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FTIR, FT-Raman and NMR are studied to explore the functional groups, the vibration modes and its coupling interactions for the grown single crystal piperazine-1,4-diium bis (4-aminobenzenesulfonate) (PABS). The cut-off wavelength at 303 nm of UV–Visible spectrum exhibits great transmittance over the entire visible spectrum. Photoluminescence spectral study revealed the electron excitation notably in blue emission range. The range of susceptibility and nonlinear refractive index was obtained from second and third harmonic generations of PABS crystals. At various temperatures, the thermal stability of the crystal and the crystal dielectric characteristics had been studied in relation to frequency. The hardness of the crystal was obtained by microhardness measurements. [ABSTRACT FROM AUTHOR]

Synthesis, crystallization, and in silico docking studies and third-order nonlinear optical (NLO) properties of (E)-1-(thiophen-2-yl)-3-(p-tolyl)prop-2-en-1-one (TPT) are outlined in the article. The molecular structure of TPT was established by a single-crystal X-ray diffraction study. The intermolecular interactions in the solid state were analyzed through Hirshfeld surface analysis (HSA). The third-order nonlinear optical properties were explored using open- and closed-aperture Z-scan techniques. The nonlinear co-efficient η2, third-order nonlinear susceptibility χ, and nonlinear absorption co-efficient β for the crystals are found to be 3.76E−10 cm2/W, 4.60E−08 esu, and 2.92E−06 cm/W, respectively. Density functional theory (DFT) calculations were used to optimize the molecular structure and band gap. Frontier orbital calculations showed a band gap of 4.18 eV for TPT and its value is in excellent agreement with the experimental value of 4.12 eV which is calculated by Tauc's plot. To study the substance's effectiveness as an anti-COVID target, in silico docking studies were performed with suitable receptors, and TPT is found to be a promising bioactive drug. [ABSTRACT FROM AUTHOR]

A single crystal of L-Alanine hydrogen ortho borate measuring 7 × 13 × 20 mm3 was successfully grown using slow solvent evaporation method at room temperature. Structural characterization of the grown crystal was determined by single crystal X-ray diffraction. The chemical composition of the grown crystal was identified by EDAX analysis. The functional groups were identified using FTIR spectroscopy. UV–Vis–NIR spectral studies were carried out to analyze the optical absorption, revealing low absorption in the wavelength region 212–1000 nm. The crystal exhibited excellent transparency throughout the visible region, with an optical band gap of 5.8 eV. The grown crystal of L Alanine hydrogen ortho borate crystal displayed good second-order nonlinear optical susceptibilities, indicating the non-centrosymmetric nature of the crystal. Z-scan analysis revealed saturation absorption. Various parameters such as nonlinear refractive index, absorption coefficient and non-linear optical susceptibility were calculated, demonstrating excellent third order susceptibilities. The thermal behavior of the grown crystal was analyzed by TG/DSC that shows the grown crystal was thermally stable up to 255 °C. The laser damage threshold value of L-Alanine hydrogen ortho borate was found to be 42 mV for 1.2 mJ/pulse. These crystals exhibit exceptional nonlinear optical characteristics, making them ideal candidates towards advanced optical applications in mere future. [ABSTRACT FROM AUTHOR]

Nonlinear optical crystals are the core devices of all-solid-state lasers, and have extensive and important applications in information technology and national security. With the development of high-performance computing, the "top-down" computer-aided design methods have gradually become an important part of nonlinear optical materials design. In addition, the large-scale structural and properties information obtained based on high-throughput computing provides a solid data foundation for data mining and machine learning algorithm training, accelerating the development of the fourth paradigm of material design. This paper starts with the computational design of nonlinear optical materials, and then, discusses the new paradigm of data-driven nonlinear optical materials theoretical design. Finally, the recent research progress of our team in high-throughput screening, crystal structure prediction, and machine learning accelerated nonlinear optical materials are reviewed. [ABSTRACT FROM AUTHOR]

The negative environmental impact of fossil fuel and the ever-increasing need for renewable energy materials necessitate a rigorous search for optoelectronic materials. Photon reabsorption due to a small Stokes shift limits the light-emitting potentials of many optical materials. In this research, two benzimidazole Schiff bases, 3-(((1H-benzo[d]imidazol-2-yl)imino)methyl)phenol (1) and N-(1H-benzo[d]imidazole(-2-yl)-1-(3-nitrophenyl))methanimine (2), were synthesized via one-pot single-step condensation and characterized using spectrometric (1H NMR, 13C NMR, HRMS and FTIR) techniques. The optoelectronic, nonlinear optical (NLO), adsorption properties and natural bond orbital (NBO) analysis of 1 and 2 were explored using spectroscopic, density functional theory (DFT) and Monte Carlo (MC) simulation approaches. The absorption, light-harvesting efficiency (LHE) and fluorescence properties were studied in solution. Static and dynamic first and second hyperpolarizabilities and parameters for power conversion efficiency (Voc and ΔGinj) were computed using the time-dependent DFT/B3LYP/6–311++G(d,p) method. Hyperpolarizabilities were compared with those of urea (standard). The binding properties of 1 and 2 on TiO2 (anatase 101) were investigated using the MC method. The calculated electronic properties agree with the experimental results. The compounds display large Stokes shifts (> 200 nm), appreciable quantum yields and low band gaps. High LHE (87%) and large hyperpolarizabilities were obtained for 2. Dye 2 displayed a high Voc, while 1 exhibited a more negative ΔGinj. The negative adsorption energies of the 1-TiO2 (− 52.9 kJ/mol) and 2-TiO2 (– 57.1 kJ/mol) interfaces indicate their strong binding interactions with anatase. NBO analysis revealed that conjugation and hyperconjugation were the primary interactions responsible for the stabilization of the dyes. These dyes have the potential for use in optoelectronic and nonlinear optical applications. [ABSTRACT FROM AUTHOR]

The preparation of high-performance electro-optical materials is one of the key factors determining the application of optoelectronic communication technology such as 5G communication, radar detection, terahertz, and electro-optic modulators. Organic electro-optic materials have the advantage of a high electro-optic coefficient (~1000 pm/V) and could allow the utilization of photonic devices for the chip-scale integration of electronics and photonics, as compared to inorganic electrooptic materials. However, the application of organic nonlinear optical materials to commercial electro-optic modulators and other fields is also facing technical bottlenecks. Obtaining an organic electro-optic chromophore with a large electro-optic coefficient (r33 value), thermal stability, and longterm stability is still a difficulty in the industry. This brief review summarizes recent great progress and the strategies to obtain high-performance OEO materials with a high electro-optic coefficient and/or strong long-term stability. The configuration of D-π-A structure, the types of materials, and the effects of molecular engineering on the electro-optical coefficient and glass transition temperature of chromophores were summarized in detail. The difficulties and future development trends in the practical application of organic electro-optic materials was also discussed. [ABSTRACT FROM AUTHOR]

The semi-organic nonlinear optical single crystal Bis (L-Tyrosinato) Cupric acetate (BLTC) was synthesized through a slow evaporation process in atmospheric conditions. A single crystal X-ray diffraction analysis of the formed crystal revealed that it is an orthorhombic crystal system with the space group P212121. Additionally, the powder X-ray diffraction patterns and diffracting planes of the BLTC crystal were recorded and identified. Fourier Transform Infrared (FTIR) spectroscopy analysis was used to characterize the formed crystals in order to identify the various vibrational modes caused by the different functional groups present in BLTC. The 1H and 13C NMR spectra were used to examine the crystal's hydrogen and carbon environments. The UV-visible, near-infrared, and photoluminescence (PL) analyses have been used to do optical studies. According to our findings, the material has a decreased cut-off wavelength and a high transparency window, making it suitable for nonlinear optical (NLO) and optoelectronic applications. The BLTC crystal's predicted band gap was found to be 4.1 eV. Thermo gravimetric (TG) and differential thermal analysis (DTA) techniques were used to determine the thermal properties of BLTC. With three different frequencies, the dielectric measurement of the crystal was observed with respect to temperature. An analysis has been done on the harvested crystals mechanical characteristics. In the developed BLTC crystal, morphological changes on the surface are seen. The material's second harmonic generation (SHG) was tested using the Kurtz and Perry powder method, and it was found to be higher than the KDP. [ABSTRACT FROM AUTHOR]

An improved design is described for ferroelectric crystals and implemented with the "methoxyphenyl series" of acetophenone azines, (MeO−Ph, Y)‐azines with Y=F (1), Cl (2), Br (3), or I (4). The crystal structures of these azines exhibit polar stacking of parallel beloamphiphile monolayers (PBAMs). Azines 1, 3, and 4 form true racemates whereas chloroazine 2 crystallizes as a kryptoracemate. Azines 1–4 are helical because of the N−N bond conformation. In true racemates the molecules of opposite helicity (M and P) are enantiomers A(M) and A*(P) while in kryptoracemates they are diastereomers A(M) and B*(P). The stacking mode of PBAMs is influenced by halogen bonding, with 2–4 showcasing a kink due to directional interlayer halogen bonding, whereas fluoroazine 1 demonstrates ideal polar stacking by avoiding it. Notably, (MeO−Ph, Y)‐azines display a stronger bias for dipole parallel alignment, attributed to the linearity of the biphenyl moiety as compared to the phenoxy series of (PhO, Y)‐azines with their non‐linear Ph−O−Ph moiety. The crystals of 1–4 all feature planar biphenyls and this synthon facilitates their crystallization through potent triple T‐contacts and enhances their nonlinear optical (NLO) performance by increasing conjugation length and affecting favorable chromophore conformations in the solids. [ABSTRACT FROM AUTHOR]

Phase matching is indispensable for high efficiency of second‐order nonlinear optical (NLO) crystals. Thousands of these crystals rely on birefringence phase matching, whereas only a few of them are quasi‐phase matching without the restriction of birefringence. Herein, using oriented seeds inch‐sized LiNH4SO4 (LAS) single crystals are successfully grown. LAS is NLO‐active with a very short deep‐UV absorption edge of 171 nm and high laser damage threshold up to 1.47 GW cm−2 at 1064 nm, 10 ns, but its birefringence is merely 0.0078@532 nm, which is too small to realize birefringence phase matching in deep‐UV region. Fortunately, P−E hysteresis loop, variable‐temperature NLO tests, and ferroelectric domain observations confirm that LAS is ferroelectric. Furthermore, LAS exhibits small refractive index dispersion resulting in a relatively long periodic length of 1.4 µm and its single domain structure can be easily obtained by electrical poling. These attributes make LAS a scarce NLO candidate for deep‐UV quasi‐phase matching. This work highlights the longly overlooked potential of sulfates and provides new opportunities for deep‐UV NLO materials. [ABSTRACT FROM AUTHOR]

A novel crystal benzophenone's nonlinear optical applications are pivotal. Benzophenone is one of the promising organic nonlinear optics materials for their high energy laser photonic application. It has already been possible to generate crystals of benzophenone in various ways. In this research, the slow evaporation method at room temperature was successful in making a single crystal of benzophenone. In this paper, synthesis, growth, characterization and applications of low melting organic nonlinear optics benzophenone crystal in order to improve their structural and physical properties are reported. Different characterization methods were applied to the grown crystals. The lattice parameters of the grown material were obtained by single crystal X-ray diffraction (XRD) study. The results of the single crystal XRD analysis showed that the produced crystals are a component of an orthorhombic system with the space group P212121 and the lattice parameters are a = 7. 9 9 9 5 (9)  Å, b = 1 0. 2 8 6 5 (1 0)  Å, c = 1 2. 1 2 4 7 (1 3)  Å, α = β = γ = 9 0 ∘ and V = 9 9 7. 7 0 (1 8)  Å3. Ultraviolet-visible (UV–Vis) spectrum indicates that the crystal is transparent (72%) in the entire visible region with a cutoff wavelength of 258 nm. The transparency of the grown crystals has been confirmed using the UV–Vis spectrum. The second harmonic generation (SHG) efficiency of the grown crystal was measured using an Nd-YAG laser and it was found to be 1.8 greater than potassium dihydrogen orthophosphate (KDP). The FT-IR spectrum was examined in order to identify the many functional groups. The formation of the material was confirmed qualitatively by FT Raman spectral analyses. Mechanical properties such as Vicker's microhardness number, Yield strength, Fracture toughness, Brittleness index and Elastic stiffness constant values were determined using Vicker's microhardness test. The thermal stability of the grown crystal was studied by thermal analysis. [ABSTRACT FROM AUTHOR]

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.

4-Methylbenzylammonium hydrogen maleate (4MBAHM), a novel organic nonlinear optical single (NLO) crystal has been developed by solvent evaporation method at ambient temperature. The structure of the 4MBAHM crystal has been solved and it reveals monoclinic system and space group P21/c. FT-IR and FT-Raman analyses are carried out to ascertain the functional groups present in the crystal structure. Optical properties are determined by UV–Vis-NIR analysis. 4MBAHM crystal is transparent from 262 to 1100 nm. Proton and carbon environment have been identified using NMR spectroscopy. The NMR spectroscopy reveals the formation of N–H...O, O–H...O and C–H...O bonds between 4-methylbenzylammonium (C8H12N)+ cation and hydrogen maleate (C4H3O4)− anion. The nonlinear optical parameters have been determined using Z-scan study. The third order NLO susceptibility (χ3) value is found to be 2.8975 × 10−5 esu. The closed aperture curve reveal 4MBAHM possess self-defocusing nature and the open aperture curve reveals reverse saturable absorption which find application in the field of night vision devices and optical limiting. [ABSTRACT FROM AUTHOR]

NaSrBS3, the first noncentrosymmetric alkali and alkaline earth metal mixed thioborate with the isolated [BS3] as the building units, has been synthesized successfully under the guidance of theoretical prediction. Comprehensive characterizations reveal that NaSrBS3 exhibits wide bandgap (3.94 eV), large birefringence (0.185 at 1064 nm), a high laser‐induced damage threshold (9 × AGS), and a suitable phase‐matching second‐harmonic generation (SHG) response (0.3 × AGS). Structure‐properties analyses illustrate that the [BS3] units determine the bandgap and contribute the most to the birefringence and SHG response. This work is the first successful case of "prediction to synthesis" involving infrared (IR) nonlinear optical (NLO) crystals in the thioborate system and provides an avenue to SHG materials design. [ABSTRACT FROM AUTHOR]

NaSrBS3, the first noncentrosymmetric alkali and alkaline earth metal mixed thioborate with the isolated [BS3] as the building units, has been synthesized successfully under the guidance of theoretical prediction. Comprehensive characterizations reveal that NaSrBS3 exhibits wide bandgap (3.94 eV), large birefringence (0.185 at 1064 nm), a high laser‐induced damage threshold (9 × AGS), and a suitable phase‐matching second‐harmonic generation (SHG) response (0.3 × AGS). Structure‐properties analyses illustrate that the [BS3] units determine the bandgap and contribute the most to the birefringence and SHG response. This work is the first successful case of "prediction to synthesis" involving infrared (IR) nonlinear optical (NLO) crystals in the thioborate system and provides an avenue to SHG materials design. [ABSTRACT FROM AUTHOR]

A semi-organic nonlinear optical crystal of L-alanine nickel chloride (LAN) has been successfully grown by a slow evaporation solution method. The single-crystal x-ray diffraction technique determined the lattice parameters of the crystal. Fourier-transform infrared spectral analysis confirmed the functional groups present in the crystal lattice. The crystal was subjected to UV–Visible-NIR transmittance measurements, and its band-gap energy was determined using transmittance studies. A Nyquist plot was used to determine the crystal's bulk resistance and dc conductivity. Fluorescence analysis was performed on the crystal, and green visible light was emitted from it when it was excited by UV light. Microhardness measurements were made on the crystal, and numerous parameters were analyzed. We studied the crystal's nonlinear optical properties, while its magnetic properties were determined using a vibrating sample magnetometer. TGA/DTA analysis was performed on the crystal, and it was found that its Second-harmonic Generation efficiency was more than that of the standard KDP sample. Hence, this crystal could be useful in laser technology, optical communication, optical computing, optical data processing, and photonics. [ABSTRACT FROM AUTHOR]

Traditional infrared (IR) nonlinear optical (NLO) materials such as AgGaS2 are crucial to key devices for solid‐state lasers, however, low laser damage thresholds intrinsically hinder their practical application. Here, a robust strategy is proposed for unbiased high‐throughput screening of more than 140 000 materials to explore novel IR NLO materials with high thermal conductivity and wide band gap which are crucial to intrinsic laser damage threshold. Via our strategy, 106 compounds with desired band gaps, NLO coefficients and thermal conductivity are screened out, including 8 nitrides, 68 chalcogenides, in which Sr2SnS4 is synthesized to verify the reliability of our process. Remarkably, thermal conductivity of nitrides is much higher than that of chalcogenides, e.g. 5×AgGaS2 (5.13 W/m K) for ZrZnN2, indicating that nitrides could be a long‐neglected system for IR NLO materials. This strategy provides a powerful tool for searching NLO compounds with high thermal conductivity. [ABSTRACT FROM AUTHOR]

The synthesis of (E)-isobutyl2-(2-(4-chlorophenyl)hydrazono)-3-oxobutanoate derivatives has been achieved by condensation of 4-chloroaniline and isobutyl 3-oxobutanoate using benzene diazonium chloride. Physicochemical and spectroscopic methods such as IR, 1H-NMR, 13C-NMR, and melting point measurements were used for the examination of the synthesized compound. Density functional theory was used along with the basic set of B3LYP/6-311 G (d, p) for optimizing the geometrical structure. The stability of the molecule as well as charge delocalization was examined using natural bond orbital analysis. The frontier molecular orbital energies give a description of the transfer of charge that occurs within the molecule. Analysis has been done on molecular electrostatic potential. Since the reported molecule has a high hyperpolarizability value, it is considered a potential nonlinear optical material. To conduct studies on drug similarity and oral activity, Lipinski's rule of five was used. The binding energy of the drug to several Covid receptors is examined using molecular docking experiments and it is determined that this compound is a superior antiviral agent. [ABSTRACT FROM AUTHOR]

Nonlinear optical phenomena enable novel photonic and optoelectronic applications. Especially, metallic nanoparticles and thin films with nonlinear optical properties offer the potential for micro-optical system integration. For this purpose, new nonlinear materials need to be continuously identified, investigated, and utilized for nonlinear optical applications. While noble-metal nanoparticles, nanostructures, and thin films of silver and gold have been widely studied, iridium (Ir) nanoparticles and ultrathin films have not been investigated for nonlinear optical applications yet. Here, we present a combined theoretical and experimental study on the linear and nonlinear optical properties of iridium nanoparticles deposited via atomic layer deposition (ALD). Linear optical constants, such as the effective refractive index and extinction coefficient, were evaluated at different growth stages of nanoparticle formation. Both linear and nonlinear optical properties of these Ir ALD coatings were calculated theoretically using the Maxwell Garnett theory. The third-order susceptibility of iridium nanoparticle samples was experimentally investigated using the z-scan technique. According to the experiment, for an Ir ALD coating with 45 cycles resulting in iridium nanoparticles, the experimentally determined nonlinear third-order susceptibility is about χIr(3) = (2.4 − i2.1) × 10−17 m2/V2 at the fundamental wavelength of 700 nm. The theory fitted to the experimental results predicts a 5 × 106-fold increase around 230 nm. This strong increase is due to the proximity to the Mie resonance of iridium nanoparticles. [ABSTRACT FROM AUTHOR]

Organic NLO materials, 2-methoxy-N,N-diphenylbenzamide (2MNNDPB), 4-Methoxy-N,N-diphenylbenzamide (4MNNDPB) and 3-methoxy-N,N-diphenylbenzamide (3MNNDPB), were synthesized by benzoylation of N,N-diphenylamine with methoxy substituted benzoyl chlorides. The single crystals of 2MNNDPB (3a), 3MNNDPB (3b) and 4MNNDPB (3c) were grown by a slow evaporation method in a dimethyl sulfoxide solvent. The X-ray diffraction shows that 2MNNDPB, 3MNNDPB and 4MNNDPB crystals belong to triclinic, orthorhombic and monoclinic crystallographic systems with space groups Pbca, P-1 and P21/n, respectively. FTIR spectra revealed the various functional groups and the chemical bonding, with the amide carbonyl peak appearing at 1658, 1649 and 1656 cm−1 in 2MNNDPB, 3MNNDPB and 4MNNDPB, respectively, and also confirmed by NMR spectra (1H and 13C) the number of protons and carbons present in the synthesized materials. UV–Vis spectra show 67%, 59% and 72% transmission in the visible region of the 2MNNDPB, 3MNNDPB and 4MNNDPB crystals. TGA/DTA analysis revealed that the 2MNNDPB, 3MNNDPB and 4MNNDPB crystals were thermally stable up to 354 K, 402 K, and 418 K, respectively. The second harmonic generation (SHG) of 2MNNDPB (3a), 3MNNDPB (3b) and 4MNNDPB (3c) crystals was determined by Kurtz–Perry powder method and found that 2.3, 2.7 and 2.2 times higher than that of KDP crystal. [ABSTRACT FROM AUTHOR]

Nonlinear optical (NLO) crystal, which simultaneously exhibits strong second‐harmonic‐generation (SHG) response and desired optical anisotropy, is a core optical material accessible to the modern optoelectronics. Accompanied by strong SHG effect in a NLO crystal, a contradictory problem of overlarge birefringence is ignored, leading to low frequency doubling efficiency and poor beam quality. Herein, a series of rare earth cyanurates RE5(C3N3O3)(OH)12 (RE=Y, Yb, Lu) were successfully characterized by 3D electron diffraction technique. Based on a "three birds with one stone" strategy, they enable the simultaneous fulfillment of strong SHG responses (2.5–4.2× KH2PO4), short UV cutoff (ca. 220 nm) and applicable birefringence (ca. 0.15 at 800 nm) by the introduction of rare earth coordination control of π‐conjugated (C3N3O3)3− anions. These findings provide high‐performance short‐wavelength NLO materials and highlight the exploration of cyanurates as a new research area. [ABSTRACT FROM AUTHOR]

A quaternary metal chalcogenide, namely K2CdGe3S8 (I), is obtained through a high-temperature solid-state approach. Compound I crystallizes with the non-centrosymmetric space group P212121. It features a 2D layer structure with [CdGe3S8] layers consisting of tetrahedral GeS4 and CdS4 units, and counter K+ embedded between the layers. The compound exhibits a powder second-harmonic generation (SHG) response of ~0.1 times that of KH2PO4 (KDP) with phase-matchable character at the laser wavelength of 1064 nm. Remarkably, it has a wide band gap (3.20 eV), which corresponds to a favorable high laser-induced damage threshold of 6.7 times that of AgGaS2. In addition, the calculated birefringence (Δn) is 0.039 at the wavelength of 1064 nm, which satisfies the Δn criteria for a promising infrared NLO material. [ABSTRACT FROM AUTHOR]

This study aims to explore the optoelectronic properties of a pyrene derivative 1,3-dinitropyrene using density functional theory to determine molecular electrostatic potential and Van der Waals surface, frontier molecular orbitals, and molecular orbital surfaces. The Mulliken charges, molecular electrostatic potential, and Van der Waals surface are accounted to show the availability of the electron donor-acceptor moieties, resulting in the charge transfer within the molecule. Theoretical electronic spectra are computed using Time-dependent density functional theory that shows the charge transfer process between nitro groups and C–H bonds of benzene rings. Vibrational features and chemical shifts are evaluated using Raman spectra and nuclear magnetic resonance shifts. The computed first-order hyperpolarizability of 1,3-dinitropyrene is 26 times higher than that of Urea showing its immensely high non-linear optically active responses. The smaller reorganization energy for hole transportation of the 1,3-dinitropyrene validates its application as a hole transport layer in organic light-emitting diodes. [ABSTRACT FROM AUTHOR]

The trigonal planar unit possesses significant hyperpolarizability and polarizability anisotropy, which makes it useful for optimizing nonlinear optical (NLO) materials, however, chalcogenide with this unit has seldom been reported. In this work, a novel approach is introduced by integrating the unprecedented trigonal planar MS 3 (M = Cd/In, Hg/In) motifs into the nearly optically isotropic tetrahedral units, resulting in two novel chalcogenides CsM 2 In 2 S 6 (M = Cd/In, 1; Hg/In, 2). Notably, structures 1 and 2 feature nearly planar triangular units at the center, encircled by three trimers, further interconnecting each other to create 3D frameworks. Importantly, phases 1 and 2 display phase-matching (PM) capabilities, primarily attributed to incorporating trigonal planar MS 3 units that additionally enhance polarizability anisotropy. Furthermore, compounds 1 and 2 demonstrate moderate second-harmonic generation (SHG) signals (0.70 and 0.84 × AgGaS2@1.7 µm). This study pioneers an efficient strategy for the design of infrared NLO crystals with PM capabilities., (© 2024 Wiley‐VCH GmbH.)

The slow evaporation technique was used to successfully grown amino acid doped sodium acid phthalate (NaAP) crystals at room temperature. A great deal of research has been done on the effects of amino acids on NaAP growth and characteristics. X-ray diffraction was used to examine the crystal structure and lattice parameters of the grown crystals. Functional groups were found in the title crystals, which revealed themselves utilizing FTIR spectra. The optical transparency of the doped crystals was noticed by measurements of optical absorption. In order to assess the mechanical strength of the produced crystals, Vickers microhardness tests were employed. The technique of Kurtz powder was utilized to calculate the second harmonic generation (SHG) performance of the cultivated crystals.

A new design for a tunable multi-channel plasmonic bandpass filter was numerically investigated using the two-dimensional finite element method (2D-FEM). The proposed multi-channel plasmonic bandpass filter consists of a metal-insulator-metal waveguide (MIM-WG) and double-sided arrow-shaped cavities. Silver (Ag) and a non-linear optical medium (InGaAsP) are used in the designed filter. InGaAsP fills the bus waveguide and arrow-shaped cavities. The refractive index of InGaAsP is sensitive to the incident light intensity, therefore the resonance wavelengths can be controlled. Utilizing different incident light intensities (such as 1017 v2/m2 and 2 × 1017 v2/m2) on the InGaAsP, the filter wavelengths can be tuned over a range from 600 nm to 1200 nm. The proposed filter with a confinement area of 0.5 μm2 can be used in wavelength division multiplexing (WDM), photonic systems, coloring filters, sensing, and 5G+ communication. [ABSTRACT FROM AUTHOR]

Design and exploratory synthesis of new mid‐infrared (mid‐IR) nonlinear optical (NLO) materials are urgently needed for modern laser science and technology because the widely used IR NLO crystals still suffer from their inextricable drawbacks. Herein, a multi‐level data‐driven approach to realize fast and efficient structure prediction for the exploration of promising mid‐IR NLO materials is proposed. Techniques based on machine learning, crystal structure prediction, high‐throughput calculation and screening, database building, and experimental verification are tightly combined for creating pathways from chemical compositions, crystal structures to rational synthesis. Through this data‐driven approach, not only are all known structures successfully predicted but also five thermodynamically stable and 50 metastable new selenides in AIBIIISe2 systems (AI = Li, Na, K, Rb, and Cs; BIII = Al and Ga) are found, among which eight outstanding compounds with wide bandgaps (> 2.70 eV) and large SHG responses (>10 pm V−1) are suggested. Moreover, the predicted compounds I4¯2d‐LiGaSe2 and I4/mcm‐KAlSe2 are successfully obtained experimentally. In particular, LiGaSe2 exhibits a robust SHG response (≈2 × AGS) and long IR absorption edge that can cover two atmospheric windows (3–5, 8–12 µm). Simultaneously, this new research paradigm is also applicative for discovering new materials in other fields. [ABSTRACT FROM AUTHOR]

Noncentrosymmetric hybrid framework (HF) materials are an important system in discovering new practical second-order nonlinear optical materials. We calculated the second harmonic generation (SHG) response of a noncentrosymmetric (NCS) organic–inorganic HF compound, CuMoO3(p2c) (p2c = pyrazine-2-carboxylate) to find that it exhibits the largest SHG response among all known NCS HF materials with one-dimensional helical chains. Further atom response theory analysis revealed that the metal atoms Cu and Mo contribute much more strongly than do nonmetal atoms in determining the strength of the SHG response, which is a novel example in nonlinear optical materials known to date. [ABSTRACT FROM AUTHOR]

In recent years, with the rapid development of ultrastrong and ultrafast lasers, it has become essential to develop new materials with excellent nonlinear optical (NLO) properties. Porphyrin-based metal-organic frameworks (MOFs) have great potential for application in the field of NLO due to their large conjugated structure and good stability. As a typical porphyrin-based MOF, porphyrin paddle-wheel framework-3 (PPF-3) has been prepared and applied in the fields of catalysis and sensing, yet the investigation of PPF-3 in NLO remains unexplored. In this study, the ZnS/PPF-3 composite was successfully prepared using a solvent thermal method to in situ load ZnS on the surface of PPF-3. Utilizing the Z-scan technique, the NLO properties of ZnS, PPF-3, and ZnS/PPF-3 composite were investigated under different input energy intensities. ZnS/PPF-3 composite material exhibits significantly enhanced NLO properties, with the third-order nonlinear absorption coefficient (β eff ) of up to 7.00 × 10 -10 m/W and a limiting threshold as low as 1.52 J/cm 2 , indicating its promising application potential value in the field of optical limiting. To enhance the practical utility, the ZnS/PPF-3/PVA film was prepared via the drop-casting method, achieving a maximum β eff of 5.00 × 10 -8 m/W. The smaller optical bandgap of ZnS/PPF-3 and electron transfer from PPF-3 to ZnS are the key factors that enable the ZnS/PPF-3 composite to a superior NLO performance.

Van der Waals (vdW) deep‐UV (DUV) nonlinear optical (NLO) crystal is an important material system recently developed. Herein, we review its concept and original intention, and then summarized the discovery process of related materials, including the role of A‐site cations and the resulting two‐/one‐dimensional vdW DUV NLO systems. Finally, we evaluate the practical DUV NLO performance and prospected the opportunities and challenges. [ABSTRACT FROM AUTHOR]

In this study, a new Schiff base, 3-(5-(4-hydroxybenzylideneamino)naphthalen-1-yliminomethyl)phenol, has been synthesized via one-pot two-step condensation of benzaldehyde derivatives with 1,5-diaminonaphthalene. The Schiff base was characterized using nuclear magnetic resonance (NMR), Fourier transform infrared (FTIR) spectrophotometry and mass spectrometry. Photophysical and optical properties of the imine system were investigated using Ultraviolet–Visible (UV–Vis) and fluorescence spectrophotometry, and computational calculation. Quantum chemical investigations of the excited state energies, energy gap (ΔE), light harvesting efficiency (LHE), polarizability (α), first hyperpolarizability (β) and second hyperpolarizability (γ) at time-dependent density functional theory (TD-)DFT/B3LYP/6–311 + + G(d,p) level were conducted in vacuum, cyclohexane and ethanol. The hyperpolarizabilities were compared with those of urea (standard nonlinear optical (NLO) material). The UV–Vis result shows a low-energy absorption edge and an appreciable fluorescence quantum yield (Φf = 0.45). Large Stokes shift (59 nm) and high LHE (85%) were obtained in cyclohexane. Calculated quantum chemical parameters were solvent-sensitive and suggested that the molecule is reactive and kinetically less stable. Low ΔE (3.25 eV) was observed which suggests semiconducting potential of the material. The first and second hyperpolarizabilities are about fifteen times and ninety times larger than those of urea, respectively, indicating its good potentials as NLO and photonic materials. [ABSTRACT FROM AUTHOR]

We report on synthesis, growth and characterization of an organic nonlinear optical (NLO) crystal 2‐{3‐[2‐(4‐dimethylaminophenylvinyl]‐5,5‐dimethylcyclohex‐2‐enylidene}‐malonitrile (DAT2). The functional groups are identified by 1H‐NMR. Large size single crystal of DAT2 of size 1.2 × 0.5 × 0.2 cm3 is grown for the first time using solution growth technique. The physicochemical properties of DAT2 crystal such as crystal structure, melting point, optical reflectance and photoluminescence are studied experimentally. Density functional theory (DFT) analysis is employed to study the band structure, optical and electronic properties of DAT2. The theoretical bandgap was compared with the experimental one. LDA approximation has been used to compare the GGA results. [ABSTRACT FROM AUTHOR]

A new design for a tunable multi-channel plasmonic bandpass filter was numerically investigated using the two-dimensional finite element method (2D-FEM). The proposed multi-channel plasmonic bandpass filter consists of a metal-insulator-metal waveguide (MIM-WG) and double-sided arrow-shaped cavities. Silver (Ag) and a non-linear optical medium (InGaAsP) are used in the designed filter. InGaAsP fills the bus waveguide and arrow-shaped cavities. The refractive index of InGaAsP is sensitive to the incident light intensity, therefore the resonance wavelengths can be controlled. Utilizing different incident light intensities (such as 1017 v2/m2 and 2 × 1017 v2/m2) on the InGaAsP, the filter wavelengths can be tuned over a range from 600 nm to 1200 nm. The proposed filter with a confinement area of 0.5 μm2 can be used in wavelength division multiplexing (WDM), photonic systems, coloring filters, sensing, and 5G+ communication.

The detailed study on the preparation and characterizations of N-Acetyl Glycine Hydrochloride was grown by the slow evaporation solution technique is highlighted in this article. The grown crystal was subjected to single crystal X-ray diffraction technique to determine the lattice parameters. FT-IR spectrum was analyzed to identify the presence of functional groups. UV–Vis-NIR studies were determined in the optical parameters like optical band gap, reflectance, and refractive index. Optical nonlinearities of AGC were determined by Z-scan technique with Nd:YAG laser radiation. The photo active nature of the material was established from fluorescence study. The impedance spectrum was used to determine the DC conductivity at first time. The predicted NLO properties, UV–Vis absorption, and Z-scan studies mention that the sample is an ideal material for nonlinear optics and photonics applications. [ABSTRACT FROM AUTHOR]

Ammonia (NH3) synthesis is a critical chemical process to develop nitrogen-containing commodities which remains a significant challenge in chemistry and industry. Photocatalysis reduction has been deemed as one of the most promising strategies for N2 fixation under mild conditions. Herein, a series of Pr doped LiNbO3 (Pr3+:LiNbO3) were synthesized by a facile sol–gel method. Results showed that the Pr3+:LiNbO3 upconverted visible light into ultraviolet light and had the highest up-conversion efficiency when the molar ratio of Pr3+ was 2.5 mol%. In addition, the oxygen vacancies generated by the incorporation of Pr3+ into the LiNbO3 crystal lattice acted as active sites boosting the adsorption and activation of N2. The NH4+ production rate reached the highest of 30.72 μmol/L, attributed to the synergistic effects combining spontaneous polarization of the nonlinear optical (NLO) material LiNbO3 and up-conversion luminescence of Pr3+, which not only broaden the adsorption range of solar light but also enhance the charge separation. The up-conversion NLO material Pr3+:LiNbO3 in this study provides a novel alternative for guiding the design of ammonia synthesis photocatalyst. [ABSTRACT FROM AUTHOR]

Defective crystalline semiconductor plays a significant role in photocatalytic nitrogen fixation, however the rapid recombination of photoexcited electron/hole pairs largely reduces the efficiency. Spontaneous polarization of the nonlinear optical (NLO) material has emerged as a promising strategy for addressing the problem. Herein, a defects-rich NLO crystalline LiNbO3 modulated by natural nano-mineral palygorskite (LiNbO3/Pal) has been synthesized via sol–gel method. The intrinsic polarization of LiNbO3/Pal is investigated by second harmonic generation (SHG) measurements, which indicates an intensity of about 3.1 times that of typical NLO material KH2PO4 (KDP). The strong polarization can facilitate the separation of photogenerated charge carriers in the bulk phase and on the surface of LiNbO3/Pal. The existence of oxygen vacancies in LiNbO3/Pal may originate from doping of metal ions and active groups on the surface of Pal during crystallization of LiNbO3, which shortens the bandgap of LiNbO3 and facilitates the absorption and activation of N2 molecules. As a result, the polarization effect and rich oxygen vacancies make the LiNbO3/Pal an exceptional photocatalyst for N2 fixation. The 40 wt% LiNbO3/Pal composite achieves an average rate of photocatalytic NH4+ production of 52.57 μmol gcat−1 h−1 under simulated solar light, which is about sixfold higher than that of bulk LiNbO3. This work not only presents a new perspective on mineral modification of NLO material but also offers a cost-effective photocatalyst for nitrogen fixation. [ABSTRACT FROM AUTHOR]

4-N,N-dimethylamino-4′-N′-methyl-stilbazolium tosylate (DAST) is one of the most important organic nonlinear optical (NLO) materials, but its controlled growth remains a challenge. Herein, we describe a novel method to control the growth of DAST on the surfaces of indium tin oxides coated with the patterned photoresists by electric field. Results indicate that zero-dimensional (0D) spherical DAST microcrystals tend to grow along the photoresist lines if an electric field with a low frequency of 500 Hz is applied. Rather differently, one-dimensional (1D) DAST microwires preferentially grow along the gaps of the photoresist lines under the control of an electric field with a high frequency of 1000 Hz. Growth of DAST microcrystals controlled by electric field leads to the increase in the crystallinity, but the chemical structures remain unchanged. Moreover, second harmonic generation signal was measured from the as-grown DAST microcrystals. The results presented in this work are helpful for rationally controlling the growth of 0D or 1D DAST microcrystals, and particularly, the strategy can be further expanded to control the growth of DAST derivatives or other organic NLO materials with similar chemical structures. [ABSTRACT FROM AUTHOR]

Urea glutaric acid (UGA), an organic crystal, was synthesized and grown using a low temperature solution technique. Single crystal XRD revealed a monoclinic structure with a C2/C space group. The various cell data were identified. The optical parameters were calculated from UV-visible spectrum. The transmittance spectra showed the cutoff wavelength as 240 nm (low) and the energy gap determined from the spectra was compared with the theoretical energy gap. The transition number revealed the electron transition, which corresponded to direct allowed transition. The diverse optical parameters like reflectance, extinction coefficient, refractive index and optical susceptibility were determined. The least value of Urbach energy caused less defects and a good crystalline nature. The steepness value and electron phonon interaction were calculated. The positions of lower and higher band energy levels were identified. Electronic polarizability was found using the Clausius–Mossoti relation and tabulated. The mechanical fitness was measured from Vickers hardness analysis. The nonlinear optical property was measured from Z-scan analysis. Thus, the optical results support the material suitability and fitness for optical and electronic domain applications.

l-Glutamic acid hydrobromide single crystals were grown by Sankaranarayanan–Ramasamy (SR) method for the first time. Seed crystals were prepared from the solvent evaporation technique. Using single-crystal X-ray diffraction (XRD) analysis, the crystal system and the cell parameters were determined. The TG/DTA analysis shows that the crystal is stable up to 200°C and further increase of temperature decomposition was observed. The crystal has a sharp cutoff around 230 nm and is transparent in the UV region. High-resolution XRD curve of 22 arc s FWHM shows the excellent crystallinity nature. Further, the Vicker's hardness test proved that the hardness of the crystal grown using SR method is found to be higher than the crystal grown with the conventional solution grown technique. Etching studies were performed to find the growth pattern and the results are presented and discussed in detail. [ABSTRACT FROM AUTHOR]

The current work is to spotlight the key structure-property features of a novel thiourea complex bis(thiourea) silver(I) nitrate (BTSN) for future applications in nonlinear optical devices through dual approach involving experimental and theoretical techniques. The synthesis and growth of good quality single crystals of a relatively new material BTSN have been done. The crystal structure, quantitative and qualitative, vibrational, optical and dielectric analysis of the grown single crystals was carried out. The optical transparency of the grown crystals is found to be more than 80% confirms its colorless nature and applications in optoelectronic devices. Further, the state-of-art computational methods have been applied to obtain the ground state molecular geometry at B3LYP/6-31G∗, MP2/6-31G∗ and M06/6-31G∗ levels of theory. Various key electro-optical properties (complementary to experimental results) such as IR, Raman, and polarizabilities have been determined at the same levels of theory. The static and dynamic polarizability and first hyperpolarizability both were calculated to comprehend the potential applications of BTSN in nonlinear optics. In addition to the above, numerous novel molecular level insights have been achieved in the form of total and partial density of states, HOMO-LUMO gap and molecular electrostatic potential map. The calculated values of static and frequency dependent dynamic first hyperpolarizability are found to be 8.46 × 10−30 and 2.30 × 10−30 esu which are about 23 times and 13 times greater than those of prototype urea molecule, respectively, calculated at the same B3LYP/6-31G∗ level of theory. From the analyzed results it is clear that the titled compound possesses excellent electro-optic properties that make it a decent contestant for photonic devices. [ABSTRACT FROM AUTHOR]