Maximization of carbon nanotube yield by solid carbon-assisted dewetting of iron catalyst films
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99 GENERAL AND MISCELLANEOUS↗
SEARCH · Engineering Papers
Results for “RAMAN EFFECT”
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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Engineering Interlayer Electron–Phonon Coupling in WS 2 /BN Heterostructures
In van der Waals (vdW) heterostructures, the interlayer electron–phonon coupling (EPC) provides one unique channel to nonlocally engineer these elementary particles. However, limited by the stringent occurrence conditions, the efficient engineering of interlayer EPC remains elusive. Here we report a multitier engineering of interlayer EPC in WS2/boron nitride (BN) heterostructures, including isotope enrichments of BN substrates, temperature, and high-pressure tuning. The hyperfine isotope dependence of Raman intensities was unambiguously revealed. In combination with theoretical calculations, we anticipate that WS2/BN supercells could induce Brillouin-zone-folded phonons that contribute to the interlayer coupling, leading to a complex nature of broad Raman peaks. We further demonstrate the significance of a previously unexplored parameter, the interlayer spacing. By varying the temperature and high pressure, we effectively manipulated the strengths of EPC with on/off capabilities, indicating critical thresholds of the layer–layer spacing for activating and strengthening interlayer EPC. Our findings provide new opportunities to engineer vdW heterostructures with controlled interlayer coupling.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
One-step aluminium-assisted crystallization of Ge epitaxy on Si by magnetron sputtering
In this work, one-step aluminium-assisted crystallization of Ge on Si is achieved via magnetron sputtering by applying an in-situ low temperature (50 °C to 150 °C) heat treatment in between Al and Ge depositions. The effect of heat treatment on film properties and the growth mechanism of Ge epitaxy on Si are studied via X-ray diffraction, Raman and transmission electron microscopy analyses. Compared with the conventional two-step process, the one-step aluminium-assisted crystallization requires much lower thermal budget and results in pure Ge epitaxial layer, which may be suitable for use as a virtual substrate for the fabrication of III-V solar cells.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Density measurement in air with a saturable absorbing seed gas
Resonantly enhanced scattering from the iodine molecule is studied experimentally for the purpose of developing a scheme for the measurement of density in a gas dynamic flow. A study of the spectrum of iodine, the collection of saturation data in iodine, and the development of a mathematical model for correlating saturation effects were pursued for a mixture of 0.3 torr iodine in nitrogen and for mixture pressures up to one atmosphere. For the desired pressure range, saturation effects in iodine were found to be too small to be useful in allowing density measurements to be made. The effects of quenching can be reduced by detuning the exciting laser wavelength from the absorption line center of the iodine line used (resonant Raman scattering). The signal was found to be nearly independent of pressure, for pressures up to one atmosphere, when the excitation beam was detuned 6 GHz from line center for an isolated line in iodine. The signal amplitude was found to be nearly equal to the amplitude for fluorescence at atmospheric pressure, which indicates a density measurement scheme is possible.
Baganoff, D.↗
Spontaneous Raman Scattering Diagnostics for High-pressure Gaseous Flames
A high-pressure (up to 60 atm) gaseous burner facility with optical access that provides steady, reproducible flames with high precision, and the ability to use multiple fuel/oxidizer combinations has been developed. In addition, a high-performance spontaneous Raman scattering system for use in the above facility has also been developed. Together, the two systems will be used to acquire and establish a comprehensive Raman scattering spectral database for use as a quantitative high-pressure calibration of single-shot Raman scattering measurements in high-pressure combustion systems. Using these facilities, the Raman spectra of H2-Air flames were successfully measured at pressures up to 20 atm. The spectra demonstrated clear rotational and ro-vibrational Raman features of H2, N2, and H2O. theoretical Raman spectra of pure rotational H2, vibrational H2, and vibrational N2 were calculated using a classical harmonic-oscillator model with pressure broadening effects and fitted to the data. At a gas temperature of 1889 K for a phi = 1.34 H2-Air flame, the model and the data showed good agreement, confirming a ro-vibrational equilibrium temperature.
Kojima, Jun↗
Relaxor-like ferroelectric behaviour favoured by short-range B-site ordering in 10% Ba{sup 2+} substituted MgFe{sub 2}O{sub 4}
Graphical abstract: - Highlights: • Mechanism driving polarization in MgFe{sub 2}O{sub 4} is the Maxwell–Wagner polarization. • But Raman studies confirm the existence of local P4{sub 1}22/P4{sub 3}22 symmetry in MgFe{sub 2}O{sub 4}. • Ba{sup 2+} substitution increases ferroelectric ordering, ΔT{sub m} span, and masks electronic contribution. - Abstract: Using the molten salt method, pristine and Ba{sup 2+} substituted MgFe{sub 2}O{sub 4} are prepared. The relaxor-like behaviour observed in the dielectric dispersion indicates the existence of B-site short-range ordering with the local P4{sub 1}22/P4{sub 3}22 symmetry which is confirmed by the Raman spectroscopy. The paper further analyses the origin of polarization using Maxwell–Wagner fit and Nyquist plot. This work suggests a possible way to increase the relaxor-like ferroelectric ordering, larger span of relaxation temperature (ΔT{sub m}) and the effective masking of electronic contribution by the substitution of Ba{sup 2+} ion.
36 MATERIALS SCIENCE↗
Microbial Pigments and Their Degradation Products as Biosignatures
Carotenoids are a class of vibrant biological pigments that have a characteristic chemical structure centered around a polyene core (Lu et al. 2018). Carotenoids and their derivatives are candidate biosignatures because they can persist in the terrestrial geologic record for up to 1.73 billion years (Vinnichenko et al. 2020), have specific structures that are likely the result of complex pathways, mediate the survival of many microorganisms in Mars and Ocean Worlds analog environments, and are detectable with multiple techniques, including Raman spectroscopy. In this project, we aim to investigate the detectability of carotenoid pigments with different spectroscopic methods to inform future instrument selection. We compare the spectra of five unaltered carotenoids, two model compounds, and carotenoid-forming archaeon with visible and deep UV Raman spectroscopy and UVVis absorption spectrophotometry. We then use one model pigment, beta-carotene, to evaluate the likelihood that unique spectral properties of carotenoids, or their refractory byproducts, would be preserved and detectable on a remote planetary surface by exposing it to simulated conditions for Mars. Sample Acquisition. Pigments betacarotene, lutein, zeaxanthin, astaxanthin, and lycopene were purchased from Sigma Aldrich. Halobacterium salinarum NRC-1 was acquired from Carlina Biological and grown in Halobacterium media. Mineral salts including sodium sulfate, sodium carbonate, and halite were used to form matrices in which the beta-carotene was embedded before exposure. Pigment-mineral mixes were at a 1:10 ratio in water. Analytical Techniques. Deep UV Raman data were collected on a custom laboratory mapping spectrometer called MOBIUS (Mineral and Organic Based Investigations using Ultraviolet Spectroscopy), which is an analog to the SHERLOC instrument on the Mars 2020 Perseverance rover (Bhartia et al. 2021). It features a 248.56 nm NeCu pulsed laser, liquid nitrogen-cooled detector, and tunable optical setup. Visible Raman data were collected using a Horiba Jobin Yvon LabRam HR spectrometer with a frequencydoubled Nd:YAG laser (532 nm) and a HeNe laser (633 nm). A VWR 6300 PC UV/Visible Spectrophotometer was used to collect absorption data for carotenoid solutions, model compounds, and solvents in UVpermissible capped cuvettes. Data were collected from 190-1100 nm at 1 nm increments. All spectral data were analyzed using Igor Pro 9 (Wavemetrics). Irradiation. We used a vacuum chamber equipped with a cryostat and a flood electron gun to simulate Martian surface temperatures, low pressures, and ionizing radiation (10keV, 10μA for 6h at 200K for our initial tests). The samples were prepared by drying the pigment-mineral mix onto polished metal tabs, then mounted on the cryostat for processing. Samples were then analyzed directly on the tabs after exposure. Results: In comparing the visible and deep UV Raman spectra of unaltered pigments, we found that they differed drastically. Carotenoids are often studied with visible Raman and typically have peaks at 1525 cm-1 and 1157 cm-1, due to the stretching of the C=C and C-C bonds in the polyene structure. However, in deep UV, the strongest feature is at ~1630 cm-1 and is broad, possibly indicating that multiple peaks are forming this feature. This stark difference is likely due to different preresonant enhancement effects. The UV-Vis results show that there is an absorption band in the deep UV <300 nm, which supports the hypothesis that the 248.6 nm excitation is interrogating another aspect of carotenoids than visible Raman. Our preliminary exposure tests indicated that pigments – even without minerals present - were largely unaltered in the applied conditions, with only a slight broadening in the primary polyene peaks apparent in the visible Raman data. Figure 1. A) Visible vs. deep UV Raman spectra of unaltered beta carotene. B) Schematic of exposure. Conclusions: Our results to date indicate that deep UV and visible Raman spectroscopy, both techniques with planetary mission heritage from Mars 2020 (Wiens et al. 2021, Bhartia et al. 2021), may be used in a complementary manner to observe carotenoids. In addition, we find that beta-carotene is largely resistant to our current exposure conditions, though there may be some amount of amorphization of the material which could cause the broadening of the peaks at 1525 and 1157 cm-1. As a next step, we aim to increase the dosage and duration of exposure to observe degradation of the parent pigment, possibly add UV as a factor via an Ar mini-arc UV lamp and use GC-MS to characterize possible degradation products.
pigments↗
Study of current-voltage characteristics of ferromagnetic α-Fe{sub 1.64}Ga{sub 0.36}O{sub 3} oxide under magnetic fields
We report the influence of magnetic field on I-V characteristics of α-Fe{sub 1.64}Ga{sub 0.36}O{sub 3} sample. Synchrotron X-ray diffraction pattern and Raman Spectroscopy have confirmed rhombohedral structure with space group R3C in the sample. The sample exhibits ferromagnetic feature at room temperature and non saturation of magnetization up to 7Tesla suggests the effect of non-collinear structure (canting) of the spins on the ferromagnetic properties. We have recorded I-V characteristics of the sample under magnetic field to study the effect of non-collinear spin structure on the electrical properties. Space charge limited current mechanism controlled the nature of non-linear I-V curves and the curves are significantly affected by magnetic field.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Interfacial Thermal Conductance between Mechanically Exfoliated Black Phosphorus and SiO x : Effect of Thickness and Temperature
Black phosphorus (BP) is one of new 2D materials that have attracted wide attention. This work reports the interfacial thermal conductance between BP flake and SiO x using Raman spectroscopy. From 293 K down to the 223 K, eight BP flakes in a thickness range of 16.6–113.7 nm are characterized. At 293 K, the largest interfacial thermal conductance is 1.14 × 10 8 W m −2 K −1 for a 82.1 nm thick BP flake, and the smallest one is 2.17 × 10 7 W m −2 K −1 for a 26.6 nm thick BP flake. Such large interfacial thermal conductance can be attributed to the excellent interface contact and strong phonon coupling between BP and SiO x . Furthermore, the measured interfacial thermal conductance has a one‐fold up to around four‐fold increase with decreased temperature from 293 to 223 K, which is a result of thermal‐expansion‐mismatch induced variation in the morphology of BP flakes. Additionally, it demonstrates no thickness‐dependent behavior. It is speculated the intrinsic thickness dependence is weak and is overshadowed by the large variation in the interface contact of different samples. As a new 2D material, BP shows great potential to be a thermal interface material for heat dissipation in electronics.
36 MATERIALS SCIENCE↗
Controlled synthesis of α-MnO{sub 2} nanowires and their catalytic performance for toluene combustion
Highlights: • One-dimensional α-MnO{sub 2} nanowires were prepared by a facile hydrothermal route. • Shape and crystal phase of the products were controlled by tuning reaction conditions. • A possible formation mechanism of the α-MnO{sub 2} nanowires was discussed. • The α-MnO{sub 2} nanowires showed great catalytic activity for toluene combustion. - Abstract: α-MnO{sub 2} nanowires with a length about 6–10 μm and an average diameter of 20 nm were synthesized through a facile hydrothermal process without any templates or surfactants. The products were characterized by X-ray powder diffraction, Raman spectroscopy, field emission scanning electron microscopy, transmission electron microscopy, hydrogen temperature-programmed reduction techniques, X-ray photoelectron spectroscopy and surface area analysis. The effects of the hydrothermal temperature and the concentration of CH{sub 3}COOH on the crystal phase and morphology of the final products were studied in detail. The hydrothermal temperature and the concentration of CH{sub 3}COOH play crucial roles in determining the crystal phase and morphology of the products. The possible formation mechanism of the α-MnO{sub 2} nanowires was investigated and discussed. Additionally, the as-prepared α-MnO{sub 2} nanowires showed higher catalytic activity for toluene combustion than the commercial MnO{sub 2}, suggesting their potential applications in the elimination of volatile organic compounds.
36 MATERIALS SCIENCE↗
The influence of lattice defects, recombination, and clustering on thermal transport in single crystal thorium dioxide
Thermal transport is a key controlling property for thorium dioxide in many applications where defect-generating radiation fields are present. An understanding of the effect of nanoscale lattice defects on thermal transport in this material is currently unavailable due to a lack of high-quality, single crystal material from which unit processes may be investigated. In this work, a series of thorium dioxide single crystals are exposed to 2 MeV proton irradiation at room temperature and 600°C to create microscale regions with varying densities and types of point and extended defects. Defected regions are investigated using spatial domain thermoreflectance to quantify the change in thermal conductivity as a function of ion fluence as well as transmission electron microscopy and Raman spectroscopy to interrogate the structure of the generated defects. Together, this com- bination of methods provides important initial insight into defect formation, recombination, and clustering in thorium dioxide and the effect of those defects on thermal transport. These methods also provide a promising pathway for the quantification of the smallest-scale defects which cannot be captured using traditional microscopy techniques and play and outsized role in degrading thermal performance.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Temperature-induced hexagonal–orthorhombic phase transition in lutetium ferrite nanoparticles
The x-ray diffraction, Raman, and infrared spectroscopies and magnetic measurements were used to explore the correlated changes of the structure, lattice dynamics, and magnetic properties of the LuFeO3 nanoparticles, which appear in dependence on their sintering temperature. We revealed a gradual substitution of the hexagonal phase by the orthorhombic phase in the nanoparticles, with sintering temperature increasing from 700 to 1100 °C. The origin and stability of the hexagonal phase in the LuFeO3 nanoparticles are of the special interest, because the nanoparticles in the phase can be a room-temperature multiferroic with a weak ferromagnetic and pronounced structural and ferroelectric long-range ordering. The antiferromagnetic and nonpolar orthorhombic phase is more stable in the bulk LuFeO3. To define the ranges of the hexagonal phase stability, we determine the bulk and interface energy densities of different phases from the comparison of the Gibbs model with experimental results. Using effective parameters of the Gibbs model, we predict the influence of size effects and temperature on the structural and polar properties of the LuFeO3 nanoparticles. Analysis of the obtained results shows that the combination of the x-ray diffraction, Raman and infrared spectroscopies, magnetic measurements, and theoretical modeling of structural and polar properties allows us to establish the interplay between the phase composition, lattice dynamics, and multiferroic properties of the LuFeO3 nanoparticles prepared under different conditions.
Materials Science↗
Local Oscillations of Silicon–Silicon Bonds in Silicon Nitride
Raman spectra of films of nearly stoichiometric amorphous silicon nitride (a-Si{sub 3}N{sub 4}) reveal a contribution due to local oscillations of silicon–silicon (Si–Si) bonds. This observation directly confirms that the almost stoichiometric a-Si{sub 3}N{sub 4} contains Si–Si bonds, which, according to theoretical predictions, act as electron and hole traps that are responsible for the memory effect in Si{sub 3}N{sub 4}.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Ion irradiation induced strain and structural changes in LiTaO 3 perovskite
LiTaO 3 crystals irradiated with 3 MeV and 1.162 GeV Au ions were studied by single crystal x-ray diffraction and Raman scattering measurements. The maximum lattice strains after 3 MeV Au ion irradiation to a fluence of 1.2 × 10 13 cm -2 were 1.2% and 0.6% along the c- and a-/b-axes, respectively. Two effects were observed in 1.162 GeV Au ion irradiated samples: (i) the (0006) and (1120) Bragg peaks were split into doublets, which suggested a subtle structural change due to slight modification of chemical composition; and (ii) the pre-damaged 1.2% lattice strain along the c-axis was relaxed to 0.9% after subsequent irradiation with 1.162 GeV Au ions, while relaxation along the a- or b-axis was not obvious. A distinct change in the Raman spectrum of the <0001> oriented LiTaO 3 crystals was observed after 1.162 GeV Au ion irradiation, but no obvious change was observed in the <1120> oriented samples or in 3 MeV Au ion irradiated samples. Strain and structural changes in crystalline LiTaO3, with or without pre-existing defects, upon ion irradiation are delineated in its responding to inelastic ionization and elastic nuclear collisions.
36 MATERIALS SCIENCE↗
Effects of B{sub 2}O{sub 3} on Crystallization, Structure, and Heat Transfer of CaO-Al{sub 2}O{sub 3}-Based Mold Fluxes
The reaction between traditional CaO-SiO{sub 2}-based mold fluxes and high-Al steel inevitably changes flux composition, and, consequently, flux properties. This problem can be mitigated by using CaO-Al{sub 2}O{sub 3}-based mold fluxes. To maintain appropriate melting properties, CaO-Al{sub 2}O{sub 3}-based mold fluxes contain B{sub 2}O{sub 3}, which is an effective fluxing agent that decreases the liquidus temperature. In this article, the effects of B{sub 2}O{sub 3} on crystallization behavior, structure, and heat transfer of CaO-Al{sub 2}O{sub 3}-based mold fluxes were studied using single/double hot thermocouple technique, Raman spectroscopy, and infrared emitter technique. The increase of B{sub 2}O{sub 3} content from 7.6 to 13.1 mass pct suppressed the crystallization tendency of mold fluxes in continuous cooling experiments and isothermal experiments conducted over 1273 K (1000 °C). The isothermal crystallization below 1273 K (1000 °C) was also inhibited when B{sub 2}O{sub 3} content increased from 7.6 to 9.6 mass pct; but a further increase of B{sub 2}O{sub 3} content to 13.1 mass pct did not show a visible effect on the crystallization tendency. The increase of B{sub 2}O{sub 3} content from 9.6 to 13.1 mass pct improved the heat fluxes under an incident thermal radiation of 1.6 MW/m{sup 2}; however, the increase of B{sub 2}O{sub 3} content from 7.6 to 9.6 mass pct slightly decreased the heat transfer rate. Crystallization of fluxes and heat transfer were discussed in relation to flux structure.
36 MATERIALS SCIENCE↗
Nonlinear post-compression to sub-20 fs using a single-stage multipass cell filled with ambient air
Noble gas-filled multipass cells have proven to be very effective in compressing high-energy, hundreds-of-femtoseconds pulses down to tens of femtoseconds. Molecular gases can be an attractive alternative to noble gases since they provide additional Raman nonlinearities that can be much stronger than the electronic Kerr nonlinearity and can therefore enable more spectral broadening and shorter compressed pulses. Air at atmospheric pressure offers molecular gases in their simplest format, with both easy access and no costs for implementing a gas chamber. Here we demonstrate a single-stage, air-filled multipass cell that spectrally broadens 145- μ J, 185-fs pulses with >90% throughput, with a small fraction of the output compressed to sub-20 fs using a prism-pair compressor. The multipass cell uses standard broadband mirrors without dispersion engineering and ambient air as the nonlinear medium, making it the simplest and most cost-effective solution for generating few-cycle femtosecond pulses.
47 OTHER INSTRUMENTATION↗
Processing Raman Spectra of High-Pressure Hydrogen Flames
The Raman Code automates the analysis of laser-Raman-spectroscopy data for diagnosis of combustion at high pressure. On the basis of the theory of molecular spectroscopy, the software calculates the rovibrational and pure rotational Raman spectra of H2, O2, N2, and H2O in hydrogen/air flames at given temperatures and pressures. Given a set of Raman spectral data from measurements on a given flame and results from the aforementioned calculations, the software calculates the thermodynamic temperature and number densities of the aforementioned species. The software accounts for collisional spectral-line-broadening effects at pressures up to 60 bar (6 MPa). The line-broadening effects increase with pressure and thereby complicate the analysis. The software also corrects for spectral interference ("cross-talk") among the various chemical species. In the absence of such correction, the cross-talk is a significant source of error in temperatures and number densities. This is the first known comprehensive computer code that, when used in conjunction with a spectral calibration database, can process Raman-scattering spectral data from high-pressure hydrogen/air flames to obtain temperatures accurate to within 10 K and chemical-species number densities accurate to within 2 percent.
Nguyen, Quang-Viet↗
Effect of hydrogen bonding on the vibrational dephasing time in glycerol
The vibrational dephasing of the methyl CH2 symmetric stretch mode in glycerol was directly measured over an extended temperature range using picosecond coherent Raman pump and probe spectroscopy. The dephasing time was found to increase dramatically as the temperature of the supercooled liquid was lowered. This observation is attributed to the increased hydrogen bonding with decreasing temperature which hinders the dephasing of the CH2 vibration by reducing molecular motions.
Dorsinville, R.↗