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At least 55 records · Page 3

Quantitative time-resolved diagnostics of electric field dynamics during individual plasma breakdown events using burst laser pulse electric field induced second harmonic generation

In plasma discharges, the acceleration of electrons by a fast varying electric field and the subsequent collisional electron energy transfer determines the plasma dynamics, chemical reactivity, and breakdown. Current in situ electric field measurements require reconstruction of the temporal profile over many observations. However, such methods are unsuitable for non-repetitive and unstable plasmas. Here, in this paper, we present a method for creating “movies” of dynamic electric fields in a single acquisition at sample rates of 500 × 10 6 fps. This ultrafast diagnostic was demonstrated in radio frequency electric fields between two parallel plates in air, as well as in Ar nanosecond-pulsed single-sided dielectric barrier discharges.

42 ENGINEERING

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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

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.

Lal, R. B.

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.

Marder, Seth R.

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.

Salama, K.

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.

Byer, Robert L.

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.

Marder, Seth R.

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.

Siegman, A. E.

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.

Chang, Daniel

Switchable planar chirality and spin texture in highly ordered ferroelectric hybrid perovskite domains

Chiral organic-inorganic hybrid perovskites offer a promising platform for developing non-linear chiro-optical applications and chiral-induced spin selectivity. Here, we show that achiral hybrid perovskites that have highly ordered ferroelectric domains with orthogonal polarization exhibit planar chirality, as manifested by second harmonic generation with strong circular dichroism. Interestingly, the handedness of the second harmonic generation circular dichroism response can be alternatingly switched between orthogonally polarized domains and domain walls. To correlate the origin of planar chirality in these domains, atom-resolved atomic force microscopy is used to reveal distinct arrangements of atomic rows in these ferroelectric crystals that indicate planar symmetry breaking. Remarkably, a large SHG anisotropy factor of 0.41 is measured at the domain wall. Additionally, spatially resolved two-photon photoluminescence excitation measurement provide evidence of larger Rashba spin-splitting in these chiral ferroelectric domains compared to domain-free areas. Our discoveries of domain-dependent planar chirality and spin texture hold great promise for advancement of domain-specific chiro-optical applications.

36 MATERIALS SCIENCE

Nonlinear van der Waals Metasurfaces with Resonantly Enhanced Light Generation

Efficient nonlinear wave mixing is of paramount importance for a wide range of applications. However, weak optical nonlinearities pose significant challenges for accessing nonlinear light–matter interaction in compact systems. Here, we experimentally study second harmonic generation in deeply subwavelength 3R-MoS 2 metasurfaces (<λ/13 thick). Our measurements, supported by theoretical analysis, reveal a complex interplay and coupling between geometric resonances, optical extinction, and exciton-driven strong nonlinear susceptibility dispersion. We further demonstrate >150-fold enhancement in second harmonic signal at 740 nm mediated by the A exciton resonance. Additionally, our theoretical studies predict an enhancement of more than 10 6 in second harmonic generation in <100 nm thick structures exhibiting bound states in the continuum resonance. These findings provide insight into accessing and harnessing the unprecedented 3R-MoS 2 nonlinearities at a subwavelength scale, paving the way to ultracompact nonlinear photonic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY

Colossal Strain Tuning of Ferroelectric Transitions in KNbO 3 Thin Films

Strong coupling between polarization ( P ) and strain (ɛ) in ferroelectric complex oxides offers unique opportunities to dramatically tune their properties. Here colossal strain tuning of ferroelectricity in epitaxial KNbO 3 thin films grown by sub‐oxide molecular beam epitaxy is demonstrated. While bulk KNbO 3 exhibits three ferroelectric transitions and a Curie temperature ( T c ) of ≈676 K, phase‐field modeling predicts that a biaxial strain of as little as −0.6% pushes its T c > 975 K, its decomposition temperature in air, and for −1.4% strain, to T c > 1325 K, its melting point. Furthermore, a strain of −1.5% can stabilize a single phase throughout the entire temperature range of its stability. A combination of temperature‐dependent second harmonic generation measurements, synchrotron‐based X‐ray reciprocal space mapping, ferroelectric measurements, and transmission electron microscopy reveal a single tetragonal phase from 10 K to 975 K, an enhancement of ≈46% in the tetragonal phase remanent polarization ( P r ), and a ≈200% enhancement in its optical second harmonic generation coefficients over bulk values. These properties in a lead‐free system, but with properties comparable or superior to lead‐based systems, make it an attractive candidate for applications ranging from high‐temperature ferroelectric memory to cryogenic temperature quantum computing.

36 MATERIALS SCIENCE

A contactless in situ EFISH method for measuring electrostatic potential profile of semiconductor/electrolyte junctions

In photoelectrochemical cells, promising devices for directly converting solar energy into storable chemical fuels, the spatial variation of the electrostatic potential across the semiconductor–electrolyte junction is the key parameter that determines the cell performance. In principle, electric field induced second harmonic generation (EFISH) provides a contactless in situ spectroscopic tool to measure the spatial variation of electrostatic potential. However, the total second harmonic generation (SHG) signal contains the contributions of the EFISH signals of semiconductor space charge layer and the electric double layer, in addition to the SHG signal of the electrode surface. The interference of these complex quantities hinders their analysis. In this work, to understand and deconvolute their contributions to the total SHG signals, bias-dependent SHG measurements are performed on the rutile TiO2(100)–electrolyte junction as a function of light polarization and crystal azimuthal angle (angle of the incident plane relative to the crystal [001] axis). A quadratic response between SHG intensity and the applied potential is observed in both the accumulation and depletion regions of TiO2. The relative phase difference and amplitude ratio are extracted at selected azimuthal angles and light polarizations. At 0° azimuthal angle and s-in–p-out polarization, the SHG intensity minimum has the best match with the TiO2 flatband potential due to the orthogonal relative phase difference between bias-dependent and bias-independent SHG terms. We further measure the pH-dependent flatband potential and probe the photovoltage under open circuit conditions using the EFISH technique, demonstrating the capability of this contactless method for measuring electrostatic potential at semiconductor–electrolyte junctions.

Chemistry

Determining the complex second-order optical susceptibility in macroscale van der Waals heterobilayers

In this work, we report on the experimental characterization of the second-order susceptibility in MoSe 2 /WS 2 heterobilayers, including their hidden complex phases. To this end, we developed a heterodyne-detection scheme for second-harmonic generation and applied it to macroscale heterobilayer samples prepared using the gold-tape exfoliation method. The heterodyne scheme enabled us to distinguish the relative orientation of the crystal domains, and furthermore, it allowed us to characterize the complex phases of the susceptibility relative to a reference quartz sample. By comparing the results from the monolayer regions and the heterobilayer region over several hundred microns of the sample area, we determined that the contribution of interlayer effects to second-harmonic generation is within the experimental uncertainty arising from the sample inhomogeneity. The results here provide fundamental quantitative information necessary for the precise design of nanophotonic systems based on stacking engineering.

2D materials

Solid-state Laser Development for the in Situ Spectroscopic Europa Explorer Instrument

The in Situ Spectroscopic Europa Explorer (iSEE) instrument is an ultra-compact laser-enabled Raman spectrometer instrument that meets the top-level science requirements for multiple future planetary in situ missions to explore the surface and atmospheric chemistry of planetary bodies across the Solar System. Enceladus, Europa, the Moon, Mars, and Venus are some of the primary targets for future NASA missions to search for extraterrestrial life and potentially habitable environments beyond Earth, further our understanding of the timing and formation of the Solar System and identify potentially viable economic resources such as water and/or valuable metal assets. We report on the advancement and space flight qualification of a compact, robust, solid-state laser operating at 515 nm that serves as the excitation source for the iSEE investigation. The iSEE instrument is being developed under a NASA Maturation of Instruments for Solar System Exploration (MatISSE) program. The iSEE laser is a diode pumped 1030 nm Yb:YAG microchip laser with a second harmonic generator to achieve an output wavelength of 515 nm and coupled to a multi-mode fiber for delivery to the Raman spectrometer probe. The fundamental 1030 nm laser operates at a pulse repetition frequency (PRF) of 1-10 kHz with pulse energy of 95 μJ and ~800 ps pulse width. A 15 mm long Type II KTP crystal is used for second harmonic generation from 1030 nm to 515 nm. The residual fundamental 1030 nm is separated from the 515 nm beam using a pair of dichroic filters. A focusing lens couples the 515 nm beam to the optical fiber to produce an output laser pulse energy of 20 μJ. A custom vacuum fiber feedthrough assembly was designed with two 105 μm core fibers, and two 200 μm core fibers. One fiber is needed for coupling the laser to the iSEE instrument, and the additionally fibers provide redundancy and design flexibility. The laser enclosure is pressurized with >1 atm of clean dry air. The laser has been designed to minimize the size, weight, and power (SWaP) for a lander instrument with minimal resources. The laser will go through environmental testing including vibration and thermal vacuum testing for space flight qualification. Here we discuss the design, trade studies, performance, and environmental qualificationtesting of the iSEE laser.

Solid state laser, Raman spectrometer, visible las

Program Predicts Performance of Optical Parametric Oscillators

A computer program predicts the performances of solid-state lasers that operate at wavelengths from ultraviolet through mid-infrared and that comprise various combinations of stable and unstable resonators, optical parametric oscillators (OPOs), and sum-frequency generators (SFGs), including second-harmonic generators (SHGs). The input to the program describes the signal, idler, and pump beams; the SFG and OPO crystals; and the laser geometry. The program calculates the electric fields of the idler, pump, and output beams at three locations (inside the laser resonator, just outside the input mirror, and just outside the output mirror) as functions of time for the duration of the pump beam. For each beam, the electric field is used to calculate the fluence at the output mirror, plus summary parameters that include the centroid location, the radius of curvature of the wavefront leaving through the output mirror, the location and size of the beam waist, and a quantity known, variously, as a propagation constant or beam-quality factor. The program provides a typical Windows interface for entering data and selecting files. The program can include as many as six plot windows, each containing four graphs.

Cross, Patricia L.