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A series of KDP crystals at different rotation speeds ranging from 9 to 120 rpm were grown by rapid growth method. The results fully demonstrate that rotation speed as a key kinetic parameter has a great influence on the whole crystallization process. Moreover, an important characteristic has been proved that the growth rates along X and Z-direction increase with the increase of rotation speed lower than 100 rpm, while the rates of X-direction are always greater than Z-direction. Combined with numerical simulation method, the correlations of solution stability with kinetic factors including rotation speed, crystal size and growth platform are explored in detail. During the crystallization process, the thickness of boundary layer decrease and a higher flow rate is caused with the increase of rotation speed below 100 rpm, and the generation of inclusions at lower speed may be associated with the slower flow rate of growth solution. The stability of solution gradually decreases as the rotation speed ranges from 100 to 120 rpm. Furthermore, the computed results of Re imply that reducing rotation speed as increasing of crystal size may be an effective method to obtain high-quality and large-scale KDP crystal by rapid growth technique. Comparing to the growing platform with four columns, the platform with two circular connecting columns play an active role in influencing the growth rate of KDP crystal, especially in axial direction.

For KDP and 70%-DKDP crystals, knowledge of thermal-stress distribution induced by weak absorption effect is crucial for their applications, especially in high-power laser systems. Based on photo-thermal common-path interferometry (PCI) technique, the correlations of weak absorption effect with different crystal orientations were systematically evaluated at 1064 nm. An obviously anisotropic property is demonstrated, and a similar pattern of z > x > I > II is also represented for KDP and 70%-DKDP crystals. More importantly, crystal uniformity could be reflected by the weak absorption results, indicating that PCI method could be considered as a novel way to identify the crystal quality. Meanwhile, Thermal parameters including thermal expansion and thermal conductivity were obtained. Using the finite-element method (FEM), the temperature gradients and thermal-stresses along z and x-cut samples were distinctly explored, implying that the corresponding distributions are mainly attributed to crystal orientations. Importantly, another fundamental factor is confirmed that the variation of deuterium content could influence the behaviors of temperature gradients and thermal-stresses distributions. Thus, taking advantage of PCI and FEM as a new approach is more conducive to better understanding the mechanism of laser-matter interactions.

A large sized Nd-doped Ca2Ga2SiO7 single crystal was successfully grown by the Czochralski technique. The effective segregation coefficient of Nd3+ was measured to be 1.16. The thermal, spectroscopic and laser properties were systematically investigated. The thermal conductivity was found to increase with increasing temperature, exhibiting glass or alloy like behavior, and is inherently associated with the disordered structure of the Ca2Ga2SiO7 crystal. The polarized absorption and fluorescence spectra were measured at room temperature, and the spectrum parameters were calculated using the Judd-Ofelt theory. Furthermore, continuous wave laser operation at 1.06 μm along the crystallographic a- and c-axes was demonstrated. A laser output power of 430 mW with an optical conversion efficiency of 14.2% and a slope efficiency of 16.7% was achieved. These results show that Nd:Ca2Ga2SiO7 holds excellent promise for use as a disordered crystalline laser material.

Potassium dihydrogen phosphate (KDP) crystals were grown from aqueous solutions with different concentrations of cyclohexane diamine tetraacetic acid (CDTA) by the “point seed” rapid growth technique. The effects of CDTA on the surface micro morphology of KDP crystals were systematically studied by atomic force microscopy. The prismatic face growth rates of KDP crystals grown from various solutions were measured by a laser polarization interference system. The results shown that the steps became smooth after CDTA doping. When the doping concentration of CDTA is 100 ppm, the bunching of steps on the (100) face reduced dramatically and the step velocity increased obviously due to the complexation between CDTA and the metal impurities in the original solution. When the doping concentration of CDTA is 500 ppm, the excess CDTA adsorbed on the growth surface and impeded the step movement, leading to an increase in step bunching and reduction in step velocity compared with the situation of 100 ppm.

A series of potassium dihydrogen phosphate (KDP) crystals and Fe3+ doped KDP crystals were grown at different temperatures and at the same supersaturation value of 0.02. The prismatic face growth rates of the KDP crystals were measured using a laser polarization interference system. The surface morphologies of the growth steps on the {100} face were comparatively studied using an atomic force microscope systematically. The results showed that the bunching of steps was related to the supersaturation interval in which it was located, and approached the supersaturation dead zone of σd in which the bunching and the slope of the steps were high. The supersaturation dead zone σd and linear zone σ* decreased with rising temperature. Varying the temperature caused considerable changes in the growth speed, step morphology and step motion speed. For the crystal grown in a doped solution, the bunching and slope of the steps reached a maximum value at around 45 °C. It was interesting that the crystal growth rate in the doped solution was higher than that in the undoped solution at around 65 °C and 75 °C, the bunching of the steps was reduced and the width of the steps widened significantly. At the same supersaturation, the growth rate increased with rising temperature and the steps became straight.

Transient numerical calculations were carried out to predict the evolution of temperature and thermal stress in traditionally grown large-size KDP crystals during the removal process, considering two methods that are used to accomplish the crystal extraction. The influence of the crystal size and the difference of temperature between the crystal and environment on the stresses inside the KDP crystals were also investigated in detail. Results indicate that, in both processes of isolating crystals, the highest stress transfers from the crystal periphery to the internal part from the early to the later time stage. In the case of extracting the crystal from solution directly after crystallization and exposing to air, the maximum stress at the crystal periphery is larger than that inside the crystal, and the probability of failure from the outside surface of crystals is large. In the case of retaining the solution for a time after crystallization, the maximum stress in the crystal internal region is larger than that of the crystal surface, leading to a large possibility to originate cracks in the inner region. Both increased crystal sizes and increased temperature differences between the crystals and the environment at the end of crystal growth are factors which aggravate crystal cracking. The maximum stress in crystals in the case of retaining the solution is less than that in the case of extracting the solution, which brings about a decreased likelihood of cracking. Thus, retaining solution for a period of time after the growth is completed, such as 96 h, is suggested to be adopted to accomplish successful crystal extraction.

Two new organic&ndash, inorganic hybrid molecular single crystals, 4-Iodoanilinium perchlorate 18-crown-6 (1) and 4-Iodoanilinium borofluorate 18-crown-6 (2), with large sizes and high thermal stability were successfully synthesized by solution method. Their structures, phase purities, thermal stability, dielectric, absorption and fluorescence spectra were systematically investigated for potential applications. Compounds 1 and 2 crystallize in orthorhombic crystal system, in same space group, namely Pnma. The thermal measurements shown 1 and 2 maintain high thermal stability up to 150 &deg, C. The temperature dependency of dielectric constant was studied, and no distinct anomaly was observed. The band gap were calculated to be 3.38 eV and 3.57 eV for 1 and 2, respectively, slightly smaller than those of layer perovskite (benzylammonium)2PbCl4 semiconducting materials, which have potential applications in optoelectronic detection field. The investigations throw light on the semiconductor properties of organic&ndash, inorganic hybrid crown type material and provide two types of crown compounds with high thermal stability.

The nonlinear refractive index n2 is an important parameter for the nonlinear optical properties of a medium. This study primarily targets to measure the third-order nonlinear optical properties of potassium dihydrogen phosphate (KDP) and deuterated potassium dihydrogen phosphate (DKDP) with 70% deuteration content at λ = 532 nm using the Z-scan technique. The relationship between nonlinear refraction and direction has been studied in detail. Nonlinear refractive index n2, γ and third-order nonlinear susceptibilities xk3 (esu) were calculated through normalized transmittance curves and theoretical formulas. The results indicate that the nonlinear refractive indexes of KDP and DKDP are positive and possess obvious self-focusing effects in high-power laser systems.

Black phosphorous (BP), the most thermodynamically stable allotrope of phosphorus, fills up the lacuna left by other two-dimensional materials with a band gap from 0.3 to 2 eV. The narrow direct band gap and the strong light-matter interaction make BP a promising nonlinear optical (NLO) nano-material. In this paper, the NLO properties of multilayer BP nano-sheets were researched by an open aperture z-scan method. Optical limiting (OL) behavior was observed in the BP material. Three different excitation wavelengths (1064, 532 and 355 nm) were used in the experiments, and the long wavelength excitation exhibited superior NLO performance, including OL and saturable absorption (SA). Our results demonstrate that BP is a promising candidate for OL applications.

The band structure of graphene can be adjusted by incorporating other elements or functional groups, correspondingly, the response to an external light field will also be changed. In this study, we investigated the nonlinear optical (NLO) responses of N-doped graphene nanosheets (N-Gns) with an open aperture Z-scan method, under the excitation of picosecond laser pulses. To the best of our knowledge, this is the first time that two-photon absorption (2PA) of N-Gns has been reported. The normalized nonlinear transmission demonstrates that with the increasing excitation energy, the saturable absorption (SA) and the 2PA appear successively. Compared to the 532 nm excitation, the 1064 nm excitation exhibits smaller saturable intensity Is and larger 2PA coefficient β. At the same time, the N-Gns present superior NLO property compared to pure graphene. Consequently, N-Gns will be a promising candidate for SA or optical limiting (OL) applications.

Nonlinear optical absorption effect in KDP and 70%-DKDP crystals, which were grown by the conventional temperature cooling method, was systematically studied using picosecond pulse laser excitation. Using open aperture Z-scan measurements, the dependence of nonlinear absorption effect on sample orientations (I, II, and z) as well as laser intensity was systematically measured at λ = 1064 and 532 nm. According to the experimental results, the nonlinear absorption effect at λ = 532 nm was confirmed, while at λ = 1064 nm no nonlinear absorption was observed for KDP and 70%-DKDP crystals. In addition, the optical absorption along I- and II-type affected by laser intensity was larger than that along the z-direction. The important nonlinear absorption coefficients β and χ I ( 3 ) (esu) measured along different orientations were exhibited in detail at wavelengths of 1064 nm and 532 nm. The results indicate that nonlinear absorption coefficients increase first and then decrease with the increment of laser intensity for KDP and 70%-DKDP crystals.

Potassium dihydrogen phosphate crystals were grown around 65 °C. The growth rate of KDP (KH2PO4) crystal prismatic faces was measured by laser polarization interference system. The surface micro morphology of KDP crystals grown at various supersaturation were comparatively observed by atomic force microscope systematically. The results show that the growth rate increased with the rise of supersaturation, the aspect ratio reduced. The steps bunching height occurred at σ = 0.03 and 0.04. At this point, the steps height reached maximum value about 11.3~24.4 nm. The step bunching was almost constant at higher supersaturation. A few pits and holes appeared on the crystal surface at high supersaturation. In our opinion, the forming of these pits and holes might be related with the step movement and 2D nuclei mechanism.

Potassium dihydrogen phosphate (KDP) crystals were grown in the presence of a series of chromate (CrO\(_{4}^{2-}\)) additive concentrations via rapid growth method. CrO\(_{4}^{2-}\) made KDP crystals were coloured by yellow-green, suggesting CrO\(_{4}^{2-}\) had entered into the crystal lattice. The elemental analysis indicated that Cr element in KDP crystal was at ppm level. High resolution X-ray diffraction data revealed that the crystalline perfection of these as-grown KDP crystals was destroyed after CrO\(_{4}^{2-}\) entered into crystal lattice, embedded in the full width at half maximum was broadened and satellite peaks appeared. Additionally, the extinction ratio was decreased with rise of CrO\(_{4}^{2-}\) concentration. CrO\(_{4}^{2-}\) introduced two absorption peaks centred at 360 and 280 nm and enhanced the intrinsic absorption near 220 nm, which were at the same band positions compared with the CrO\(_{4}^{2-}\) or HCrO\(_{4}^{-}\) transmittance spectra. Additionally, CrO\(_{4}^{2-}\) could increase the size of light scattering, which was attributed to the point defects and microscopic defects by the replacement by CrO\(_{4}^{2-}\) at PO\(_{4}^{3-}\) position.

In this work, using large-sized single crystals of high optical quality, the optical properties of Ba2TiSi2O8 were systematically investigated, including transmission spectra, refractive indices and nonlinear absorption properties. The crystal exhibits a high transmittance (>84%) over a wide wavelength range from 340 to 2500 nm. The refractive indices in the range from 0.31256 to 1.01398 μm were measured, and Sellmeier’s equations were fitted by the least squares method. The nonlinear absorption properties were studied by using the open-aperture Z-scan technique, with a nonlinear absorption coefficient measured to be on the order of 0.257 cm/GW at the peak power density of 16.4 GW/cm2. Such high transmittance and wide transparency indicate that optical devices using the Ba2TiSi2O8crystal can be applied over a wide wavelength range. Furthermore, the small nonlinear absorption observed in Ba2TiSi2O8 will effectively increase the optical conversion efficiency, decreasing the generation of laser damage of the optical device.

High-quality KDP and DKDP crystals with 12%, 70% and 80%-deuterium content were grown by the conventional temperature cooling method. The nonlinear optical characteristics of K(DxH1-x)2PO4 crystals, including nonlinear absorption and refraction, were systematically investigated through the Z-scan method at λ = 532 nm. The results demonstrate the existence of nonlinear absorption and refraction, and a nonlinear refractive index with a positive sign indicates the generation of self-focusing effect. Moreover, the results indicate that nonlinear absorption and refraction were associated with crystal direction and structure, especially the distribution of H2PO4 - or D2PO4 - groups. For K(DxH1-x)2PO4 crystals, a similar rule of β was z > I > II, while n2 (or χR(3)) was z > II ≈I. These results will evoke more attention to KDP and DKDP applications, especially frequency conversion and electro-optic switch.

Topological Kondo insulators have been attracting great attention from the condensed-matter physics community due to their fascinating topological and strongly correlated properties. Here, we report angle-dependent c-axis magnetoresistance (MR) oscillations in a Kondo insulator, SmB6 single crystal, in a magnetic field of up to 13 T rotated in the ab-plane. Four-fold symmetric MR oscillations are first observed above 8 K, which result from the four-fold (C4) degeneracy of the bulk Fermi surface of SmB6. With decreasing temperature down to 2.3 K, the C4 symmetry of the MR oscillations gradually weakens and C2 symmetry appears. This demonstrates a crossover from three-dimensional bulk states to two-dimensional surface states and implies the possible emergence of topological nematic states. Our experimental observations shed new light on the metallic surface states and nematic states in the Kondo insulator SmB6., 8 pages, 4 figures