Crystal growth and negative thermal expansion properties of a Y2Mo4O15 single crystal.

A bulk-size single crystal of Y2Mo4O15 with 20 × 11 × 8 mm3 was successfully grown by the top-seed solution growth (TSSG) method. The full-width at half maximum of (100) and (010) crystal faces is 37 and 27 arcsec, respectively. The thermal conductivity coefficients κ 11, κ 22, κ 33, and κ 13 are determined to be 1.519, 2.097, 0.445, and 0.997 W m-1 K-1, respectively. It is worth noting that the Y2Mo4O15 crystal shows significant anisotropy thermal expansion properties, which exhibits a negative thermal expansion along the b-axis (α 22 = -5.11 × 10-6 K-1). The crystal structure analysis shows that the shrinking of Mo-O bond lengths along the b-axis with the increasing temperature would be the main origin of the negative thermal expansion properties for Y2Mo4O15 crystal, which does not comply with the current mechanism.

Li2 MTeO6 (M=Ti, Sn): Mid-Infrared Nonlinear Optical Crystal with Strong Second Harmonic Generation Response and Wide Transparency Range.

Oxide crystals have been widely used in nonlinear optics (NLO) in the ultraviolet-visible and near-infrared regions. Most traditional oxide crystals are restricted to the mid-infrared region due to their narrow transmission window. Hence, attempting to extend infrared cutoff wavelength of oxides has attracted much attention. Herein, we report two new tellurates Li2 TiTeO6 (LTT) and Li2 SnTeO6 (LST) with broad transparent regions of 0.38-6.72 and 0.38-6.86 µm, respectively, as excellent candidates for mid-infrared NLO applications. Both LTT and LST crystallize in the orthorhombic space group Pnn2. The LTT crystal exhibits intense powder second-order generation efficiency (26×KDP) under the fundamental wavelength of 1064 nm. First-principles calculations and dipole moments were used to illustrate the results of the powder second-harmonic generations based on the crystal structures. Our results provide a novel oxide NLO crystal with a strong SHG and wide transparency range. They also pave a way for the design of new oxide mid-IR NLO crystals.

Generation of a simultaneous orthogonally polarized dual-wavelength Raman laser with power ratio tunability by a single hexagonal crystal: Cs2TeMo3O12.

A new generation of orthogonally polarized dual-wavelength lasers was demonstrated using a dye mode-locked neodymium-doped yttrium aluminum garnet laser for the first time. With a hexagonal Cs2TeMo3O12 as the Raman medium, efficient dual-wavelength stimulated Raman scattering was obtained at 1175 and 1154 nm with similar output power, corresponding to the stretching vibration of Mo-O and the asymmetric stretching vibrations of Mo-O and Te-O groups, respectively. The power ratio of two Raman components can be flexibly adjusted by tuning the polarization of the incident laser, which can be tuned from 0% to 100%. Laser sources with such a small wavelength separation could prove interesting for the difference-frequency generation of terahertz waves in the 4.6 THz range. Our study provides a simple and flexible method to achieve a promising dual-wavelength laser source in orthogonal polarization by Raman-based nonlinear frequency conversions.

Design, growth, and characterization of Y2Mo4O15 crystals for Raman laser applications.

A new crystal Y2Mo4O15 with dimensions of 14 × 12 × 5 mm3 was successfully grown via a top-seeded solution growth (TSSG) method. The crystal structure shows that Y2Mo4O15 crystallizes in the monoclinic space group P21/c (No. 14, a = 6.8110(4) Å, b = 9.5833(6) Å, c = 10.5124(7) Å, ß = 105.512(7)°, and Z = 2) with Mo4O15 and YO7 polyhedra as basic structural units. Optical transmittance spectra of the Y2Mo4O15 crystal exhibited a broad transmission range from 345 nm to 5575 nm. The group theory calculation and spontaneous Raman spectra show that the Y2Mo4O15 crystal has 63 IR-active modes (32Au + 31Bu) and 60 Raman-active modes (30Ag + 30Bg). The strongest Raman shift is located at 953 cm-1 caused by the asymmetric stretching vibrations of the Mo-O bonds. The spontaneous Raman spectra and the possibility of rare-earth doping to the Y2Mo4O15 crystal indicate the Y2Mo4O15 crystal to be a promising Raman and self-Raman crystal.

Shedding Light on the Intrinsic Characteristics of 3D Distorted Fluorite-Type Zirconium Tellurite Single Crystals.

Transition-metal tellurites have motivated growing research interest in both fundamental and applied chemistry, and the corresponding single crystals could serve as rich and fascinating platforms to regulate, explore, and elucidate the intrinsic characteristics of different structures from 0D to 3D architectures. In this context, a zirconium tellurite (namely, ZrTe3O8) single crystal featuring a 3D distorted fluorite-type structure with a size of 35 × 32 × 21 mm3 was successfully harvested by the top-seeded solution growth (TSSG) technique. The X-ray diffraction rocking curve reflects that the crystallinity of the as-grown ZrTe3O8 crystal is quite perfect with a small full-width at half-maximum (fwhm) value (∼39 arcsec). The temperature dependence of the thermophysical properties of the ZrTe3O8 single crystal has been systematically analyzed. The ZrTe3O8 single crystal exhibits a wide transparency window, as the UV and IR absorption cutoff edges are respectively 278 and 7788 nm. The refractive indices over the region from the visible to the near-IR have been determined and manifested relatively large values of 2.0889-2.0370 over a wavelength range of 632.8-1553 nm. Furthermore, the fundamental physical characteristics of the ZrTe3O8 single crystal associated with its distinctive 3D framework structure have been evaluated with density functional theory (DFT) calculations.

Rational Design of a LiNbO3-like Nonlinear Optical Crystal, Li2ZrTeO6, with High Laser-Damage Threshold and Wide Mid-IR Transparency Window.

With existing and emerging technologies urgently demanding the expansion of the laser wavelengths, high-performance nonlinear optical (NLO) crystals are becoming indispensable. Here, a prospective NLO crystal, Li2ZrTeO6, is rationally designed by the element substitution of Nb for Zr and Te from LiNbO3, which has been recognized as one of the most commercial NLO crystals. Li2ZrTeO6 with R3 symmetry inherits the structural merits of LiNbO3 (space group R3 c) and thus meets the requirements for NLO applications, including noncentrosymmetric crystal structure, moderate birefringence, and phase-matchability. Moreover, it can be exploited to achieve more outstanding optical damage resistant behavior (>1.3 GW cm-2), exceeding 22 times that of LiNbO3, which is more suitable for high-energy laser applications. Notably, this compound displays the widest IR absorption edge (7.4 µm) among all of the noncentrosymmetric tellurates reported so far. These excellent attributes suggest that Li2ZrTeO6 is a promising candidate for providing high NLO performance. The substitution of Nb for Zr and Te from LiNbO3 demonstrates a viable strategy toward the rational design of NLO crystals with anticipated properties.

Biaxial crystal ß-BaTeMo2O9: theoretical analysis and the feasibility as high-efficiency acousto-optic Q-switch.

The high efficiency acousto-optic modulators become indispensable in photonics and optoelectronics for the pulse generation and signal modulation in optical display and telecommunications. In this paper, the validity and feasibility of the biaxial crystals as acousto-optic mediums have been theoretically analyzed and confirmed by experiments using a biaxial crystal of ß-BaTeMo2O9. The diffraction angle and diffraction efficiency of the ß-BaTeMo2O9 acousto-optic Q-switch are determined to be 1.420° and 78.1%, which are comparable with that of TeO2 acousto-optic modulator at the identical operating wavelength of 1064 nm and 100 MHz, respectively. The minimum of the modulated pulse width can be achieved to be 6 ns at 5 kHz with Nd:YVO4 as the gain medium. The results not only provide an excellent acousto-optic medium, but also explore the field of biaxial acousto-optic medium for device fabrications.

Theoretical and experimental studies on output characteristics of an intracavity KTA OPO.

An acousto-optically Q-switched Nd:YVO(4)/KTiOAsO(4) (KTA) intracavity optical parametric oscillator (OPO) is efficiently realized in singly resonated scheme. With an end-pumping diode power of 25.9 W, output signal (1535 nm) power of 3.77 W and idler power (3467 nm) of 1.18 W are obtained at a pulse repetition rate of 50 kHz. A rate-equation model is set up to simulate the output power and time characteristics of both signal and idler waves. And both the numerical and experimental results show that the idler pulse width is shorter than the signal one in a singly resonant OPO.

Self-frequency-doubled KTiOAsO4 Raman laser emitting at 573 nm.

A self-frequency-doubled KTiOAsO4 (KTA) Raman laser is realized in a diode-end-pumped acousto-optically Q-switched intracavity Raman laser configuration. A 30-mm-long x-cut KTA crystal is used as the Raman medium, and its 671 cm(-1) Raman mode is employed to finish the conversion from 1064 nm fundamental laser to 1146 nm Raman laser. Self-frequency doubling of the Raman laser is accomplished in the same KTA crystal, and a 573 nm yellow laser is obtained. With an incident diode power of 10.9 W and a pulse repetition rate of 20.8 kHz, a yellow-laser power of 0.82 W is obtained. The conversion efficiency from diode power to yellow-laser power is 7.5%.

A diode side-pumped KTiOAsO4 Raman laser.

A KTiOAsO(4) Raman laser is realized within a diode side-pumped acousto-optically Q-switched Nd:YAG laser. Efficient nanosecond first-Stokes generations at 1091.4 nm are obtained with three 30-mm-long KTA crystals. Under an incident diode power of 60.9 W and a pulse repetition rate of 4 kHz, a first-Stokes power of 4.55 W is obtained, corresponding to a diode-to-Stokes conversion efficiency of 7.5%. The single pulse energy is up to 1.14 mJ and the peak power is 18.0 kW.