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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Harnessing complexity: Nonlinear optical phenomena in L-shapes, nanocrescents, and split-ring resonators

Here, we conduct systematic studies of the optical characteristics of plasmonic nanoparticles that exhibit C 2v symmetry. In particular, we analyze three distinct geometric configurations: an L-type shape, a crescent, and a split-ring resonator shaped like the Greek letter π. Optical properties are examined using the finite-difference time-domain method. It is demonstrated that all three shapes exhibit two prominent plasmon modes associated with the two axes of symmetry. This is in addition to a wide range of resonances observed at high frequencies corresponding to quadrupole modes and peaks due to sharp corners. Next, to facilitate nonlinear analysis, we employ a semiclassical hydrodynamic model, where the electron pressure term is explicitly accounted for. This model goes beyond the standard Drude description and enables capturing nonlocal and nonlinear effects. Employing this model enables us to rigorously examine the second-order angular resolved nonlinear optical response of these nanoparticles in each of the three configurations. Two pumping regimes are considered, namely, continuous wave (CW) and pulsed excitations. For CW pumping, we explore the properties of the second harmonic generation (SHG). Polarization and angle-resolved SHG spectra are obtained, revealing strong dependence on the nanoparticle geometry and incident wave polarization. The C 2v symmetry is shown to play a key role in determining the polarization states and selection rules of the SHG signal. For pulsed excitations, we discuss the phenomenon of broadband terahertz (THz) generation induced by the difference-frequency generation . It is shown that the THz emission spectra exhibit unique features attributed to the plasmonic resonances and symmetry of the nanoparticles. The polarization of the generated THz waves is also examined, revealing interesting patterns tied to the nanoparticle geometry. To gain deeper insight, we propose an analytical theory that agrees very well with the numerical experiments. The theory shows that the physical origin of the THz radiation is the mixing of various frequency components of the fundamental pulse by the second-order nonlinear susceptibility. An expression for the far-field THz intensity is derived in terms of the incident pulse parameters and the nonlinear response tensor of the nanoparticle. The results presented in this work offer new insights into the linear and nonlinear optical properties of nanoparticles with C 2v symmetry. The demonstrated strong SHG response and efficient broadband THz generation hold great promise for applications in nonlinear spectroscopy, nanophotonics, and optoelectronics. The proposed theoretical framework also provides a valuable tool for understanding and predicting the nonlinear behavior of other related nanostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

QRCODE: Massively parallelized real-time time-dependent density functional theory for periodic systems

We present a new software module, QRCODE (Quantum Research for Calculating Optically Driven Excitations), for massively parallelized real-time time-dependent density functional theory (RT-TDDFT) calculations of periodic systems in the open-source Qbox software package. Our approach utilizes a custom implementation of a fast Fourier transformation scheme that significantly reduces inter-node message passing interface (MPI) communication of the major computational kernel and shows impressive scaling up to 16,344 CPU cores. In addition to improving computational performance, QRCODE contains a suite of various time propagators for accurate RT-TDDFT calculations. As benchmark applications of QRCODE, we calculate the current density and optical absorption spectra of hexagonal boron nitride (h-BN) and photo-driven reaction dynamics of the ozone-oxygen reaction. We also calculate the second and higher harmonic generation of monolayer and multi-layer boron nitride structures as examples of large material systems. Our optimized implementation of RT-TDDFT in QRCODE enables large-scale calculations of real-time electron dynamics of chemical and material systems with enhanced computational performance and impressive scaling across several thousand CPU cores.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Low duty cycle pulsed UV technique for spectroscopy of aluminum monochloride

We present what we believe to be a novel technique to minimize UV-induced damage in experiments that employ second-harmonic generation cavities. The principle of our approach is to reduce the duty cycle of the UV light as much as possible to prolong the lifetime of the used optics. The low duty cycle is achieved by ramping the cavity into resonance for a short time during the experimental cycle when the light is used and tuning it to an off-resonant state otherwise. The necessary fast ramp and length-stabilization control of the cavity is implemented with the FPGA-based STEMlab platform. We demonstrate the utility of this method by measuring the isotope shift of the electronic transition (X 1 Σ ← A 1 Π) in AlCl at 261.5 nm in a pulsed molecular beam experiment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

High-entropy 1D halide perovskite piezoelectrics found by megalibrary synthesis and rapid nonlinear optical screening

Piezoelectric molecular crystals offer excellent compositional and structural tunability and sustainable processability. However, their discovery is slow, primarily due to the serial synthesis and screening processes used. Here, we report an approach that combines massively parallel megalibrary synthesis with scanning second harmonic generation (SHG) microscopy for rapid screening of piezoelectric molecular crystals. Megalibraries consisting of more than 1,000,000 compositionally distinct but positionally encoded TMCM x TMA (1–x) Cd y Pb (1–y) ClzBr (3–z) (TMCM: trimethylchloromethylammonium, TMA: tetramethylammonium; 0 ≤ x ≤ 1, 0 ≤ y ≤ 1, 0 ≤ z ≤ 3) nanocrystals were synthesized. The megalibraries were rapidly screened by SHG microscopy to identify notable noncentrosymmetric structures, which were then tested for piezoelectricity, facilitating discovery of a high-entropy noncentrosymmetric material with a large d 33 (TMCM 0.75 TMA 0.25 Cd 0.75 Pb 0.25 Cl 1.5 Br 1.5 , 42.8 picocoulombs per newton). Furthermore, this approach enabled systematic investigation of the Curie temperature (T C )–composition relationship in the TMCMCdCl z Br (3–z) system, facilitating reverse design of materials with targeted T C . Our work establishes a powerful approach to accelerate the discovery and design of unusual piezoelectrics for next-generation electronics and optics.

Li, Jun [Northwestern University, Evanston, IL (Un↗
DOE OSTI2025

Crystal Growth of Quaternary Rare Earth Selenosilicates by Using the Flux-Assisted Boron Chalcogen Mixture Method: Investigation of Their Magnetic and Optical Properties

A series of rare earth magnesium selenosilicates, RE3Mg 0.5 SiSe 7 (RE = Ce, Pr, Nd, Sm, Gd, Tb, Dy) were obtained as single crystal using the flux assisted boron chalcogen mixture (BCM) method. The structures of the crystals were determined by single-crystal X-ray diffraction. The RE3Mg 0.5 SiSe 7 series crystallizes in the hexagonal crystal system in the space group P6 3 . Polycrystalline powders were synthesized to perform physical property measurements. Magnetic measurements over the 2–300 K temperature range reveal that Ce 3 Mg 0.5 SiSe 7 and Gd 3 Mg 0.5 SiSe 7 exhibit paramagnetic behavior with negative Weiss constants (θ W = −14.50, θ W = −6.13 K, respectively). The optical properties of RE 3 Mg 0.5 SiSe 7 (RE = Ce, Pr, Nd, Sm, Gd) were measured by ultraviolet–visible (UV–vis) diffuse reflectance. Density functional theory (DFT) electronic structure calculations were performed. Furthermore, a second harmonic generation measurement was performed on a polycrystalline powder of Ce 3 Mg 0.5 SiSe 7 and was found to be SHG active with an efficiency of 0.11 times the standard potassium dihydrogen phosphate (KDP).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Plasma Assisted Combustion and Chemical Processing: Chapter 9 - Plasma Diagnostics

Plasma dynamics and chemistry have a broad range of timescales from picoseconds to milliseconds. In addition, it involves nonequilibrium energy transfer between electrons, ions, electronically and vibrationally excited states, radicals, intermediate species, and reactants and products as well as surface charges and chemistry. To understand plasma physics and chemistry, it is essential to conduct time and space resolved, quantitative detection of nonequilibrium temperature distributions, electron energy and number density, electric field, and species concentrations. There are enormous publications and review articles on this subject. The focus of this chapter is to be placed on the most recent progress in gas phase plasma properties and chemistry, especially on optical emission spectroscopy, laser absorption spectroscopy, Faraday rotational spectroscopy, Raman and Thompson scattering, femtosecond and picosecond (fs/ps) coherent anti-Stokes Raman scattering (CARS) spectroscopy, and electric field-induced second harmonic generation methods.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1989

Kilometric radiation power flux dependence on area of discrete aurora

Kilometer wavelength radiation, measured from distant positions over the North Pole and over the Earth's equator, was compared to the area of discrete aurora imaged by several low-altitude spacecraft. Through correlative studies of auroral kilometric radiation (AKR) with about two thousand auroral images, a stereoscopic view of the average auroral acceleration region was obtained. A major result is that the total AKR power increases as the area of the discrete auroral oval increases. The implications are that the regions of parallel potentials or the auroral plasma cavities, in which AKR is generated, must possess the following attributes: (1) they are shallow in altitude and their radial position depends on wavelength, (2) they thread flux tubes of small cross section, (3) the generation mechanism in them reaches a saturation limit rapidly, and (4) their distribution over the discrete auroral oval is nearly uniform. The above statistical results are true for large samples collected over a long period of time (about six months). In the short term, AKR frequently exhibits temporal variations with scales as short as three minutes (the resolution of the averaged data used). These fluctuations are explainable by rapid quenchings as well as fast starts of the electron cyclotron maser mechanism. There were times when AKR was present at substantial power levels while optical emissions were below instrument thresholds. A recent theoretical result may account for this set of observations by predicting that suprathermal electrons, of energies as low as several hundred eV, can generate second harmonic AKR. The indirect observations of second harmonic AKR require that these electrons have mirror points high above the atmosphere so as to minimize auroral light emissions. The results provide evidence supporting the electron cyclotron maser mechanism.

Saflekos, N. A.↗
NASA NTRS1989

New organic and organometallic salts for second-order nonlinear optics

A series of organometallic and organic salts, in which the cation has been designed to have a large molecular hyperpolarizability, has been prepared. Variation of the counterion (anion) in many cases leads to materials with large powder second harmonic generation (SHG) efficiencies, the highest of which is roughly 2000 times that of a urea reference.

Marder, Seth R.↗
NASA NTRS1990

Coherence properties of a doubly resonant monolithic optical parametric oscillator

A doubly resonant optical parametric oscillator (DRO) pumped with the second harmonic of a narrow-linewidth Nd:YAG laser is described. The linewidth of the DRO signal was less than 13 kHz, the DRO was shown to generate a phase-locked subharmonic of the pump at degeneracy, and the signal and the idler were shown to be mutually coherent with the pump and to be phase-anticorrelated with each other away from degeneracy. The signal-idler heterodyne linewidth was 500 Hz, and pump phase modulation was shown to transfer to the DRO phase at degeneracy.

Nabors, C. D.↗
NASA NTRS1985

KNbO3 single crystal growth by the radio frequency heating Czochralski method

A radio frequency heating Czochralski technique to obtain single crystal KNbO3 is first presented. The technological parameters of KNbO3 crystal growth by the Czochralski technique and its pulling conditions were studied in detail. The experiments on second harmonic generation using 1.06 micrometer Nd:YAG laser in KNbO3 have been conducted. The second harmonic efficiency for upconversion of KNbO3 is found to be as high as that of NaBa2Nb5O15. An automatic scanning measurement for the optical homogeneity of KNbO crystal is also described. KNbO3 is revealed to be a potentially useful nonlinear material for optical device applications.

Wang, W.↗
NASA NTRSDate not supplied

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↗
NASA NTRS1993

Prediction of nonlinear optical properties of organic materials. General theoretical considerations

The prediction of nonlinear optical properties of organic materials is geared to assist materials scientists in the selection of good candidate molecules. A brief summary of the quantum mechanical methods used for estimating hyperpolarizabilities will be presented. The advantages and limitations of each technique will be discussed. Particular attention will be given to the finite-field method for calculating first and second order hyperpolarizabilities, since this method is better suited for large molecules. Corrections for dynamic fields and bulk effects will be discussed in detail, focusing on solvent effects, conformational isomerization, core effects, dispersion, and hydrogen bonding. Several results will be compared with data obtained from third-harmonic-generation (THG) and dc-induced second harmonic generation (EFISH) measurements. These comparisons will demonstrate the qualitative ability of the method to predict the relative strengths of hyperpolarizabilities of a class of compounds. The future application of molecular mechanics, as well as other techniques, in the study of bulk properties and solid state defects will be addressed. The relationship between large values for nonlinear optical properties and large conjugation lengths is well known, and is particularly important for third-order processes. For this reason, the materials with the largest observed nonresonant third-order properties are conjugated polymers. An example of this type of polymer is polydiacetylene. One of the problems in dealing with polydiacetylene is that substituents which may enhance its nonlinear properties may ultimately prevent it from polymerizing. A model which attempts to predict the likelihood of solid-state polymerization is considered, along with the implications of the assumptions that are used. Calculations of the third-order optical properties and their relationship to first-order properties and energy gaps will be discussed. The relationship between monomeric and polymeric third-order optical properties will also be considered.

Cardelino, B.↗
DOE OSTI2024

Layered and Low-Dimensional Lead, Silver, and Bismuth Halide Perovskites Directed by Halogen-Substituted Spacer Cations

Hybrid organic–inorganic metal halides provide a diverse parameter space in which the optoelectronic properties can be tuned through the composition. The compositional tunability extends to the metal site, which can be expanded from single valent metals (e.g., Pb 2+ ) to multivalent metals (e.g., Ag + and Bi 3+ ), and the dimension (2D, 1D, or 0D). However, a deeper understanding of how the organic cations template these metal halide structures is needed. Here, we synthesize and study the structures of a series of new layered and low-dimensional metal (Pb, Ag, and Bi) halides templated by the halogenated aryl spacer cations 2-chlorobenzylammonium (2ClBZ) and 3-chloro-2-fluorobenzylammonium (3Cl2FBZ). We report new lead perovskites, (3Cl2FBZ) 2 PbBr 4 , (2ClBZ) 3 PbI 5 , and (3Cl2FBZ) 2 PbI 4 , and compare them to their silver and/or bismuth analogs (2ClBZ) 4 AgBiBr 8 , (3Cl2FBZ) 4 AgBiBr 8 , (2ClBZ) 3 Bi 2 I 9 , and (3Cl2FBZ) 4 Bi 2 I 10 . In all structures, the halogen-substituted cations result in 2D or “pseudo-2D” layering, but the different halogen substituents introduce different distortions (tilting, octahedral distortion) and dimensional reduction to 1D or 0D depending on the metal and halide compositions. Optical absorption measurements reveal the bandgaps are tunable through metal sites, dimension, and cations to different extents. Furthermore, the 1D (3Cl2FBZ) 4 Bi 2 I 10 crystallizes in the noncentrosymmetric space group Cmc2 1 and exhibits second-harmonic generation (SHG). Furthermore, the organic–inorganic interactions and resultant structural distortions examined here provide insights toward the engineering of noncentrosymmetry and dimensional control in hybrid metal halide perovskites.

Cations↗
DOE OSTI2024

Near Room Temperature Solvothermal Growth of Ferroelectric CsPbBr 3 Nanoplatelets with Ultralow Dark Current

CsPbBr 3 exhibits outstanding optoelectronic properties and thermal stability, making it a coveted material for detectors, light-emitting diodes, and solar cells. Despite observations of ferroelectricity in CsPbBr 3 quantum dots, synthesizing bulk ferroelectric CsPbBr 3 crystals has remained elusive, hindering its potential in next-generation optoelectronic devices like optical switches and ferroelectric photovoltaics. Here, a breakthrough is reported: a novel solvothermal technique enabling the growth of ferroelectric CsPbBr 3 nanoplatelets with lateral dimensions in the tens of micrometers. This represents a significant step toward achieving large-area ferroelectric CsPbBr 3 crystals. Unlike traditional methods, this approach allows for growth and crystallization of CsPbBr 3 in alcohol solutions by enhancing precursor solubility. Further this study confirms the ferroelectric nature of these nanoplatelets using second harmonic generation, electrical characterizations, and piezoresponse force microscopy. This work paves the way for utilizing ferroelectric CsPbBr 3 in novel optoelectronic devices, significantly expanding the potential of this material and opening doors for further exploration in this exciting field.

25 ENERGY STORAGE↗
NASA NTRS2011

Controlling Second Harmonic Efficiency of Laser Beam Interactions

A method is provided for controlling second harmonic efficiency of laser beam interactions. A laser system generates two laser beams (e.g., a laser beam with two polarizations) for incidence on a nonlinear crystal having a preferred direction of propagation. Prior to incidence on the crystal, the beams are optically processed based on the crystal's beam separation characteristics to thereby control a position in the crystal along the preferred direction of propagation at which the beams interact.

Barnes, Norman P.↗
NASA NTRS1985

The 1984 solar oscillation program of the Mount Wilson 60-foot tower

The instrumentation, data, and preliminary results from the summer, 1984, solar oscillation observing program which was carried out using the 60-foot tower telescope of the Mt. Wilson Observatory are described. This program was carried out with a dedicated solar oscillation observing system and obtained full-disk Dopplergrams every 40 seconds for up to 11 hours per day. Between June and September, 1984, observations were obtained with a Na magneto-optical filter on 90 different days. The data analysis has progressed to the point that spherical harmonic filter functions were employed to generate a few one-dimensional power spectra from a single day's observations.

Rhodes, E. J., Jr.↗
NASA NTRS1986

The 1984 solar oscillation program of the Mt. Wilson 60-foot tower

The instrumentation, data, and preliminary results from the summer, 1984, solar oscillation observing program which was carried out using the 60-foot tower telescope of the Mt. Wilson Observatory are described. This program was carried out with a dedicated solar oscillation observing system and obtained full-disk Dopplergrams every 40 seconds for up to 11 hours per day. Between June and September, 1984, observations were obtained with a Na magneto-optical filter on 90 different days. The data analysis has progressed to the point that spherical harmonic filter functions were employed to generate a few one-dimensional power spectra from a single day's observations.

Rhodes, Edward J., Jr.↗