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At least 127 records · Page 7

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NASA NTRS1973

SO2 Spectroscopy with A Tunable UV Laser

A portion of the fluorescence spectrum of SO2 has been studied using a narrow wavelength doubled dye laser as the exciting source. One purpose of this study is to evaluate the use of SO2 resonance re-emission as a probe of SO2 in the atmosphere. When the SO2 is excited by light at 300.2 nm, for example, a strong reemission peak is observed which is Stokes-shifted from the incident light wavelength by the usual Raman shift (the VI symmetric vibration frequency 1150.5/cm ). The intensity of this peak is sensitive to small changes (.01 nm) in the incident wavelength. Measurements of the N2 quenching and self quenching of this re-emission have been obtained. Preliminary analysis of this data indicates that the quenching is weak but not negligible. The dye laser in our system is pumped by a pulsed N2 laser. Tuning 'and spectral narrowing are accomplished using a telescope-echelle grating combination. In a high power configuration the resulting pulses have a spectral width of about 5 x 10(exp -3) nm and a time duration of about 6 nsec. The echelle grating is rotated by a digital stepping motor, such that each step shifts the wavelength by 6 x 10(exp -4) nm. In addition to the tunable, narrow wavelength uv source and spectral analysis of the consequent re-emission, the system also provides time resolution of the re-emitted light to 6 nsec resolution. This capability is being used to study the lifetime of low pressure S02 fluorescence at different wavelengths and pressures.

Morey, W. W.↗

NASA NTRS2000

High-Frequency Excitation of a Plane Wake

In the early 1990's, Glezer and his co-workers at Georgia Tech made a startling discovery. They found that forcing at frequencies too high to directly affect the production scales led to a dramatic alteration in the development of a turbulent shear layer. An experimental study of this phenomenon is presented in Wiltse and Glezer. They used piezoelectric actuators located near the jet exit plane to force the shear layers of a square low-speed jet. The actuators were driven at a high frequency in the Kolmogorov inertial subrange, much higher than the frequencies associated with the large-scale motion (where the turbulent energy is produced and located) but much lower than those associated with the Kolmogorov scale (where the turbulent energy is dissipated). Measurements of the shear-layer turbulence showed that direct excitation of small-scale motion by high-frequency forcing led to an increase in the turbulent dissipation of more than an order of magnitude in the initial region of the shear layer! The turbulent dissipation gradually decreased with downstream distance but remained above the corresponding level for the unforced flow at all locations examined. The high-frequency forcing increased the turbulent kinetic energy in the initial region near the actuators, but the kinetic energy decreased quite rapidly with downstream distance, dropping to levels that were a small fraction of the level for the unforced case. Perhaps most importantly from the present standpoint, the high-frequency forcing significantly decreased the energy in the large-scale motion, increasingly so with downstream distance. Wiltse and Glezer interpreted this behavior as an enhanced transfer of energy from the large scales to the small scales. The initial work by Wiltse and Glezer has expanded into other applications. To explore the potential of high-frequency forcing for active acoustic suppression, in 1998 the first author proposed a set of experiments involving an edge tone shear layer and an open cavity flow. This work was funded by the US Air Force Research Laboratory, and the experiments were developed and executed at Boeing by Raman and Kibens. These experiments involved high-frequency forcing applied to low-speed flows using wedge piezo actuators and powered resonance tubes. The system is simple, open loop, compact, potentially requires little power, and is easily integrated. Dramatic results, such as reductions of 20 dB in spectral peaks and 5-8 dB in overall levels across the entire acoustic spectrum, were obtained in some cases. Sample results are presented. Following this success in low-speed flows, an international cooperative program continuing this work involved transonic experiments in a mid-size facility in the United Kingdom. Similar reductions in noise level were obtained in these transonic experiments. Discussion of this work is given in Raman et at. and Stanek, Raman, Kibens, and Ross. Other experiments at Georgia Tech have shown significant potential of high-frequency forcing in controlling reaction rates in chemically reacting flows.

Cain, Alan B.↗

DOE OSTI2020

Surface Hydration and Hydroxyl Configurations of Gibbsite and Boehmite Nanoplates

Discontinuation of the bulk structure at the interface between metal oxide particles and water leads to altered bonding characteristics and unique facet-dependent molecular environments. Surface hydration and consequent hydroxylation adds further complexity to the interface, details that for metal (oxy)hydroxides are especially difficult to isolate from the background signal of bulk structural hydroxyls. Here we probe for the first time the hydroxylation and hydration structures on basal surfaces of gibbsite (?-Al(OH)3) and boehmite (?-AlOOH) nanoplates at ambient conditions, using the interface-sensitive technique vibrational sum frequency generation spectroscopy (VSFG). Hydroxyl stretching modes at the interfaces with adsorbed water layers compared directly to Raman and infrared bulk modes show that while gibbsite surface frequencies were sharp and nearly identical to those in the bulk, boehmite surface hydroxyls displayed a very different broad spectrum of states. Ab initio molecular dynamics simulations of both basal surfaces with and without hydration waters reveal that gibbsite surface hydroxyls interact only weakly with overlying hydration waters remaining essentially unperturbed, whereasthose on boehmite can interact more strongly facilitated by higher configurational degrees of freedom at the interface. The findings clearly unveil substantial differences in the hydrated interfacial dynamics of these two otherwise similar materials, with implications for their interfacial chemistry and wettability.

Sassi, Michel JPC↗

NASA NTRS1985

Multiple Raman up-conversion of radiation from pre-existing Langmuir turbulence

Little is known regarding the mechanisms involved in the production of radiation at frequencies which are much higher than the maximum plasma frequency in nonmagnetic plasmas. It is pointed out that radiation at high multiples of the plasma frequency has been observed in laser-pellet experiments, in relativistic beam-plasma interactions, and in low-energy beam-plasma interactions. Radiation at twice the plasma frequency can be produced by coalescence of two Langmuir waves. Another approach is based on radiation near the plasma frequency or its second harmonic, produced by instability or by external sources. Raman scatter from preexisting Langmuir turbulence is permitted repeatedly. At each step such scattering will produce frequency upshifts (anti-Stokes process) and downshifts (Stokes process). The present paper is concerned with this process. Attention is given to equilibrium spectra, analytic approximations, laser-plasma interaction and coherent radiation from relativistic electron beams.

Russell, D.↗

DOE OSTI2021

Beyond single crystals: Imaging rubrene polymorphism across crystalline batches through lattice phonon Raman microscopy

Polymorphism is an issue troubling numerous scientific fields. A phenomenon where molecules can arrange in different orientations in a crystal lattice, polymorphism in the field of organic photovoltaic materials can dramatically change electronic properties of these materials. Rubrene is a benchmark photovoltaic material showing high carrier mobility in only one of its three polymorphs. To use rubrene in devices, it is important to quantify the polymorph distribution arising from a particular crystal growth method. However, current methods for characterizing polymorphism are either destructive or inefficient for batch scale characterization. Lattice phonon Raman spectroscopy has the ability to distinguish between polymorphs based on low frequency intermolecular vibrations. Here, we present here the addition of microscopy to lattice phonon Raman spectroscopy, which allows us to not only characterize polymorphs efficiently and nondestructively through Raman spectroscopy but also concurrently gain information on the size and morphology of the polymorphs. We provide examples for how this technique can be used to perform large, batch scale polymorph characterization for crystals grown from solution and physical vapor transport.We end with a case study showing how Raman microscopy can be used to efficiently optimize a green crystal growth method, selecting for large orthorhombic crystals desired for rubrene electronic device applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Structural features of solid-solid phase transitions and lattice dynamics in U 3 O 8

Triuranium octoxide (U 3 O 8 ) undergoes an orthorhombic to hexagonal structural phase transition near Ts=305°C, and a separate nonstructural phase transition at Tc=210°C. The later transition has previously been associated with temperature-induced fluctuations in the uranium oxidation state. A discontinuity in the slope of electrical conductivity versus temperature measurement at 210°C has supported this idea. The orthorhombic phase has three crystallographic sites in two distinct oxidation configurations [2 U(V) and 1 U(VI)], whereas the hexagonal phase has one distinct uranium site. High-resolution x-ray diffraction measurements eliminate the possibility of superlattice Bragg reflections to less than 0.2 e - scattering power and U 3 O 8 is not metallic; consequently, the presence of oxidation fluctuations is required for charge balancing. Interestingly, the order-to-disorder transition occurs at a much lower temperature than the structural transition. Using temperature-dependent x-ray diffraction and Raman spectroscopy, we show anisotropic lattice expansion in the in-plane b and c lattice constants. A specific discontinuity in the temperature derivatives of the b and c lattice constants are the first reported structural signatures of the order-to-disorder transition, suggestive of a change in local U–O coordination. Phonon frequencies of U 3 O 8 measured by Raman spectroscopy show significant temperature-dependent dynamics. Redshifting of several modes between 40 and 300°C cannot be explained by unit cell expansion alone because the unit cell volume decreases in this region. Instead, we show that phonon frequencies are highly correlated with the anisotropic lattice expansion/contraction along specific crystallographic directions.

36 MATERIALS SCIENCE↗

NASA NTRS1992

Femtosecond resolution of soft mode dynamics in structural phase transitions

The microscopic pathway along which ions or molecules in a crystal move during structural phase transition can often be described in terms of a collective vibrational mode of the lattice. In many cases, this mode, called a 'soft' phonon mode because of its characteristically low frequency near the phase transition temperature, is difficult to characterize through conventional frequency-domain spectroscopies such as light or neutron scattering. A femtosecond time-domain analog of light-scattering spectroscopy called impulsive stimulated Raman scattering (ISRS) has been used to examine the soft modes of two perovskite ferroelectric crystals. The low-frequency lattice dynamics of KNbO3 and BaTiO3 are clarified in a manner that permits critical evaluation of microscopic models for their ferroelectric transitions. The results illustrate the advantages of ISRS over conventional Raman spectroscopy of low-frequency, heavily damped soft modes.

Dougherty, Thomas P.↗

NASA NTRS2005

Atomic Clock Based on Opto-Electronic Oscillator

A proposed highly accurate clock or oscillator would be based on the concept of an opto-electronic oscillator (OEO) stabilized to an atomic transition. Opto-electronic oscillators, which have been described in a number of prior NASA Tech Briefs articles, generate signals at frequencies in the gigahertz range characterized by high spectral purity but not by longterm stability or accuracy. On the other hand, the signals generated by previously developed atomic clocks are characterized by long-term stability and accuracy but not by spectral purity. The proposed atomic clock would provide high spectral purity plus long-term stability and accuracy a combination of characteristics needed to realize advanced developments in communications and navigation. In addition, it should be possible to miniaturize the proposed atomic clock. When a laser beam is modulated by a microwave signal and applied to a photodetector, the electrical output of the photodetector includes a component at the microwave frequency. In atomic clocks of a type known as Raman clocks or coherent-population-trapping (CPT) clocks, microwave outputs are obtained from laser beams modulated, in each case, to create two sidebands that differ in frequency by the amount of a hyperfine transition in the ground state of atoms of an element in vapor form in a cell. The combination of these sidebands produces a transparency in the population of a higher electronic level that can be reached from either of the two ground-state hyperfine levels by absorption of a photon. The beam is transmitted through the vapor to a photodetector. The components of light scattered or transmitted by the atoms in the two hyperfine levels mix in the photodetector and thereby give rise to a signal at the hyperfine- transition frequency. The proposed atomic clock would include an OEO and a rubidium- or cesium- vapor cell operating in the CPT/Raman regime (see figure). In the OEO portion of this atomic clock, as in a typical prior OEO, a laser beam would pass through an electro-optical modulator, the modulated beam would be fed into a fiber-optic delay line, and the delayed beam would be fed to a photodetector. The electrical output of the photodetector would be detected, amplified, filtered, and fed back to the microwave input port of the modulator. The laser would be chosen to have the same wavelength as that of the pertinent ground-state/higher-state transition of the atoms in the vapor. The modulator/ filter combination would be designed to operate at the microwave frequency of the hyperfine transition. Part of the laser beam would be tapped from the fiberoptic loop of the OEO and introduced into the vapor cell. After passing through the cell, this portion of the beam would be detected differentially with a tapped portion of the fiber-optically-delayed beam. The electrical output of the photodetector would be amplified and filtered in a loop that would control a DC bias applied to the modulator. In this manner, the long-term stability and accuracy of the atomic transition would be transferred to the OEO.

Maleki, Lute↗

DOE OSTI2025

Raman Fingerprints of Phase Transitions and Ferroic Couplings in van der Waals Multiferroic CuCrP 2 S 6

CuCrP 2 S 6 (CCPS), a type-II multiferroic material, exhibits unique phase transitions involving ferroelectric, antiferroelectric, and antiferromagnetic ordering. Here, in this study, we conduct a comprehensive investigation on the intricate phase transitions and their multiferroic couplings in CCPS across a wide temperature range from 4 to 345 K through Raman spectroscopic measurements down to 5 cm –1 . We first assign the observed Raman modes with the support of theoretical calculations and angle-resolved polarized Raman measurements. We further present clear signatures of phase transitions from the analyses of temperature-dependent Raman spectral parameters. Particularly, two low-frequency soft modes are observed at 36.1 cm –1 and 70.5 cm –1 below 145 K, indicating the antiferroelectric to quasi-antiferroelectric transition. Moreover, phonon mode hardening is observed when the temperature increases from 4 to 65 K, suggesting negative thermal expansion (NTE) and strong magnetoelastic coupling below 65 K. These findings advance the understanding of vdW multiferroic CCPS, paving the way for future design and engineering of multiferroicity in cutting-edge technologies, such as spintronics and quantum devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1997

Barium Nitrate Raman Laser Development for Remote Sensing of Ozone

In order to understand the impact of anthropogenic emissions upon the earth's environment, scientists require remote sensing techniques which are capable of providing range-resolved measurements of clouds, aerosols, and the concentrations of several chemical constituents of the atmosphere. The differential absorption lidar (DIAL) technique is a very promising method to measure concentration profiles of chemical species such as ozone and water vapor as well as detect the presence of aerosols and clouds. If a suitable DIAL system could be deployed in space, it would provide a global data set of tremendous value. Such systems, however, need to be compact, reliable, and very efficient. In order to measure atmospheric gases with the DIAL technique, the laser transmitter must generate suitable on-line and off-line wavelength pulse pairs. The on-line pulse is resonant with an absorption feature of the species of interest. The off-line pulse is tuned so that it encounters significantly less absorption. The relative backscattered power for the two pulses enables the range-resolved concentration to be computed. Preliminary experiments at NASA LaRC suggested that the solid state Raman shifting material, Ba(NO3)2, could be utilized to produce these pulse pairs. A Raman oscillator pumped at 532 nm by a frequency-doubled Nd:YAG laser can create first Stokes laser output at 563 nm and second Stokes output at 599 nm. With frequency doublers, UV output at 281 nm and 299 nm can be subsequently obtained. This all-solid state system has the potential to be very efficient, compact, and reliable. Raman shifting in Ba(NO3)2, has previously been performed in both the visible and the infrared. The first Raman oscillator in the visible region was investigated in 1986 with the configurations of plane-plane and unstable telescopic resonators. However, most of the recent research has focused on the development of infrared sources for eye-safe lidar applications.

McCray, Christopher L.↗

DOE OSTI2026

Adsorption of hydroxamic acid ligands for improved extraction of rare earth elements from monazite ores

Efficient separation of rare earth element (REE) ores via froth flotation requires the development of novel ligands with enhanced adsorption capacity and selectivity. To realize these advances, understanding the mechanisms underlying interactions between the ligand and mineral surfaces is essential. This study systematically evaluates the adsorption behavior of alkyl- and aromatic alkyl-substituted hydroxamic acid ligands on monazite surfaces using complementary spectroscopic techniques, including UV–visible (UV–vis) spectroscopy, Raman spectroscopy, infrared spectroscopy, and vibrational sum frequency generation (SFG) spectroscopy, together with the ab initio molecular dynamics (AIMD) simulations. Among the studied ligands, octanohydroxamic acid (OHA) and 4-ethoxy-N,2-dihydroxybenzamide (EDHBA) exhibit high adsorption capacity under basic pH (8–10) by forming multilayers on the surface. OHA has a higher equilibrium adsorption capacity compared to EDHBA, but it forms a less stable multilayer susceptible to disruption in the presence of interfering ions. AIMD results show that OHA adopts a single stable chelating geometry, while EDHBA exhibits multiple binding modes involving distinct interactions with La surface atoms and phosphate-bound oxygens, resulting in more complex adsorption kinetics. The variations in surface binding and intermolecular interactions observed between alkyl and aromatic molecules influence the differences in adsorption kinetics, equilibrium adsorption capacities on the mineral surface, and their flotation performance. This work provides valuable insight into the adsorption mechanism of ligands at mineral interfaces, which is crucial for guiding the design of new ligands with enhanced separation performance.

Zhou, Muchu [ORNL] (ORCID:0000000182650215)↗

NASA NTRS2010

Platform for Post-Processing Waveform-Based NDE

Signal- and image-processing methods are commonly needed to extract information from the waves, improve resolution of, and highlight defects in an image. Since some similarity exists for all waveform-based nondestructive evaluation (NDE) methods, it would seem that a common software platform containing multiple signal- and image-processing techniques to process the waveforms and images makes sense where multiple techniques, scientists, engineers, and organizations are involved. NDE Wave & Image Processor Version 2.0 software provides a single, integrated signal- and image-processing and analysis environment for total NDE data processing and analysis. It brings some of the most useful algorithms developed for NDE over the past 20 years into a commercial-grade product. The software can import signal/spectroscopic data, image data, and image series data. This software offers the user hundreds of basic and advanced signal- and image-processing capabilities including esoteric 1D and 2D wavelet-based de-noising, de-trending, and filtering. Batch processing is included for signal- and image-processing capability so that an optimized sequence of processing operations can be applied to entire folders of signals, spectra, and images. Additionally, an extensive interactive model-based curve-fitting facility has been included to allow fitting of spectroscopy data such as from Raman spectroscopy. An extensive joint-time frequency module is included for analysis of non-stationary or transient data such as that from acoustic emission, vibration, or earthquake data.

Roth, Don J.↗

DOE OSTI2023

Suppressing parametric instabilities in direct-drive inertial-confinement-fusion plasmas using broadband laser light

It has long been recognized that broadband laser light has the potential to control parametric instabilities in inertial-confinement-fusion (ICF) plasmas. Here, we use results from laser-plasma-interaction simulations to estimate the bandwidth requirements for mitigating the three predominant classes of instabilities in direct-drive ICF implosions: cross-beam energy transfer (CBET), two-plasmon decay (TPD), and stimulated Raman scattering (SRS). We find that for frequency-tripled, Nd:glass laser light, a bandwidth of 8.5 THz can significantly increase laser absorption by suppressing CBET, while ∼13 THz is needed to mitigate absolute TPD and SRS on an ignition-scale platform. None of the glass lasers used in contemporary ICF experiments, however, possess a bandwidth greater than 1 THz and reaching larger values requires the use of an auxiliary broadening technique such as optical parametric amplification or stimulated-rotational-Raman scattering. An arguably superior approach is the adoption of an argon-fluoride (ArF) laser as an ICF driver. Besides having a broad bandwidth of ∼10 THz, the ArF laser also possesses the shortest wavelength (193 nm) that can scale to the high energy/power required for ICF—a feature that helps to mitigate parametric instabilities even further. We show that these native properties of ArF laser light are sufficient to eliminate nearly all CBET scattering in a direct-drive target and also raise absolute TPD and SRS thresholds well above those for broadband glass lasers. The effective control of parametric instabilities with broad bandwidth is potentially a “game changer” in ICF because it would enable higher laser intensities and ablation pressures in future target designs.

Bates, J. W. (ORCID:0000000188087240)↗

NASA NTRS2018

Fiber-Based Laser MOPA Transmitter Packaging for Space Environment

NASA’s Goddard Space Flight Center has been developing lidar to remotely measure CO2 and CH4 in the Earth’s atmosphere. The ultimate goal is to make space-based satellite measurements with global coverage. We are working on maturing the technology readiness of a fiber-based, 1.57-micron wavelength laser transmitter designed for use in atmospheric CO2 remote-sensing. To this end, we are building a ruggedized prototype to demonstrate the required power and performance and survive the required environment. We are building a fiber-based master oscillator power amplifier (MOPA) laser transmitter architecture. The laser is a wavelength-locked, single frequency, externally modulated DBR operating at 1.57-micron followed by erbium-doped fiber amplifiers. The last amplifier stage is a polarization-maintaining, very-large-mode-area fiber with ~1000 μm2 effective area pumped by a Raman fiber laser. The optical output is single-frequency, one microsecond pulses with >450 μJ pulse energy, 7.5 KHz repetition rate, single spatial mode, and > 20 dB polarization extinction.

Lasers and Masers↗

NASA NTRS2001

Frequency conversion system

A frequency conversion system comprises first and second gain sources providing first and second frequency radiation outputs where the second gain source receives as input the output of the first gain source and, further, the second gain source comprises a Raman or Brillouin gain fiber for wave shifting a portion of the radiation of the first frequency output into second frequency radiation output to provided a combined output of first and second frequencies. Powers are gain enhanced by the addition of a rare earth amplifier or oscillator, or a Raman/Brillouin amplifier or oscillator between the high power source and the NFM device. Further, polarization conversion using Raman or Brillouin wavelength shifting is provided to optimize frequency conversion efficiency in the NFM device.

Sanders, Steven↗

NASA NTRS1986

Nd:Glass-Raman laser for water vapor dial

A tunable solid-state Raman shifted laser which was used in a water vapor Differential Absorption Lidar (DIAL) system at 9400 A is described. The DIAL transmitter is based on a tunable glass laser operating at 1.06 microns, a hydrogen Raman cell to shift the radiation to 1.88 microns, and a frequency doubling crystal. The results of measurements which characterize the output of the laser with respect to optimization of optical configuration and of Raman parameters were reported. The DIAL system was also described and preliminary atmospheric returns shown.

Kagann, R. H.↗

NASA NTRS1991

Study of cluster formation and its effects on Rayleigh and Raman scattering measurements in a Mach 6 wind tunnel

Using a frequency-doubled Nd-YAG pulsed laser and a single-intensified CCD camera, Rayleigh scattering measurements have been performed to study the cluster formation in a Mach 6 wind tunnel at NASA Langley Research Center. These studies were conducted both in the free stream and in a model flow field for various flow conditions to gain an understanding of the dependence of the Rayleigh scattering (by clusters) on the local pressures and temperatures in the facility. Using the same laser system, simultaneous measurements of the local temperature have also been performed using the rotational Raman scattering of molecular nitrogen and determined the densities of molecular oxygen and nitrogen by using the vibrational Raman scattering from these species. Quantitative results are presented in detail with emphasis on the applicability of the Rayleigh scattering for obtaining quantitative measurements of molecular densities both in the free stream and in the model flow field.

Shirinzadeh, B.↗

NASA NTRS1991

Study of Cluster Formation and its Effects on Rayleigh and Raman Scattering Measurements in a Mach 6 Wind Tunnel

Using a frequency-doubled Nd-YAG pulsed laser and a single-intensified CCD camera, Rayleigh scattering measurements have been performed to study the cluster formation in a Mach 6 wind tunnel at NASA Langley Research Center. These studies were conducted both in the free stream and in a model flow field for various flow conditions to gain an understanding of the dependence of the Rayleigh scattering (by clusters) on the local pressures and temperatures in the facility. Using the same laser system, we have also performed simultaneous measurements of the local temperature using the rotational Raman scattering of molecular nitrogen and determined the densities of molecular oxygen and nitrogen by using the vibrational Raman scattering from these species. Quantitative results will be presented in detail with emphasis on the applicability of the Rayleigh scattering for obtaining quantitative measurements of molecular densities both in the free stream and in the model flow field.

Shirinzadeh, B.↗