Harmonic Generation Applications Research Articles

Growth, elemental, spectral, linear, photoconductivity, dielectric, thermal, and Z-scan analysis of benzotriazolium oxalate dihydrate single crystal for third-order harmonic generation applications

Growth, elemental, spectral, linear, photoconductivity, dielectric, thermal, and Z-scan analysis of benzotriazolium oxalate dihydrate single crystal for third-order harmonic generation applications

Large third-order nonlinear susceptibility of newly synthesized 3-amino-1H-1,2,4-triazolium p-toluene sulfonate (TPTSA) single crystal measured by the open and closed aperture of the Z-scan technique

The researchers employed the Slow Evaporation Solution Technique (SEST) to grow a third-order nonlinear optical 3-amino-1H-1,2,4-triazolium p-toluene sulfonate (TPTSA) crystal and subsequently conducted an X-ray structural examination. The resulting solution's monoclinic structure (P21/c space group) was confirmed and refined using the SHELXS 2018/3 program, and this marks the first instance of a TPTSA single-crystal structure being reported. To further investigate the optical qualities of the TPTSA crystals, including reflectance (R), bandgap (Eg), refractive index (n), and extinction coefficient (K), we utilized a UV–Vis–NIR spectrophotometer, which demonstrated a transmittance of 82%. Moreover, photoluminescence spectrum analysis revealed that the crystal emits light at 294 and 471 nm. Thermal properties of the TPTSA single crystals were also studied, and it was determined that TPTSA remains stable up to 197 °C. A Hirshfeld surface study showed various inter and intra molecular interactions within the TPTSA compound. Based on the crystal's Z-scan parameters, such as absorption coefficient (β = 1.02412 × 10−4 m/W), nonlinear refractive index (n2 = 9.7348 × 10−12 m2/W), and third-order linear optical susceptibility (χ3) of TPTSA, which was found to be 3 × 10−8 esu, it is evident that the nonlinear properties of this crystal make it suitable for third harmonic generation applications. The comprehensive structural analysis and physical characteristics of the TPTSA crystal demonstrate its potential for applications in harmonic generation.

Single Crystal Growth of 4‐Aminobenzophenone (ABP) by Solution and Seeded Czochralski Pulling Techniques for Second Harmonic Generation Applications

AbstractHighly efficient 4‐aminobenzophenone (ABP) single crystals are grown from melt by employing the seeded Czochralski pulling technique for second harmonic generation (SHG) applications. The as‐grown seed crystals from solution with dominant (100) and (001) facets are utilized to trigger the directional solidification. For successive growth, initial measurements of the furnace temperature distribution, heat flow structure, and solidification temperature of ABP in correlation with differential scanning calorimetry (DSC) analysis are made. The controlled diffusion is ensured by monitoring the interfacial layer between the melt and the growing crystal and is maintained by optimizing the melt temperature and pulling and rotation rates. Color change of the melt due to thermal‐oxidation is prevented by appropriate control of the growth environment. A slow and steady growth rate affirms the good quality of the ABP single crystal. The anisotropic growth behavior of ABP from solution and melt is reported. Internal molecular structure, crystalline purity, molecular vibrational modes, optical transmission, and thermal behavior are studied using single crystal and powder X‐ray diffraction, FTIR, UV–vis–NIR and DSC analyses. The obtained higher SHG efficiency of the grown ABP in comparison with that of the organic and inorganic standards urea and KDP reveals its suitability for SHG applications.

Investigation of the structural, Hirshfeld surface, Z-scan, and molecular modelling of imidazolium fumarate for third harmonic generation applications

• IMFA was synthesized and characterized by various physicochemical studies. • FTIR analysis is done for both parent and product materials. • The first order hyperpolarizability value of IMFA is 2.68 × 10 −30 esu. • The grown crystal becomes transparent and the E g value is 4.15 eV. • The third order NLO properties have been calculated by using Z-scan studies. Single crystals of imidazolium fumarate (IMFA) have been grown and subjected to several experimental studies. Single crystal XRD studies affirm that the IMFA crystal system belongs to the triclinic with a centrosymmetric space group of P-1. The fundamental vibrational modes were affirmed by the FTIR studies. The FT-NMR spectrum was recorded to interpret the number of protons and carbons present in the grown crystal. The grown crystal has good transmission in the region of 400 to 1050 nm. The grown crystal 3 rd order NLO properties have been calculated by using Z-scan studies. The Hirshfeld surface and related fingerprint plots of the IMFA molecule have been analysed. The title molecule electrophilicity index and energy gap HOMO-LUMO were determined. Moreover, the DFT computation of the optimized geometries, NBO, MEP, and molecule hyperpolarizability calculations were also made to explore the structure-property relationship. Graphical Abstract. .

Synthesis, characterization and theoretical calculations of four chiral schiff base materials for second harmonic generation applications

In this work, chirality combining schiff base molecular character was used to design noncentrosymmetric materials with hyperpolarizability for second harmonic generation applications. Four chiral schiff base molecualers, two pairs of enantiomers, (1S,2S)(-)-diphenen(3,5-salicylaldehyde) (S,S-DS), (1R,2R)(+)-diphenen(3,5- salicylaldehyde) (R,R-DS), (1S,2S)(-)-diphenen(9-anthraceneca) (S,S-DA) and (1R,2R)(+)- diphenen(9- anthraceneca) (R,R-DA) have been successfully designed and synthesized. And four crystal materials, S,S-DS·acetonitrile (compound 1), R,R-DS (compound 2), S,S-DA (compound 3) and R,R-DA (compound 4), were successfully prepared. Compounds 1–4 crystallized in chiral space groups (noncentrosymmetric space groups). The characterization and theoretical calculations were carried out on these four crystal materials, such as the cut-off wavelength, the UV–Vis–NIR absorption, the thermogravimetric analysis, the second harmonic generation (SHG) efficiency of the powdered compounds, the frontier molecular orbital (HOMO and LUMO) energies and the static first molecular hyperpolarizabilities. All of these results imply that compounds 1–4 are desirable candidates for non-linear optical applications.

Optoelectronic, luminescence, and nonlinear properties of a non-centrosymmetric Cd(II)-based complex

Single crystals of 1,2-diammoniumcyclohexane tetrabromocadmate(II) monohydrate, abbreviated as CdDACH, have been obtained by the slow evaporation solution growth method using methanol as solvent. Single-crystal X-ray diffraction analysis has been utilized to compute the unit cell parameters of the CdDACH crystal. The molecular structure has been analyzed by FTIR, FT-Raman, and ATG/DSC measurements. The electronic behavior has been determined by DFT methods at the B3LYP/LANL2DZ level. The UV/Visible spectrum indicates a direct band gap (4.88 eV) and a low cut-off wavelength (250 nm) for the crystal. Photoluminescence measurement of CdDACH yielded a broad peak at 506 nm with a width at half-maximum of 94 nm. Electrical and optical parameters, namely refractive index (n), extinction coefficient (k), electrical conductivity (σe), and optical conductivity (σopt), have been derived by means of diffuse-reflectance spectroscopy. With a high optical conductivity of 1010 s−1, the suitability of the photo-response of the crystal for use in devices that perform information processing has been established. The first hyperpolarizability (β) and second hyperpolarizability (γ) of the material have been theoretically investigated through TD-DFT calculations. The third-order susceptibility χ(3) of CdDACH crystals, estimated by the Lorentz approximation, was found to be of the order of 10−4 esu. The obtained results indicate that CdDACH may be adopted for future second and third harmonic generation applications.

Enhanced two-photon photoluminescence assisted by multi-resonant characteristics of a gold nanocylinder

Abstract Multi-resonant plasmonic simple geometries like nanocylinders and nanorods are highly interesting for two-photon photoluminescence and second harmonic generation applications, due to their easy fabrication and reproducibility in comparison with complex multi-resonant systems like dimers or nanoclusters. We demonstrate experimentally that by using a simple gold nanocylinder we can achieve a double resonantly enhanced two-photon photoluminescence of quantum dots, by matching the excitation wavelength of the quantum dots with a dipolar plasmon mode, while the emission is coupled with a radiative quadrupolar mode. We establish a method to separate experimentally the enhancement factor at the excitation and at the emission wavelengths for this double resonant system. The sensitivity of the spectral positions of the dipolar and quadrupolar plasmon resonances to the ellipticity of the nanocylinders and its impact on the two-photon photoluminescence enhancement are discussed.

Screw-Dislocation-Driven Growth Mode in Two Dimensional GaSe on GaAs(001) Substrates Grown by Molecular Beam Epitaxy

Regardless of the dissimilarity in the crystal symmetry, the two-dimensional GaSe materials grown on GaAs(001) substrates by molecular beam epitaxy reveal a screw-dislocation-driven growth mechanism. The spiral-pyramidal structure of GaSe multi-layers was typically observed with the majority in ε-phase. Comprehensive investigations on temperature-dependent photoluminescence, Raman scattering, and X-ray diffraction indicated that the structure has been suffered an amount of strain, resulted from the screw-dislocation-driven growth mechanism as well as the stacking disorders between monolayer at the boundaries of the GaSe nanoflakes. In addition, Raman spectra under various wavelength laser excitations explored that the common ε-phase of 2D GaSe grown directly on GaAs can be transformed into the β-phase by introducing a Se-pretreatment period at the initial growth process. This work provides an understanding of molecular beam epitaxy growth of 2D materials on three-dimensional substrates and paves the way to realize future electronic and optoelectronic heterogeneous integrated technology as well as second harmonic generation applications.

Synthesis, Growth and Characterization of New Promising Organic Non-Linear Optical Crystal: L-Alanine Alaninium Nitrate

A relative study on pure L-alanine alaninium nitrate (LAAN) single crystals and doped with lanthanum oxide, urea and glycine were developed from fluid solution by slow evaporation strategy at room temperature. X-ray diffraction result reveals that LAAN crystallites with system with space bunch P21 and cell parameters a = 7.836 Å, b = 5.428 Å, c = 12.809 Å and β = 94.25°. These parameters were marginally changes for doped crystals compared to pure LAAN crystal. The UV results recommend that the great transmission property of the doped LAAN crystal within the whole visible region guarantees its reasonableness for second harmonic generation applications. The presence of dopants within the LAAN crystal was further affirmed through ICP studies. The functional groups were analyzed through Fourier change infrared spectra investigation. The microhardness and dielectric study at 100 Hz was found to be broadly higher than that of pristine LAAN. The AC conductivity was found to extend after doping due to the induced defects in crystal lattice. The grown crystals were also subjected to second harmonic generation efficiency tests and it was found to be La2O3 doped LAAN crystal is 2.8 times greater than that of potassium dihydrogen phosphate (KDP).

An investigation on optical, mechanical and thermal properties of nickel sulphate hexahydrate single crystal—a UV band pass filter

Nickel sulphate hexahydrate (NSH) crystal is known to be an excellent material for UV light band-pass filter applications. In this research work, good quality and enhanced size of NSH single crystal has been effectively grown by implementing Sankaranarayanan—Ramasamy (SR) method. After a prolonged period of 185 days, a fine quality of transparent as well as improved size single crystal of NSH with dimension 220 mm in length and 12 mm in diameter has been successfully harvested. The grown crystal has been subjected to various characterizations as that of single crystal x-ray analysis to confirm the crystal system with unit cell parameters, UV–Vis analysis to know the transmission spectrum, FTIR spectral analysis to find out the functional groups and photoluminescence study to affirm the green emission of the crystal. NSH crystal falls into the category of soft material as identified by microhardness study and etching study confirms that it has good quality as the surfaces are almost free of defects. Photoacoustic spectroscopy has been utilized to find the thermophysical parameters. The resultant value of thermal diffusivity is compared with few other familiar nonlinear optical materials such that it is asserted by the observed superior value of NSH single crystal that it is an added advantage for band-pass filter and harmonic generation applications.

Evaluation of structural, optical and mechanical behaviour of L-argininium bis(trifluoroacetate) single crystal: An efficient organic material for second harmonic generation applications

In the present technologically advanced era, non-linear optical materials especially organic derivatives are in the limelight due to their fast response in electro-optic switches and high nonlinear efficiency. Therefore, with respect to this behaviour, single crystals of L-argininium Bis(trifluoroacetate) (here in after called LABTF) an organic material was grown by slow evaporation solution growth technique. The grown single crystal was subjected to single crystal X-Ray diffractometer to validate its chemical structure and compound formation. The titled compound crystallizes into an asymmetric entity that comprises of one divalent L-argininium cation and two monovalent trifluoroacetic anion. All the intermolecular hydrogen bonds present in the LABTF crystal structure are investigated by 3D molecular Hirshfeld surface analysis and their relative involvements are disintegrated using 2D fingerprint plots. Further, the crystalline perfection assessment was performed using high-resolution X-Ray diffractometer which divulges the absence of structural grain boundaries in the obtained crystal. Thermal transport parameters of the titled compound were measured through Photoacoustic spectroscopy. The shock strength above which the crystal induces damage was found by the shock damage threshold technique. In addition, mechanical property related parameters such as hardness, stiffness and Young's Modulus were evaluated using the nanoindentation technique. These mechanical parameters resolve the reliability of devices and it can be enhanced by improving the crystal quality.

Strong coupling of metamaterial resonances to intersubband transitions of quantum dots for enhanced second-harmonic generation.

Recently, quantum confined structures have been widely studied for their nonlinear properties and applications in harmonic generation. However, because of lower orders of susceptibility, the generated harmonic power is low. In this paper, we present coupling of metamaterial resonance to intersubband transitions of quantum dots (QDs) for enhanced second-harmonic generation efficiency. To do so, first the QDs are designed so as to exhibit three electronic energy levels with identical energy spacing. The values of energy levels and the wave functions are calculated by solving the Schrödinger equation using modified effective mass approximation. The second-order nonlinear susceptibility of QD layers is then calculated, and the results are used in finite-difference time domain (FDTD) simulation of structure. Metamaterial structure is also designed to resonate in response to the frequency of QDs. The results show that for a pump input with 24THz fundamental frequency, a harmonic with the 48THz frequency appears in the output, with conversion efficiency of about 5×10-7.

Effect of L-Cysteine doping on growth and some characteristics of potassium dihydrogen phosphate single crystals

Among quite a number of technologically important NLO materials, Potassium Dihydrogen Phosphate (KDP) is one of the most favourable ones for second harmonic generation applications, such as in electro-optic modulators, parametric oscillators and harmonic generators. The authors report here their studies on KDP crystals doped with L-Cysteine (1mol% and 2mol%). The dopant inclusion in the crystals was confirmed using Fourier transform infrared (FT-IR) spectroscopy and Powder X-Ray Diffraction (XRD). The XRD results also confirm the tetragonal structure with lattice parameters a = b = 7.45Å and c = 6.98Å. The presence of functional groups of crystals was analyzed using the FTIR spectra. For band gap evaluation, UV–Vis spectra were used and it was found to be 3.41eV, 4.40eVand 4.50eV, respectively in the cases of pure KDP, 1mol% and 2mol% L-Cysteine dopings. The spectra quality indicates good transparency of the doped crystals in the visible region, a feature quite desirable for applications in optoelectronics.

Spin-coated nickel doped cadmium sulfide thin films for third harmonic generation applications

In the current study, different percentages of Nickel (0%, 2%, 4% and 6%) doped CdS thin films have been deposited on glass substrates by the sol-gel spin-coating technique. Before performing the nonlinear optical studies, the structural, morphological and optical properties were examined as a function of Ni doping concentration through the XRD, SEM, AFM and UV–vis spectrometry, respectively. According to the XRD patterns, all films are polycrystalline and the incorporation of Ni does not change qualitatively the crystalline phase of CdS. The Ni doping affects the surface morphology of the CdS thin films which is indicated by scanning electron microscopy and atomic force microscopy images. The band gap was determined via the equation related to the absorption coefficient. It's deduced that the optical band-gap values increased from 2.35 eV to 2.41 eV depending on Ni content. Though, the nonlinear optical properties were determined based on the measurements of the third harmonic generation (THG) using the rotational Maker fringe technique. The results showed that the third order nonlinear optical susceptibilities oscillate between 5.40 × 10−21 m2/V2 for CdS:Ni (2%) and 4.98 × 10−21 m2/V2 for CdS:Ni (6%) while the pure CdS one falls inward, with a value of 5.09 × 10−21 m2/V2.

Synthesis and single crystal growth of l-proline cadmium chloride monohydrate and its characterization for higher order harmonic generation applications

Download options Please wait... Article information DOI https://doi.org/10.1039/C3CE41957F Article type Paper Submitted 27 Sep 2013 Accepted 19 Nov 2013 First published 21 Nov 2013 Download Citation CrystEngComm, 2014,16, 2802-2809 BibTex EndNote MEDLINE ProCite ReferenceManager RefWorks RIS Permissions Request permissions Synthesis and single crystal growth of L-proline cadmium chloride monohydrate and its characterization for higher order harmonic generation applications K. Thukral, N. Vijayan, B. Rathi, G. Bhagavannaryana, S. Verma, J. Philip, A. Krishna, M. S. Jeyalakshmy and S. K. Halder, CrystEngComm, 2014, 16, 2802 DOI: 10.1039/C3CE41957F To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page. If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given. If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page. Read more about how to correctly acknowledge RSC content. Social activity Tweet Share Search articles by author Kanika Thukral N. Vijayan Brijesh Rathi G. Bhagavannaryana Sunil Verma J. Philip Anuj Krishna M. S. Jeyalakshmy S. K. Halder

Investigations on the growth aspects and characterization of semiorganic nonlinear optical single crystals of l-histidine and its hydrochloride derivative

Semiorganic single crystals of l-histidine and l-histidine hydrochloride monohydrate have been obtained in a single solution prepared from the mixture of l-histidine and hydrochloric acid in 1:2M ratio. Growth aspects of the single crystals have been discussed along with characterization studies. Crystal system and lattice parameters have been identified by X-ray diffraction analyses. It has been observed that the grown crystals possess orthorhombic system but with different set of lattice parameters. Presence of various functional groups has been identified and formation of two different crystals has been confirmed by Fourier transform infrared spectral analyses and FT-Raman studies. Linear and nonlinear optical properties have been studied by UV–Vis spectral analyses and Kurtz–Perry powder technique respectively. The thermal stability of the grown crystals was determined by thermal analyses. From the characterization studies it is found that both the crystals are useful for second harmonic generation applications.

Bulk growth of ninhydrin single crystals by solvent evaporation method and its characterization for SHG and THG applications

Ninhydrin is a well-known compound generally used in amino acid synthesis and also for detecting the latent fingerprints on porous surfaces. Single crystals can be grown by dissolving the compound in double distilled water at ambient temperature, and can be used as a potential material for second and third harmonic generation applications. The grown specimen was subjected to different characterization techniques in order to find out its suitability for device fabrication. Its lattice dimensions have been confirmed by X-ray powder diffraction and its crystalline quality has been assessed by high resolution X-ray diffraction and X-ray topography methods. The presence of functional groups was identified from HETCOR analysis and confirmed the absence of impurities during crystallization. Its optical properties have been examined by photoluminescence and birefringence analyses. Its thermal parameters such as thermal diffusivity, thermal conductivity and specific capacity have been carried out by following photopyroelectric method. Third order nonlinear optical measurements have been carried out using Z-scan technique and its nonlinear optical absorption coefficient has been determined.

Attosecond control of electron–ion recollision in high harmonic generation

We show that high harmonic generation driven by an intense near-infrared (IR) laser can be temporally controlled when an attosecond pulse train (APT) is used to ionize the generation medium, thereby replacing tunnel ionization as the first step in the well-known three-step model. New harmonics are formed when the ionization occurs at a well-defined time within the optical cycle of the IR field. The use of APT-created electron wave packets affords new avenues for the study and application of harmonic generation. In the present experiment, this makes it possible to study harmonic generation at IR intensities where tunnel ionization does not give a measurable signal.

A diffraction correction for the nonlinearity parameter measured by the harmonic generation technique.

Practical applications of harmonic generation to determine the nonlinearity parameter Beta generally tend toward the lower drive (fundamental) frequencies. As a result, diffraction effects on Beta become more significant. Derivations of a number of different diffraction correction formulas, which are applied for a piston source and a receiver located some distance away, are in the literature. In the paper by Blackburn and Breazeale [J. Acoust. Soc. Am. 76, 1755–1760 (1984)] the correction formulas were applied to the amplitude of the fundamental frequency and the results on Beta were experimentally tested. By building on this earlier work, a diffraction correction formula that includes a factor from a numerical integration algorithm applied to the harmonically generated wave is provided. The formulation of this algorithm is discussed. Experimental results are given for measurements of Beta in AA 2024 to illustrate the agreement.

Nonlinear Optics, Third Edition

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