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Second-harmonic generation tensors from high-throughput density-functional perturbation theory
Optical materials play a key role in enabling modern optoelectronic technologies in a wide variety of domains such as the medical or the energy sector. Among them, nonlinear optical crystals are of primary importance to achieve a broader range of electromagnetic waves in the devices. However, numerous and contradicting requirements significantly limit the discovery of new potential candidates, which, in turn, hinders the technological development. In the present work, the static nonlinear susceptibility and dielectric tensor are computed via density-functional perturbation theory for a set of 579 inorganic semiconductors. The computational methodology is discussed and the provided database is described with respect to both its data distribution and its format. Several comparisons with both experimental and ab initio results from literature allow to confirm the reliability of our data. The aim of this work is to provide a relevant dataset to foster the identification of promising nonlinear optical crystals in order to motivate their subsequent experimental investigation.
Erratum: Insulating moiré homobilayers lack a threefold symmetric second-harmonic generation [Phys. Rev. Materials 8 , 116203 (2024)]
Erratum on article published over previous cycle, in which the symmetry of a bilayer was erroneously identified. Our results remained unchanged.
Growth and characterization of crystals for room temperature I.R. detectors and second harmonic generation devices
One of the major objectives of this program was to modify the triglycine sulfate (TGS) crystals with suitable dopants and variants to achieve better pyroelectric properties and improved infrared detectivities (D(sup *)), and higher Curie transition temperature compared to undoped TGS crystals. Towards these objectives, many promising dopants, both inorganic and organic, were investigated in the last few years. These dopants gave significant improvement in the D(sup *) value of the infrared detectors fabricated from the grown crystals with no significant increase in the Curie temperature (49 C). The IR detectors were fabricated at EDO/Barnes Engineering Division, Shelton, CT. In the last one year many TGS crystals doped with urea were grown using the low temperature solution crystal growth facility. It is found that doping with urea, the normalized growth yield increased significantly compared to pure TGS crystals and there is an improvement in the pyroelectric and dielectric constant values of doped crystals. This gave a significant increase in the materials figure of merits. The Vicker's hardness of 10 wt percent urea doped crystals is found to be about three times higher in the (010) direction compared to undoped crystals. This report describes in detail the results of urea doped TGS crystals.
Generalized Analytical and Numerical Modeling of Optical Second Harmonic Generation in Anisotropic Crystals and Complex Heterostructures Using #SHAARP Package
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Organometallic Salts Generate Optical Second Harmonics
Series of organometallic salts exhibit large second-order dielectric susceptibilities, as evidenced by generation of second harmonics when illuminated at visible and near-infrared wavelengths. Investigations of these and related compounds continue with view toward development of materials for use as optical second-harmonic generators, electro-optical modulators, optical switches, piezoelectric sensors, and parametric crystals.
Nondestructive ultrasonic characterization of engineering materials
The development of an ultrasonic method for the nondestructive characterization of mechanical properties of engineering material is described. The method utilizes the nonlinearity parameter measurement which describes the anharmonic behavior of the solid through measurements of amplitudes of the fundamental and of the generated second harmonic ultrasonic waves. The nonlinearity parameter is also directly related to the acoustoelastic constant of the solid which can be determined by measuring the linear dependence of ultrasonic velocity on stress. A major advantage of measurements of the nonlinearity parameter over that of the acoustoelastic constant is that it may be determined without the application of stress on the material, which makes it more applicable for in-service nondestructive characterization. The relationships between the nonlinearity parameter of second-harmonic generation and the percentage of solid solution phase in engineering materials such as heat treatable aluminum alloys was established. The acoustoelastic constants are measured on these alloys for comparison and confirmation. A linear relationship between the nonlinearity parameter and the volume fraction of second phase precipitates in the alloys is indicated.
Diode end pumped laser and harmonic generator using same
A second harmonic, optical generator is disclosed in which a laser diode produces an output pumping beam which is focused by means of a graded, refractive index rod lens into a rod of lasant material, such as Nd:YAG, disposed within an optical resonator to pump the lasant material and to excite the optical resonator at a fundamental wavelength. A non-linear electro-optic material such as MgO:LiNbO.sub.3 is coupled to the excited, fundamental mode of the optical resonator to produce a non-linear interaction with the fundamental wavelength producing a harmonic. In one embodiment, the gain medium and the non-linear material are disposed within an optical resonator defined by a pair of reflectors, one of which is formed on a face of the gain medium and the second of which is formed on a face of the non-linear medium. In another embodiment, the non-linear, electro-optic material is doped with the lasant ion such that the gain medium and the non-linear doubling material are co-extensive in volume. In another embodiment, a non-linear, doubling material is disposed in an optical resonator external of the laser gai medium for improved stability of the second harmonic generation process. In another embodiment, the laser gain medium andthe non-linear material are bonded together by means of an optically transparent cement to form a mechanically stable, monolithic structure. In another embodiment, the non-linear material has reflective faces formed thereon to define a ring resonator to decouple reflections from the non-linear medium back to the gain medium for improved stability.
Compounds Generate Optical Second Harmonics
Newly synthesized organic salts found to generate relatively large second-harmonic signals when illuminated by fundamental signals in near-infrared spectrum. Made by crystallizing, with appropriate counterions, organic ions having large molecular hyperpolarizibilities. Large second-order nonlinear susceptibilities observed. These and other compounds having large nonlinear optical properties used in electro-optical modulators, switches, and signal-processing equipment.
Enhancement of second-order optical nonlinearities and nanoscale periodic domain patterning in ferroelectric boron-substituted aluminum nitride thin films
The discovery and development of CMOS-compatible, nonlinear optical materials is essential to produce integrated photonic devices with advanced functionalities. AlN is a strong candidate for on-chip device demonstration due to its intrinsic second-order optical nonlinearities, large bandgap, and well-established fabrication techniques. However, AlN is not easily phase matched for the largest coefficient d 33 ; the coefficients that could potentially be dispersion phase-matched, d 31 and d 15 , have weak nonlinearities. This work investigates ferroelectric Al 1-x B x N (x = 0 to 0.11) for viability as a large bandgap nonlinear optical material with unique suitability towards ultraviolet light generation using second harmonic generation. The linear and nonlinear optical properties are characterized accounting for material anisotropy. With increasing B concentration, a large enhancement from near negligible values to d 31 = 0.9 ± 0.1 pm/V and d 15 = 1.2 ± 0.1 pm/V is observed. This compares favorably to other large bandgap materials like β-Ba(BO 2 ) 2 , where the largest nonlinear coefficient is d 22 ~ 2.3 pm/V at 800 nm. This is accompanied by a change in the bandgap from 6.1 eV to 5.8 eV as B substitution goes from 0 to 11%. A periodically poled, quasi-phase-matched ferroelectric domain pattern with 400 nm domain size and a wall roughness of <16 nm is demonstrated.
Laser system with an antiresonant optical ring
Various applications of an antiresonant ring, consisting of a beam splitter and a number of optical reflectors, are described. With a beam splitter having a transmission coefficient and a reflection coefficient, an optical beam incident on the beam splitter along a first axis is split into two components which circulate around the ring in opposite directions. They are recombined to reflect back the beam along the first axis, with none of the beam power being directed along a second axis. The ring can be part of the cavity of two otherwise independent lasers, with two separate laser mediums external to the ring, or with a multi-wavelength laser medium in the ring. The ring together with a second-harmonic generation crystal and a dispersive phase shifter in the ring can generate the second harmonic of an optical beam.
Waveguide Harmonic Generator for the SIM
A second-harmonic generator (SHG) serves as the source of the visible laser beam in an onboard calibration scheme for NASA's planned Space Interferometry Mission (SIM), which requires an infrared laser beam and a visible laser beam coherent with the infrared laser beam. The SHG includes quasi-phase-matched waveguides made of MgO-doped, periodically poled lithium niobate, pigtailed with polarization- maintaining optical fibers. Frequency doubling by use of such waveguides affords the required combination of coherence and sufficient conversion efficiency for the intended application. The spatial period of the poling is designed to obtain quasi-phase- matching at a nominal middle excitation wavelength of 1,319.28 nm. The SHG is designed to operate at a warm bias (ambient temperature between 20 and 25 C) that would be maintained in its cooler environment by use of electric heaters; the heater power would be adjusted to regulate the temperature precisely and thereby maintain the required precision of the spatial period. At the state of development at the time of this reporting, the SHG had been packaged and subjected to most of its planned space-qualification tests.