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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 109 records · Page 6

Emission of Light by CdMnTe/CdMgTe Heterostructure with Narrow Quantum Wells

The optical properties of the Cd{sub 0.4}Mn{sub 0.4}Te/Cd{sub 0.5}Mg{sub 0.5}Te heterostructure with quantum wells of 7 monolayers in thickness are studied. The temperature dependences of the integral intensity of luminescence of the barrier layer and quantum well and intracenter luminescence of manganese ions are determined, and the luminescence excitation spectra are measured. Numerous components corresponding to LO phonons of the CdTe, MgTe, and MnTe types are observed in the Raman scattering spectra.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Formation of nickel magnetic nanoparticles and modification of nickel phthalocyanine matrix by sodium doping

Data for the vapor-phase doping (300°C) of nickel phthalocyanine (NiPc) by sodium taken in different concentrations (x), as well as structural analysis data for Na{sub x=0.2}NiPc, Na{sub x=1}NiPc, and Na{sub x=3}NiPc samples, have been reported. The structure of the samples and their atomic configuration versus the doping level have been studied by transmission electron microscopy, Raman scattering, X-ray diffraction, X-ray absorption spectroscopy, and extended X-ray absorption fine structure (EXAFS) spectroscopy. The structural parameters of Ni–N, Ni–C, and Ni–Ni bonds have been determined, and it has been found that, at a low level of doping by sodium, local structural distortions are observed in some molecules of the NiPc matrix near nickel atoms. The fraction of these molecules grows as the doping level rises from x = 0.2 to x = 1.0. It has been shown that doping changes the oscillation mode of light atoms, which indicates a rise in the electron concentration on five- and six-membered rings. At a high level of sodium doping (x = 3.0), nickel nanoparticles with a mean size of 20 nm and molecule decomposition products have been observed in the NiPc matrix. It has been found that the fraction of nickel atoms in the Na{sub x=3}NiPc nanoparticles as estimated from EXAFS data is sufficient for the room-temperature magnetic properties of the samples to persist for a long time.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Synthesis of Nano-Crystalline Graphite Films in Hollow Cathode Discharge

The results of experiments on the production of nano-crystalline graphite films in the hollow cathode discharge on Ni(111)/sapphire substrate are presented. The characteristics of the discharge for different gases and pressures are given. The emission spectra of the plasma have been measured. The layers of the deposited graphite have been characterized by the methods of Raman scattering and atomic force microscopy. The field emission of nano-crystalline graphite was also measured. The produced layers have good homogeneity and high value of the electron field emission. The presence of vertically growing graphene is revealed.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Frequency Conversion of High-Power Gyrotron Radiation under Conditions of Raman Backscattering on an Auxiliary Electron Beam

The regime of Raman backscattering of a pumping wave that is cocurrent with an electron beam into the counterpropagating wave can be used for the radiation frequency conversion in high-power gyrotrons. The absolute instability developing in this system ensures generation of a scattered signal in the absence of external resonators, which allows the frequency of scattered radiation to be smoothly controlled within 20–40% by varying the electron energy in the case of high-power (megawatt) gyrotrons used as sources of pumping radiation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

How Does the Shape of the Stellar Spectrum Affect the Raman Scattering Features in the Albedo of Exoplanets?

The diagnostic potential of the spectral signatures of Raman scattering, imprinted in planetary albedo spectra at short optical wavelengths, has been demonstrated in research on planets in the solar system, and has recently been proposed as a probe of exoplanet atmospheres, complementary to albedo studies at longer wavelengths. Spectral features caused by Raman scattering offer insight into the properties of planetary atmospheres, such as the atmospheric depth, composition, and temperature, as well as the possibility of detecting and spectroscopically identifying spectrally inactive species, such as H{sub 2} and N{sub 2}, in the visible wavelength range. Raman albedo features, however, depend on both the properties of the atmosphere and the shape of the incident stellar spectrum. Identical planetary atmospheres can produce very different albedo spectra depending on the spectral properties of the host star. Here we present a set of geometric albedo spectra calculated for atmospheres with H{sub 2}/He, N{sub 2}, and CO{sub 2} composition, irradiated by different stellar types ranging from late A to late K stars. Prominent albedo features caused by Raman scattering appear at different wavelengths for different types of host stars. We investigate how absorption due to the alkali elements sodium and potassium may affect the intensity of Raman features, and we discuss the preferred strategies for detecting Raman features in future observations.

79 ASTRONOMY AND ASTROPHYSICS↗

Modeling of Raman-Scattering Signals in Biological Tissues by Direct and Two-Step Approaches

A search for an effective method of modelling of the Raman-spectroscopy problem in turbid (scattering) media has been performed taking into account the corresponding parameters of the detector and sample volume. A solution of the radiative-transfer equation by Monte-Carlo method underlies the proposed model. Two fundamental approaches to numerical modeling of Raman scattering are considered: the direct transport problem of Rayleigh and Raman photons at each point of the medium and the two-step model, in which a photon flux in the medium is calculated in the first stage, followed by generation of the corresponding number of Raman photons at each point.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Effect of an Optical Breakdown on the Stimulated Raman Scattering in Water in the Field of Picosecond Laser Pulses

Experiments on nonstationary stimulated Raman scattering (SRS) of laser pulses and an optical breakdown are performed to study water samples with gas nanobubbles (bubstons) and without the bubston phase. The SRS excitation threshold in water with the bubston phase turns out to be higher than that in bubston-free water, and the optical breakdown threshold in bubston-containing water is lower than that in bubston-free water. The spectral composition of the SRS signal from bubston-free water samples is found to differ from that of bubston-containing water samples. This effect is caused by the formation of long-lived high-molecular H{sub 2}O complexes near the bubston surface, which are stabilized by the dispersion forces acting from this surface. Since these complexes are located inside 1–2 monolayers adjacent to the surface, the volume density of these complexes is negligibly small as compared to the density of “free” (not bound to bubstons) molecules. To interpret the experimental results, we advance a hypothesis that the detected effect is related to the giant enhancement caused by the generation of a resonance plasmon inside a bubston during an optical breakdown. As follows from our estimates, the bubston-related plasma frequency falls in the range 2600–3200 cm{sup –1}; it is this range that contains the SRS spectral lines of water containing the bubston phase.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Effect of ion interactions on the Raman spectrum of NO 3 − : Toward monitoring of low-activity nuclear waste at Hanford

Raman spectroscopy is a valuable in-situ technique for many applications. The concentrations of species in complex ionic mixtures of nuclear waste can be estimated using Raman measurements. However, it has been experimentally observed that ion interactions can cause a modification of Raman peak intensities and positions. The present work explores the nonlinear behavior associated with the nitrate anion, NO 3 − , which is present in abundance in low activity nuclear waste. We examine changes in the main Raman peak of the nitrate anion in the presence of other ions. A wide range of concentrations are covered, including those expected during direct-feed low-activity waste (DFLAW) processing at the Hanford site in the State of Washington. The experiments showed that the ions interact and associate to form ion pairs, which results in a blue shift (i.e., a shift towards higher wavenumbers) in the main Raman peak of nitrate. The results indicate that cation concentration is a better predictor of the peak shift, compared to ionic strength, both for binary and multicomponent mixtures. These findings have direct implications on the development of spectra-to-composition models for the DFLAW system, since they show deviations from the linearity assumptions used in common chemometric models.

42 ENGINEERING↗

Impact of moderate pump–Stokes chirp on femtosecond coherent anti-Stokes Raman scattering spectra

The effects of inducing moderate chirp in the pump and Stokes beams in chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering (CARS) spectroscopy are discussed. This is an important issue for measurements in high-pressure systems where the CARS beams must be transmitted through glass of significant thickness to reach the probe volume of interest. The effects were investigated both experimentally, by inserting disks of SF-11 glass into the pump and Stokes beam paths, and theoretically, by incorporating pulse chirp into our time-dependent density matrix (TDDM) simulations. Experimentally, we found that inducing moderate pump and Stokes chirp produced significant spectral narrowing of the nonresonant four-wave mixing contribution to the CARS signal, and this allowed us to control the resonant excitation bandwidth to eliminate interferences from neighboring species. The temperature measurement accuracy and precision were essentially unchanged with respect to the unchirped pump and Stokes case. The effect of moderate pump and Stokes chirp on the narrowing of the Raman excitation efficiency envelope was investigated by solving the full set of TDDM through direct numerical integration. The numerical efficiency of the solutions was enhanced dramatically by developing a parallel version of the TDDM code. The calculated Raman excitation efficiency profile was incorporated in our phenomenological spectral fitting codes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Raman spectroscopy of neutron irradiated silicon carbide: Correlation among Raman spectra, swelling, and irradiation temperature

The effects of neutron irradiation on microstructural evolution and the resultant changes in physical and mechanical properties are of critical importance for the development of silicon carbide (SiC) materials for nuclear applications. This study neutron–irradiated β–SiC under a wide range of conditions at temperatures between 235 and 750°C and neutron doses of 0.01–11.8 displacements per atom, and then evaluated the effects on the SiC structure using Raman spectroscopy. The SiC optical phonon lines were shifted to lower wavenumbers by irradiation. Correlations were found among the wavenumber of the longitudinal optical phonon line, irradiation–induced swelling, and irradiation temperature. The peak shift also correlated indirectly with decreasing thermal conductivity of irradiated SiC. The irradiation–induced peak shift is explained by combinations of lattice strain, reduction of the elastic modulus, and other factors including decreasing coherent domain size. Lastly, these findings bridge irradiation–induced microstructural changes and property changes and illustrate how Raman spectroscopy is a useful tool for nondestructively assessing irradiated SiC materials for nuclear applications.

36 MATERIALS SCIENCE↗

Modeling of Atom Interferometer Accelerometer

This report presents the theoretical effort to model and simulate the atom-interferometer accelerometer operating in a highly mobile environment. Multitudes of non-idealities may occur in such a rapidly-changing environment with a large acceleration whose amplitude and direction both change quickly. We studied the undesired effect of high mobility in the atom-interferometer accelerator in a detailed model and a simulator. The undesired effects include the atom cloud's movement during Raman pulses, the Doppler effect due to the relative movement between the atom-cloud and the supporting platform, the finite atom cloud temperature, and the lateral movement of the atom cloud. We present the relevant feed-forward mitigation strategies for each identified non-ideality to neutralize the impact and obtain accurate acceleration measurements.

43 PARTICLE ACCELERATORS↗

Effect of the Plasma Functionalization of Carbon Nanotubes on the Formation of a Carbon Nanotube–Nickel Oxide Composite Electrode Material

The unique properties of carbon nanotubes (CNTs) make these systems promising for the production of composite electrode materials based on a combination of CNTs and transition metal oxides. The effect the parameters of the functionalization of vertically aligned CNT arrays in mixed argon–oxygen high-frequency plasma have on the structural characteristics of CNTs is studied by Raman spectroscopy. The effect the duration of treatment at higher partial argon consumption and low total gas consumption of the working mixture has on the distribution of nickel oxide over a CNT array deposited via SILAR is determined. Results from scanning electron microscopy show that lengthening the duration of functionalization from 30 to 1200 s allows the depth of coating a CNT surface with a nickel oxide layer to be increased from 300 nm to 2.5 μm. Composite structures produced in this work can be used as electrodes of supercapacitors.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Direct evidence of the effect of a moderate external magnetic field on stimulated Raman scattering in the kinetic regime

We present results from an experiment carried out at the OMEGA-EP laser facility that investigated the effect of a perpendicular magnetic field on stimulated Raman scattering (SRS) and report the first direct measurement of magnetic mitigation of SRS. A 13-T magnetic field generated by pulsed-power coils was imposed on a gas jet plasma, and a novel three-picket interaction beam was used to explore SRS reflectivity for several plasma conditions within single shots. The time-resolved backscattered light shows that SRS was mitigated by the external 13-T magnetic field in the kinetic regime (kλ D ∼ 0.3, where k is the electron plasma wave's wavenumber and λ D is electron Debye length) and at a density of n e /n cr ∼ 0.10. On the other hand, we also measured an enhancement of SRS reflectivity at lower density (n e /n cr < 0.08). We discuss experimental results in the context of magnetohydrodynamic and particle-in-cell simulations that scan SRS dynamics for a variety of plasma conditions. While the experimental evidence of SRS mitigation validates prior work on the kinetic simulation of SRS in an external magnetic field, we also find that other mechanisms such as SRS rescatter can lead to an enhancement of measured SRS reflectivity in simulations of parameters relevant to our experiment.

Gas jet↗

Gas Hydrate Film Growth in Microfluidic Channels for Carbon Dioxide Capture and Sequestration Applications

Gas or clathrate hydrates are a solid, crystalline compound composed of water and guest molecules that typically form at high pressure and low temperature conditions. Carbon dioxide (CO2) hydrates may be involved in several carbon dioxide capture and sequestration (CCS) applications, including CO2 pipeline transportation and CO2 offshore sequestration. Within these applications, the formation mechanism and kinetics must be well understood to manage the CCS processes, either by preventing or promoting hydrate formation. In this work, a high-pressure glass microfluidic reactor is used in tandem with visual microscopy and in-situ Raman spectroscopy to study both the morphological and kinetic behavior of gas hydrate crystals. Subcooling, pressure, and CO2 flow rate are investigated for their impact on the thickening behavior of pure CO2 hydrates, with flow rate being the only parameter to have a significant effect. Visual and Raman spectroscopy evidence show that both a dense hydrate layer and a porous hydrate layer form, and the latter may provide a path for mass transfer to continue hydrate crystallization. A first principles mass transfer model is developed to describe CO2 hydrate crystal thickening at the interface between gas and water. The impacts of gas impurities and channel wettability are also studied. This method is further applied to investigate the conversion of methane hydrate to CO2 hydrate for combined energy recovery and methane hydrate formation. The authors acknowledge the US Department of Energy Basic Energy Science award # DE-SC0022162.

Wadsworth, Lindsey [Colorado School of Mines, Gold↗

Quantum Isotope Effect in Silicon at Low Temperatures

High-precision studies of Raman scattering in isotopically pure {sup 28}Si, {sup 29}Si, {sup 30}Si single crystals have been performed in the temperature range from 8 to 300 K. It has been found that a difference of about (0.4 ± 0.1) cm{sup –1} observed at temperatures T ≤ 100 K between the normalized Raman frequencies of the {sup 28}Si and {sup 30}Si isotopes measured with an accuracy of 0.1 cm{sup –1} is certainly due to quantum effects damping with increasing temperature. The possibility of observing quantum isotope effects in germanium has been estimated using experimental data on isotope effects in diamond and silicon.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Polarization-separated double-imaging spectroscopy for weakly-ionized plasma diagnostics

Laser Thomson scattering, which provides thermal properties of electrons, has been extensively utilized in plasma diagnostics. However, being a non-resonant linear light scattering technique, it often encounters several challenges in weakly-ionized plasma diagnostics due to spectral overlap with different scatterings induced from other existing species, including Mie, Rayleigh, and rotational Raman scatterings. To address this challenge, we propose an imaging spectroscopy technique, polarization-separated double-imaging spectroscopy (PoDIS), which selectively separates specific scatterings based on their polarization characteristics. Using an atmospheric plasma jet as a plasma source for demonstration, we show that PoDIS can effectively separate rotational Raman and Thomson scatterings from a superimposed spectrum without prior knowledge or assumptions about the thermal properties of neutrals or electrons. This separation enables independent fitting of the rotational Raman and Thomson scattering spectra, allowing for precise determination of the thermal properties of neutral particles and electrons separately.

Bak, Junhwi [Texas A&M University, College Station↗

Anomalous phonon-mode dependence in polarized Raman spectroscopy of the topological Weyl semimetal TaP

Topological Weyl semimetals (WSMs) have attracted widespread interest due to the chiral Weyl fermions and surface Fermi arcs that enable unique optical and transport phenomena. In this work, we present angle-resolved Raman spectroscopy of TaP, a prototypical noncentrosymmetric WSM, for five excitation wavelengths ranging from 364 to 785 nm. The Raman-active modes, $A_1$, $B^1_1$, and $B^2_1$ modes, exhibit two main unique features beyond the conventional Raman theory. First, the relative intensities of Raman-active modes change as a function of the excitation wavelength. Second, angle-resolved polarized Raman spectra show systematic deviation from the Raman tensor theory. In particular, the $B^1_1$ mode is absent for 633-nm excitation, whereas the $B^2_1$ mode shows an unusual twofold symmetry instead of a fourfold symmetry for 488-, 532-, and 633-nm excitations. Finally, these unconventional phenomena are attributed to the interference effect in the Raman process owing to the existence of multiple carrier pockets with almost the same energy but different symmetries.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗