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At least 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Deterministic fabrication of graphene hexagonal boron nitride moiré superlattices

The electronic properties of moiré heterostructures depend sensitively on the relative orientation between layers of the stack. For example, near-magic-angle twisted bilayer graphene (TBG) commonly shows superconductivity, yet a TBG sample with one of the graphene layers rotationally aligned to a hexagonal Boron Nitride (hBN) cladding layer provided experimental observation of orbital ferromagnetism. To create samples with aligned graphene/hBN, researchers often align edges of exfoliated flakes that appear straight in optical micrographs. However, graphene or hBN can cleave along either zig-zag or armchair lattice directions, introducing a 30° ambiguity in the relative orientation of two flakes. By characterizing the crystal lattice orientation of exfoliated flakes prior to stacking using Raman and second-harmonic generation for graphene and hBN, respectively, we unambiguously align monolayer graphene to hBN at a near-0°, not 30°, relative twist angle. We confirm this alignment by torsional force microscopy of the graphene/hBN moiré on an open-face stack, and then by cryogenic transport measurements, after full encapsulation with a second, nonaligned hBN layer. This work demonstrates a key step toward systematically exploring the effects of the relative twist angle between dissimilar materials within moiré heterostructures.

boron nitride↗
DOE OSTI2024

Phase-Selective Synthesis of Rhombohedral WS 2 Multilayers by Confined-Space Hybrid Metal–Organic Chemical Vapor Deposition

Rhombohedral polytype transition metal dichalcogenide (TMDC) multilayers exhibit non-centrosymmetric interlayer stacking, which yields intriguing properties such as ferroelectricity, a large second-order susceptibility coefficient χ (2) , giant valley coherence, and a bulk photovoltaic effect. These properties have spurred significant interest in developing phase-selective growth methods for multilayer rhombohedral TMDC films. Here, in this study, we report a confined-space, hybrid metal–organic chemical vapor deposition method that preferentially grows 3R-WS 2 multilayer films with thickness up to 130 nm. We confirm the 3R stacking structure via polarization-resolved second-harmonic generation characterization and the 3-fold symmetry revealed by anisotropic H 2 O 2 etching. The multilayer 3R WS 2 shows a dendritic morphology, which is indicative of diffusion-limited growth. Multilayer regions with large, stepped terraces enable layer-resolved evaluation of the optical properties of 3R-WS 2 via Raman, photoluminescence, and differential reflectance spectroscopy. These measurements confirm the interfacial quality and suggest ferroelectric modification of the exciton energies.

3R-WS2↗
NASA NTRS1990

Generating Second Harmonics In Nonlinear Resonant Cavities

Single-axial-mode lasers pump very-low-loss doubling crystals. Important advance in making resonant generation of second harmonics possible for diode-laser-pumped solid-state lasers is recent development of monolithic nonplanar ring geometries in neodymium:yttrium aluminum garnet (Nd:YAG) lasers that produce frequency-stable single-mode outputs. Other advance is development of high-quality MgO:LiNbO3 as electro-optically nonlinear material. Series of experiments devised to improve doubling efficiency of low-power lasers, and particularly of diode-laser-pumped continuous-wave Nd:YAG lasers.

Kozlovsky, William J.↗
NASA NTRS2010

Fiber-Coupled Planar Light-Wave Circuit for Seed Laser Control in High Spectral Resolution Lidar Systems

Precise laser remote sensing of aerosol extinction and backscatter in the atmosphere requires a high-power, pulsed, frequency doubled Nd:YAG laser that is wavelength- stabilized to a narrow absorption line such as found in iodine vapor. One method for precise wavelength control is to injection seed the Nd:YAG laser with a low-power CW laser that is stabilized by frequency converting a fraction of the beam to 532 nm, and to actively frequency-lock it to an iodine vapor absorption line. While the feasibility of this approach has been demonstrated using bulk optics in NASA Langley s Airborne High Spectral Resolution Lidar (HSRL) program, an ideal, lower cost solution is to develop an all-waveguide, frequency-locked seed laser in a compact, robust package that will withstand the temperature, shock, and vibration levels associated with airborne and space-based remote sensing platforms. A key technology leading to this miniaturization is the integration of an efficient waveguide frequency doubling element, and a low-voltage phase modulation element into a single, monolithic, planar light-wave circuit (PLC). The PLC concept advances NASA's future lidar systems due to its compact, efficient and reliable design, thus enabling use on small aircraft and satellites. The immediate application for this technology is targeted for NASA Langley's HSRL system for aerosol and cloud characterization. This Phase I effort proposes the development of a potassium titanyl phosphate (KTP) waveguide phase modulator for future integration into a PLC. For this innovation, the proposed device is the integration of a waveguide-based frequency doubler and phase modulator in a single, fiber pigtail device that will be capable of efficient second harmonic generation of 1,064-nm light and subsequent phase modulation of the 532 nm light at 250 MHz, providing a properly spectrally formatted beam for HSRL s seed laser locking system. Fabrication of the integrated PLC chip for NASA Langley, planned for the Phase II effort, will require full integration and optimization of the waveguide components (SHG waveguide, splitters, and phase modulator) onto a single, monolithic device. The PLC will greatly reduce the size and weight, improve electrical- to-optical efficiency, and significantly reduce the cost of NASA Langley s current stabilized HSRL seed laser system built around a commercial off-the-shelf seed laser that is free-space coupled to a bulk doubler and bulk phase modulator.

Cook, Anthony↗
DOE OSTI2024

Dephasingless two-color terahertz generation

A laser pulse composed of a fundamental and an appropriately phased second harmonic can drive a time-dependent current of photoionized electrons that generates broadband THz radiation. Over the propagation distances relevant to many experiments, dispersion causes the relative phase between the harmonics to evolve. This “dephasing” slows the accumulation of THz energy and results in a multi-cycle THz pulse with significant angular dispersion. Here, we introduce a novel optical configuration that compensates the relative phase evolution, allowing for the formation of a half-cycle THz pulse with almost no angular dispersion. The configuration uses the spherical aberration of an axilens to map a prescribed radial phase variation in the near field to a desired longitudinal phase variation in the far field. Simulations that combine this configuration with an ultrashort flying focus demonstrate the formation of a half-cycle THz pulse with a controlled emission angle and 1/4 the angular divergence of the multi-cycle pulse created by a conventional optical configuration.

47 OTHER INSTRUMENTATION↗
NASA NTRS2008

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↗
DOE OSTI2024

Frequency-domain computing using nonlinear acoustic-wave device on lithium niobate

Abstract Multiply-accumulation are crucial computing operations in signal processing, numerical simulations, and machine learning. In recent years, optical analog approaches have demonstrated higher computing performance and better power efficiency than their digital counterparts. However, analog computing chips usually need large areas and complex structures for parallel computing, as a single device element only executes one computing operation at a single time. Here, we demonstrate frequency-domain computing using the nonlinear acoustic-wave devices on lithium niobate, featuring a normalized external second-harmonic generation conversion efficiency of ~ 5.7 × 10-4 W-1. The second-order sum-frequency nonlinear process of lithium niobate enables multiplication of inputs encoded in the frequency domain. Compared to the analog schemes, our device features a notably simpler design, and nanofabrication requires only one lift-off. Using a single acoustic-wave device within an area of 0.03 mm2, we can simultaneously conduct over 130,000 multiply-accumulation operations. Our acoustic-wave device shows applications in real and complex vector convolutions and image processing. This demonstration sets the stage for experimental realizations into frequency-domain integrated nonlinear acoustic computing systems, potentially shaping future developments in acoustic neural networks and quantum computing.

chai, mingzhao (ORCID:0009000466226341)↗
DOE OSTI2025

Long-lived photoinduced polar states in metal halide perovskites

Ferroic polarization in hybrid perovskites is crucial for enhancing photovoltaic performance and developing potential electronic applications. Controlling ferroic polarization with an optical field enables probing of ferroic polarization without the unwanted interface ionic effects caused by electronic contacts. This study employs ultrafast near-infrared photoexcitation to control dynamic structural transitions in soft single crystalline hybrid Cu (II) halide perovskites, achieving a long-lived polar state (beyond 104 s) at room temperature. We probe reversible long-lived polar domains under near-infrared photoexcitation using in-situ second harmonic generation microscopy. Theoretical calculation informs the polar lattice microstrain likely induced by anisotropic structure deformation in octahedral copper halide under near-infrared photoexcitation. The reversible slow structure deformation is further confirmed by in-situ photo-induced X-ray diffraction measurement. This work provides a material platform for understanding, controlling, and probing polarization under photoexcitation. Our methodology enables the identification of previously undiscovered polar phases in ferroelectric halide perovskites.

Dou, Yixuan↗
NASA NTRS1993

Quantum noise and squeezing in optical parametric oscillator with arbitrary output coupling

The redistribution of intrinsic quantum noise in the quadratures of the field generated in a sub-threshold degenerate optical parametric oscillator exhibits interesting dependences on the individual output mirror transmittances, when they are included exactly. We present a physical picture of this problem, based on mirror boundary conditions, which is valid for arbitrary transmittances. Hence, our picture applies uniformly to all values of the cavity Q factor representing, in the opposite extremes, both perfect oscillator and amplifier configurations. Beginning with a classical second-harmonic pump, we shall generalize our analysis to the finite amplitude and phase fluctuations of the pump.

Prasad, Sudhakar↗
DOE OSTI2025

Phonon second harmonic generation in NaBr studied by inelastic neutron scattering and computer simulation

The phenomenon of second harmonic generation (SHG) was found for phonons in anharmonic NaBr by inelastic neutron scattering. The temperature dependence of this phonon SHG was measured from 300 K to 650 K. At 300 K the second harmonic (SH) is seen as a high-energy branch around 33 meV, nearly independent of $\overrightarrow{Q}$. The temperature effective potential (TDEP) method and classical molecular dynamics (MD) simulation with machine learning interatomic potential were able to reproduce the SH, and showed that SHG occurs with the flat transverse optical (TO) phonon branch. A classical model of a nonlinear medium explains the intensity and lifetime of the SH, compared to those of the TO modes. Also successful was a quantum model based on the Heisenberg-Langevin equation for interacting phonons coupled to a thermal bath, which also predicts a spectral distribution of the SH. In conclusion, the measured temperature dependence of the intensity of the second harmonic showed that it follows the Planck distribution of a one-phonon quasiparticle, and not two TO phonons.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Non-resonant picosecond three-wave mixing in the gas phase

We report on the experimental observation of non-resonant, second-order optical sum-frequency generation (SFG) in five different atomic and molecular gases. The measured signal is attributed to a SFG process by characterizing its intensity scaling and its polarization behavior. We show that the electric quadrupole mechanism cannot explain the observed trends and suggest a mechanism based on symmetry breaking along the incident beam path arising from laser-induced species ground state number density gradients. Our results demonstrate that the SFG is about four orders of magnitude stronger than the third-harmonic generation (THG) and independent from any externally applied electric fields. In conclusion, these features make this method suitable for gas number density measurements at the picosecond time scale in reactive flows and plasmas.

LaCombe, Grayson↗
NASA NTRS1993

Optimum wavelengths for two color ranging

The range uncertainties associated with the refractive atmosphere can be mitigated by the technique of two color, or dual wavelength, ranging. The precision of the differential time of flight (DTOF) measurement depends on the atmospheric dispersion between the two wavelengths, the received pulsewidths and photoelectron counts, and on the amount of temporal averaging. In general, the transmitted wavelengths are not independently chosen but instead are generated via nonlinear optics techniques (harmonic crystals, Raman scattering, etc.) which also determine their relative pulsewidths. The mean received photoelectrons at each wavelength are calculated via the familiar radar link equation which contains several wavelength dependent parameters. By collecting the various wavelength dependent terms, one can define a wavelength figure of merit for a two color laser ranging system. In this paper, we apply the wavelength figure of merit to the case of an extremely clear atmosphere and draw several conclusions regarding the relative merits of fundamental-second harmonic, fundamental-third harmonic, second-third harmonic, and Raman two color systems. We find that, in spite of the larger dispersion between wavelengths, fundamental-third harmonic systems have the lowest figure of merit due to a combination of poor detector performance at the fundamental and poor atmospheric transmission at the third harmonic. The fundamental-second harmonic systems (approximately 700 nm and 350 nm) have the highest figure of merit, but second-third harmonic systems, using fundamental transmitters near 1000 nm, are a close second. Raman-shifted transmitters appear to offer no advantage over harmonic systems because of the relatively small wavelength separation that can be achieved in light gases such as hydrogen and the lack of good ultrashort pulse transmitters with an optimum fundamental wavelength near 400 nm.

Degnan, John J.↗
DOE OSTI2026

Crystal Structures, Optical Behavior, and Magnetic Properties in Hydrated Lanthanide Iron Sulfates

Single crystals of LnFe(SO 4 ) 3 (H 2 O) 2 (Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Dy, Ho, Er, Tm; compounds 1–11) and LnFe(SO 4 ) 3 (H 2 O) (Ln = Tm, Yb, Lu; compounds 12–14) were synthesized under hydrothermal conditions. Single-crystal X-ray diffraction (SCXRD) analysis revealed that the dihydrated compounds (1–11) crystallize in centrosymmetric (CS) structures, with the lanthanide ions adopting eight-coordinate geometries. In contrast, the monohydrated compounds (12–14) exhibit noncentrosymmetric (NCS) structures, where the lanthanide ions are seven-coordinated. Vibrating sample magnetometry (VSM) confirmed that compounds 2, 4, and 7–11 are paramagnetic below 400 K, with compound 8 displaying the highest magnetic susceptibility. Compounds 1, 5, 6, 13, and 14 show a sharp increase in magnetic susceptibility at Néel temperatures ( T N ) of approximately 72, 76, 70, 58, and 56 K, respectively, indicating antiferromagnetic ordering. High-temperature magnetic susceptibility measurements further support the presence of antiferromagnetic transitions in these compounds. Second harmonic generation (SHG) measurements showed that the noncentrosymmetric Yb (compound 13) and Lu (compound 14) compounds exhibit SHG intensities of 0.3× and 1.6× that of potassium dihydrogen phosphate (KDP), respectively.

anions↗
DOE OSTI2026

Adaptive nonlinear wavefront shaping in layered TMDs

Two-dimensional transition metal dichalcogenides are promising candidates for nonlinear photonics applications, offering strong nonlinear susceptibility and compatibility with integrated platforms. Although considerable effort has been devoted to manipulating second harmonic generation in these materials, the dynamic control of nonlinear wavefronts remains largely unexplored. Metasurfaces have enabled significant progress in nonlinear beam engineering, yet their practical implementation is limited by low conversion efficiencies and restricted design flexibility. In this work, we employ feedback-based wavefront shaping using spatial light modulators to enhance SHG from pyramid-like WS 2 multilayer structures by over three orders of magnitude in selected spatial regions. This approach allows us to program nonlinear holograms and dynamically shape the SHG signal through phase-only modulation, opening new possibilities for nonlinear imaging, optical information processing, and data communication.

Mavian, Alex [Rensselaer Polytechnic Inst., Troy, ↗
NASA NTRS1999

Melt Growth of a Nonlinear Optical Crystal Triethylphosphine Sulfide using Modified Bridgman-Stockbarger Technique

Bulk single crystals of triethylphosphine sulfide (C2H5)3P(S), a potential nonlinear optical organic material has been grown from melt using Bridgman- Stockbarger method. Commercially available material triethylphosphine sulfide procured from Johnson Matthey was purified by physical vapor transport using low pressure sublimaton (about 30 mTorr). Modified Bridgman-Stockbarger technique is characterized by the smallest possible quantity of product in the melt for a short period of time. The temperature gradient was chosen to be about 10 C/cm and the ampoule was lowering rate was chosen to be 0.2-0.3 mm/h. For various growth conditions, several single crystal of triethylphosphine sulfide have been grown with sizes 10X10X15mm(exp 3). The second harmonic generation (SHG) efficiency was measured and has been found to be comparable to phase matched potassium dihydrogen phosphate crystals. Further characterization of the grown single crystals is in progress and the results will be presented at the symposium.

Curry, K.↗
NASA NTRS2000

Molecular Modeling and Experimental Study of Nonlinear Optical Compounds: Mono-Substituted Derivatives of Dicyanovinylbenzene

A search for potential nonlinear optical (NLO) compounds has been performed using the Cambridge Structural Database and molecular modeling. We have studied a series of mono-substituted derivatives of dicyanovinylbenzene as the NLO properties of one of its derivatives (o-methoxy-dicyanovinylbenzene, DIVA) were described earlier. The molecular geometry in the series of the compounds studied was investigated with an X- ray analysis and discussed along with results of molecular mechanics and ab initio quantum chemical calculations. The influence of crystal packing on the molecular planarity has been revealed. Two new compounds from the series studied were found to be active for second harmonic generation (SHG) in the powder. The measurements of SHG efficiency have shown that the o-F- and p-Cl-derivatives of dicyanovinylbenzene are about 10 and 20- times more active than urea, respectively. The peculiarities of crystal structure formation in the framework of balance between the van der Waals and electrostatic interactions have been discussed. The crystal morphology of DIVA and two new SHG-active compounds have been calculated on the basis of their known crystal structures.

Timofeeva, Tatyana V.↗
NASA NTRS1996

Incorporation of New Benzofulvene Derivatives Into Polymers to Give New NLO Materials

The need for fast electro-optic switches and modulators for optical communication, and laser frequency conversion has created a demand for new second-order non-linear optical materials. One approach to produce such materials is to align chromophores with large molecular hyperpolarizabilities in polymers. Recently fulvenes and benzofulvenes which contain electron donating groups have been shown to exhibit large second-order non-linear optical properties. The resonance structures shown below suggest that intramolecular charge transfer (ICT) should be favorable in omega - (hydroxyphenyl)benzofulvenes and even more favorable in omega-omega - (phenoxy)benzofulvenes because of the enhanced donor properties of the O group. This ICT should lead to enormously enhanced second-order hyperpolarizability. We have prepared all three new omega - (hydroxyphenyl)benzofulvenes by the condensation of indene with the appropriate hydroxyaryl aldehyde in MeOH or MeOH/H2O under base catalysis. In a similar fashion we have prepared substituted benzofulvenes with multipal donor groups. Preliminary studies show that some of our benzofulvene derivatives exhibit second order harmonic generation (SHG). Measurements were carried out by preparing host-guest polymers. The results of our work on benzofulvene derivatives in host-guest polymers when covalently bonded in the polymer will be described.

Bowens, Andrea D.↗