser full width half maximum value confirms the presence of very fewer defects in the grown crystal. An electric response of the title compound shows the normal dielectric behavior. The piezoelectric charge co-efficient (d33) was found to be 4.5 p C/N. Photo luminescence study confirms that the synthesized sample possess violet, blue and red emission behaviors. Presences of various functional groups in the title sample were identified by FT-IR study. Thermal stability of the compound BDHCTH was found to be 135 °C. Kinetic parameters such as activation energy, Arrhenius factor, standard entropy of activation, standard enthalpy of activation, standard Gibb's energy of activation (ΔG*) and induction time of the grown sample were found to be 161.6396 k J mol−1, 7.4854 s−1, -230.8278 J K mol−1, 154.854 k J mol−1, 249.0314 k J mol−1 and 52 days respectively. At the end of an optical, electrical and thermal analysis, we concluded that the grown crystal is an optimistic tool for microelectronics, OPO and OLED applications due to existence of good SHG value, lesser defect and red emission behavior.

AIE‐Active Ferrocene Appended Linear (D‐π‐A) Aromatic Ester Chromophores: Structural, Theoretical and Effect on Phenyl Ring on Luminescence and Nonlinear Optical Properties

AbstractIn the present research, a new ferrocene‐appended linear donor‐π‐acceptor (D‐π‐A) ester chromophore Fc‐(C6H4)2‐COOC2H5 (2) was synthesized and characterized using various spectroscopic techniques. The molecular structure of chromophore 2 was determined using single‐crystal X‐ray diffraction analysis, revealing its crystallization in the monoclinic crystal system with the P21/n space group. The chromophore Fc‐C6H4‐COOC2H4 (1) was utilized to compare its photophysical and nonlinear optical characteristics with those of 2. Cyclic voltammetry revealed a single‐electron transfer mechanism from Fe2+↔Fe3+. The emission solvatochromism studies show a polarized excited state in response to increasing solvent polarity, indicating charge transfer processes. Interestingly, in mixed aqueous media (THF/H2O), the chromophores exhibit intensified fluorescence due to restricted intra‐molecular rotation (RIR), despite weak emission in THF solvent. Chromophore 2 demonstrated 1.5 times higher second harmonic generation (SHG) efficiency than 1, attributed to its extended π‐conjugation from an additional phenyl ring and reduced antiparallel alignments. Despite its centrosymmetric crystal packing, chromophore 2 exhibited SHG efficiency due to non‐covalent interactions (C−H⋅⋅⋅π) in the crystal lattice. Density Functional Theory (DFT) calculations, employing various functionals, provided insights into dipole moment and first hyperpolarizability, with B3LYP‐hybrid functional underestimating hyperpolarizability values owing to long‐range charge transfer interactions within the D‐π‐A systems, aligning closely with experimental findings.

How much length of boron-nitride incorporated benzene like structures can produce efficient harmonic generation at their low-lying excited states?

In this study, exploring the nonlinear optical (NLO) responses by utilizing boron nitride (BN) units as benzene like fused ring chromophores (BTN1-BTN8) are made by correlating their planarity. The chromophore structures containing ring sizes of 3 and 4 (BTN3 and BTN4) demonstrates their significant NLO responses, while higher ring sizes show a decline as their structure become more curved. Their quantum chemical calculations are performed to optimize their molecular structures for their various chemical stability related parameters. Their dipole moments (µtot) ranges between 1.27D for BTN2 to 4.43 D for BTN8 while their average linear polarizability (<α0>) varies from 5.98–7.56 electrostatic units (e.s.u). The chromophore BTN4 exhibits its highest first order hyperpolarizability (β0) value of 9.91 e.s.u. The chromophore BTN3 has the largest second order hyperpolarizability (γ0) value of 11.98 e.s.u and it also has the highest ionization potential (IP) of 5.64 eV, while chromophore BTN4 had a remarkably low EA of −4.91 eV. Their vertical IP (VIP) values ranged from 6.21 eV for BTN1 to 7.56 eV for chromophore BTN7. The chromophore BTN1 displayed a maximum absorption (λmax) at 656 nm with an oscillator strength (f) of 0.0473 and an excitation energy (E) of 1.89 eV. The chromophore BTN4 exhibits a λmax of 366 nm, an f of 0.0012, and an E value of 3.39 eV. The chromophore BTN8 showed the highest λmax value of 1023 nm, an f of 0.0023, and an E value of 1.21 eV.

Modal Phase-Matched Bound States in the Continuum for Enhancing Third Harmonic Generation of Deep Ultraviolet Emission.

Coherent deep ultraviolet (DUV) light sources are crucial for various applications such as nanolithography, biomedical imaging, and spectroscopy. DUV light sources can be generated by using conventional nonlinear optical crystals (NLOs). However, NLOs are limited by their bulky size, inadequate transparency at the DUV regime, and stringent phase-matching requirements for harmonic generation. Recently, dielectric metasurfaces support high Q-factor resonances and offer a promising approach for efficient harmonic generation at short wavelengths. In this study, we demonstrated a crystalline silicon (c-Si) metasurface simultaneously exciting modal phase-matched bound states in the continuum (BIC) resonance at the fundamental wavelength of 840 nm with a higher degree of freedom for precise control of the BIC resonance and a plasmonic resonance at the wavelength of 280 nm in the DUV to enhance third harmonic generation (THG). We experimentally achieved a Q-factor of ∼180 owing to the relatively large refractive index of the c-Si and the geometric symmetry breaking of the structure. We realized THG at a wavelength of 280 nm with a power of 14.5 nW by using a peak power density of 15 GW/cm2 excitation. The measured THG power is 14 times higher than the state-of-the-art THG dielectric metasurfaces using the same peak power density in the DUV regime, and the maximum obtained THG power enhancement factor is up to 48. This approach relies on the significant third-order nonlinear susceptibility of c-Si, the interband plasmonic nature of the c-Si in the DUV, and the strong field confinement of BIC resonance to boost overall nonlinear conversion efficiency to 5.2 × 10-6% in the DUV regime. Our work shows the potential of c-Si BIC metasurfaces for developing efficient and ultracompact DUV light sources using high-efficacy nonlinear optical devices.

Asymmetric-coupled Ge/SiGe quantum wells for second harmonic generation at 7.1 THz in integrated waveguides: a theoretical study

Abstract We present a theoretical investigation of guided second harmonic generation at THz frequencies in SiGe waveguides embedding n-type Ge/SiGe asymmetric coupled quantum wells to engineer a giant second order nonlinear susceptibility. A characteristic of the chosen material system is the existence of large off-diagonal elements in the χ 2 tensor, coupling optical modes with different polarization. To account for this effect, we generalize the coupled-mode theory, proposing a theoretical model suitable for concurrently resolving every second harmonic generation interaction among guide-sustained modes, regardless of which χ 2 tensor elements it originates from. Furthermore, we exploit the presence of off-diagonal χ 2 elements and the peculiarity of the SiGe material system to develop a simple and novel approach to achieve perfect phase matching without requiring any fabrication process. For a realistic design of the quantum heterostructure we estimate second order nonlinear susceptibility peak values of ∼7 and ∼1.4 × 105 pm/V for diagonal and off diagonal χ 2 elements, respectively. Embedding such heterostructure in Ge-rich SiGe waveguides of thicknesses of the order of 10–15 μm leads to second harmonic generation efficiencies comprised between 0.2 and 2 %, depending on the choice of device parameters. As a case study, we focus on the technologically relevant frequency of 7.1 THz, yet the results we report may be extended to the whole 5–20 THz range.

Crystal growth, structural, optical, mechanical characterization and quantum chemical analysis by DFT of an organic nonlinear optical single crystal 4-Hydroxy pyridinium succinate for photonic and optoelectronic devices

A new organic nonlinear optical single crystal 4-Hydroxypyridinium Succinate was synthesized and grown successfully by slow evaporation method using methanol as solvent at ambient temperature. Single crystal X –ray diffraction studies on the grown crystal reveals that 4HPS crystallizes into orthorhombic structure with the non-centrosymmetric space group (Pna21). In structural point of view, the 4-Hydroxypyridinium cation is bonded to the hydrogen succinate anion by direct electron conjugation through nitrogen atom. In addition, the UV visible transmittance spectrum implies that the crystal has high transparency domain in the entire UV visible region with a lower cut-off wavelength of 286 nm. The various functional groups present in the crystal and their frequency assignments are derived from FTIR spectral analysis. The Photoluminescence spectrum brings forth that the grown crystal has violet emission property. The microhardness measurements testify that the crystal belongs to soft material category with reasonable hardness parameters. The compound was found to be thermally stable up to 188 °C without any weight loss from the TGA and DTG traces. The detailed quantum chemical calculation done by density functional theory (DFT) indicates the Homo –Lumo energy gap of the molecule is 3. 956 eV and 4. 289 eV for α and β wave functions respectively. The Laser induced damage threshold of the crystal investigated using Nd: YAG laser of 1064 nm radiation was found to be 21. 93 Gw/cm2. The second harmonic generation efficiency of the 4HPS crystal was confirmed by the emission of green light under Kurtz and Perry powder test.

Nucleation kinetics, chemical etching, hirshfeld surface, and photoluminescence of Rubidium hydrogen oxalate dihydrate NLO single crystal

The nucleation dynamics of a semi-organic Rubidium hydrogen oxalate dihydrate (RbHOH) crystal were assessed using double-distilled water as a solvent medium to obtain good quality crystal using the solution growth technique. Gravimetric analysis of solubility revealed that it has a positive temperature coefficient of solubility, which is appropriate for bulk growth. Other nucleation parameters such as metastable zonewidth, induction period, and interfacial energy were carried out using the classical theory of nucleation. The photoconductivity experiments reveal that the grown crystal exhibits a positive photoconductivity nature. Chemical etching and atomic force microscopy (AFM) experiments were performed on the produced crystal surface. From AFM experiments, effectively assessed amplitude parameters were calculated. Etching studies showed the presence of etch pit patterns such as tiny hillocks and rectangular shapes. Intermolecular interactions were analysed by using Hirshfeld surface analysis. In the photoluminescence (PL) studies, the grown crystal indicates green emission peaks at 519 nm, and the bandgap energy is found to be 4.8 eV. At room temperature, the refractive index of the RbHOH crystal was determined to be 1.669. The nonlinear optical (NLO) efficiency of the grown crystal was examined using a second harmonic generation efficiency test, and it was determined to be 0.58 times that of KDP.

Synthesis, structure, growth, characterization and quantum chemical studies on 2-amino-5-bromopyridinium trichloroacetate: A novel phasematchable organic NLO single crystal

Organic crystals have become excellent candidates towards nonlinear optical (NLO) applications as they possess superior second and third order optical nonlinearities and high electro-optic coefficients when compared with their inorganic counterparts. In this direction, 2-Amino-5-bromopyridinium trichloroacetate (2A5BPT), a new organic second-order nonlinear optical compound is synthesized and optical grade single crystals are formed utilizing a slow evaporation solution growth approach at room temperature while using methanol as the solvent. Single crystal X-ray diffraction study shows that the title compound is assigned to monoclinic crystal system having non-centrosymmetric space group Cc. The crystal is transparent ( ̴ 85%) throughout the whole visible spectrum, according to the Ultraviolet-Visble (UV–Vis) spectra, with a cutoff wavelength of 367 nm and an optical energy band gap Eg of 3.32 eV. The crystal possesses good thermal stability. The compound has a 1.6 times greater powder second harmonic generation (SHG) efficiency than potassium dihydrogen phosphate (KDP). The phase matchability of the 2A5BPT is studied through particle size dependence of SHG. The intermolecular connection demonstrated by numerous inter contacts has been shown by a molecular Hirshfeld surface analysis of the crystal structure, and the related 2-dimensional finger print analysis further evaluates the individual contribution from each atom. In order to examine the first order hyperpolarizability, molecular electrostatic potential, and Highest occupied molecular orbital-Lowest unoccupied molecular orbital (HOMO-LUMO) energies, the quantum chemical calculations for the title molecule (2A5BPT) were carried out by density functional theory (DFT) utilizing the B3LYP/6–311++G(d,p) basis set. According to these results, the 2A5BPT crystal could be suitable for optoelectronic applications.

Investigation of nonlinear optical properties in α-A2BB'O6 (A = Li, Na, K; B = Ti, Zr, Hf; B' = Se, Te) by first-principles calculations.

Nonlinear optical (NLO) crystals based on oxides typically have wide bandgaps and large laser damage thresholds (LDTs), which are important for generating high-power and continuous terahertz radiation. Recently, a new family of NLO materials α-A2BB'O6 including Li2TiTeO6 (LTTO) with a strong second harmonic generation (SHG) efficiency of 26 × KH2PO4 (KDP) and a large LDT of 550 MW cm-2 were reported. Herein, we systematically study the electronic structures and NLO properties of α-A2BB'O6 (A = Li, Na, K; B = Ti, Zr, Hf; B' = Se, Te) to explore the relationship between the structure and SHG coefficient. First, 15 members of the A2BB'O6 family are demonstrated to be highly stable and NLO materials, excluding K2TiTeO6, K2TiSeO6 and K2ZrSeO6. Then, the electronic band structure, dipole moment and distortion of BO6/B'O6 octahedrons, SHG coefficient and terahertz absorption spectrum are calculated comprehensively with the element variation of A-site, B-site and B'-site. Finally, the magnitude of the SHG coefficient is found to be directly proportional to the value of total dipole moment and distortion, and inversely proportional to the bandgap value. Most importantly, among the A2BB'O6 materials, K2HfSeO6 shows the smallest direct bandgap of 2.99 eV, the largest SHG coefficient d33 of about 5 × LTTO and low terahertz absorbance from 0.1 to 9 THz. Our results provide new NLO crystals that may have potential application in terahertz radiation sources and other nonlinear electronics.

Halide-Driven Polarity Tuning and Optimized SHG-Bandgap Balance in (C4H11N2)ZnX3 (X = Cl, Br, I)

In the quest for organic-inorganic metal halides (OIMHs) that harmoniously combine large second harmonic generation (SHG) efficiency with broad bandgaps, our study introduces a series of noncentrosymmetric and polar piperazine...