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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
NASA NTRS2018

Nanoscale Fabrication of Microwave Detectors from Commercially-Available CVD-Grown Monolayer Graphene

Using commercially-available monolayer graphene, synthesized by means of chemical vapor deposition, microwave power sensing elements have been nanofabricated and integrated with microwave-grade test structures suitable for on-wafer probing. The graphene, situated on a thermal oxide, was first cleaned of stray contaminants in a forming gas environment briefly held at 250 degrees Celsius using a rapid thermal annealer. Immediately following this step, the graphene was passivated with a protective aluminum oxide layer (approximately S nm in thickness). Micrometer-scale Corbino disc test structures were then fabricated in direct contact with the graphene using a self-aligned process, which relies on the fact that tetramethylammonium hydroxide develops the photoresist while removing the aluminum oxide. Graphene nanoribbons (with widths as small 400 nm) were then fabricated across the Corbino disc gaps using electron-beam writing in conjunction with a negative tone resist. The same developer exposed the majority of the graphene while defining nanometer-scale lines of photoresist stacked upon aluminum oxide. These stacks served as etch-stops while the unprotected graphene was ion-milled in an oxygen plasma. Finally, the photoresist was removed leaving behind passivated graphene nanoribbons. Damage caused by the fabrication was evaluated by comparing the Raman spectra of the grapheme before and after processing.

detectors↗
DOE OSTI2024

Dynamic Bubbling Balanced Proactive CO 2 Capture and Reduction on a Triple-Phase Interface Nanoporous Electrocatalyst

The formation and preservation of the active phase of the catalysts at the triple-phase interface during CO 2 capture and reduction is essential for improving the conversion efficiency of CO 2 electroreduction toward value-added chemicals and fuels under operational conditions. Designing such ideal catalysts that can mitigate parasitic hydrogen generation and prevent active phase degradation during the CO 2 reduction reaction (CO 2 RR), however, remains a significant challenge. Herein, we developed an interfacial engineering strategy to build a new SnO x catalyst by invoking multiscale approaches. This catalyst features a hierarchically nanoporous structure coated with an organic F-monolayer that modifies the triple-phase interface in aqueous electrolytes, substantially reducing competing hydrogen generation (less than 5%) and enhancing CO 2 RR selectivity (~90%). This rationally designed triple-phase interface overcomes the issue of limited CO 2 solubility in aqueous electrolytes via proactive CO 2 capture and reduction. Concurrently, we utilized pulsed square-wave potentials to dynamically recover the active phase for the CO 2 RR to regulate the production of C1 products such as formate and carbon monoxide (CO). This protocol ensures profoundly enhanced CO 2 RR selectivity (~90%) compared with constant potential (~70%) applied at -0.8 V (V vs RHE). We further achieved a mechanistic understanding of the CO 2 capture and reduction processes under pulsed square-wave potentials via in situ Raman spectroscopy, thereby observing the potential-dependent intensity of Raman vibrational modes of the active phase and CO 2 RR intermediates. Finally, this work will inspire material design strategies by leveraging triple-phase interface engineering for emerging electrochemical processes, as technology moves toward electrification and decarbonization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2018

Prognostic Emissions in GEOS

Prognostic emissions enable seamless applications of atmospheric chemistry and aerosol models across scales. Prognostic emissions also facilitate direct and higher order interactions and feedbacks between components in an integrated modeling system and thus enhance the model representativeness. On the other hand they also require more attention and strict validation to ensure model integrity. In this talk I will discuss recent developments related to prognostic emissions of mineral dust, primary marine aerosols and biomass burning in the NASA GEOS model and outline some of the challenges stemming from limited ability to represent subscale and stochastic processes.

Darmenov, Anton↗
DOE OSTI2023

Boundary Layer Controls on the Shallow-to-Deep Cumulus Transition (Final Technical Report)

This project advanced our understanding of the processes governing cumulus cloud formation and provides an improved observational basis for validating earth system models. To be specific, the project used laser- and radar-remote sensors to examine the physical properties of updrafts that rise from earth’s surface and initiate clouds deeper in the atmosphere. These updrafts comprise “thermals” and “plumes” and occur at small spatial and temporal scales (e.g., 10s of minutes, 100s of meters). These small scales preclude explicit representation in most earth system and climate models, and thus necessitate “sub-grid-scale” parameterization of updraft processes. The innovation of this project was to directly measure the size, shape, strength and water vapor content of these updrafts with Doppler and Raman lidars, respectively, and to link these updraft properties to cloud processes using vertically pointed weather radars. The resulting data sets comprise 100s of thousands of updrafts and thousands of clouds, which far exceeds previous efforts, and thereby provides a robust statistical and physical representation of these processes. From these large datasets the project produced a sequence of scientific analyses that: (1) Elucidate how variations in the turbulent structure of the convective boundary layer control shallow cumulus convection, (2) Quantify the upward transport of water vapor to cloud base via thermals and plumes, (3) Validate large-eddy simulations of updrafts and shallow convective clouds, (4) Demonstrate a size-to-strength relationship between updraft width and updraft speed, and (5) Demonstrate how updrafts interact with the stability at the top of the convective boundary layer to modulate the depth and vigor of convective clouds. These results have been disseminated via several published journal articles, academic theses, and conference presentations. Collectively these results contribute to the Atmospheric System Research (ASR) program’s goal to “improve understanding of the key cloud, aerosol, precipitation, and radiation processes that affect the Earth’s radiative balance and hydrological cycle, particularly processes that limit the predictive ability of regional and global earth system models”.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1998

Towards quantifying mesoscale flows in the troposphere using Raman lidar and Sondes

Water vapor plays an important role in the energetics of the boundary layer processes which in turn play a key role in regulating regional and global climate. It plays a primary role in Earth's hydrological cycle, in radiation balance as a direct absorber of infrared radiation, and in atmospheric circulation as a latent heat energy source, as well as in determining cloud development and atmospheric stability. Water vapor concentration, expressed as a mass mixing ratio (g kg(exp -l)), is conserved in all meteorological processes except condensation and evaporation. This property makes it an ideal choice for studying many of the atmosphere's dynamic features. Raman scattering measurements from lidar also allow retrieval of water vapor mixing ratio profiles at high temporal and vertical resolution. Raman lidars sense water vapor to altitudes not achievable with towers and surface systems, sample the atmosphere at much higher temporal resolution than radiosondes or satellites, and do not require strong vertical gradients or turbulent fluctuations in temperature that is required by acoustic sounders and radars. Analysis of highly-resolved water vapor profiles are used here to characterize two important mesoscale flows: thunderstorm outflows and a cold front passage. The data were obtained at the Atmospheric Radiation Measurement Site (CART) by the groundbased Department of Energy/Sandia National Laboratories lidar (CART Raman lidar or CARL) and Goddard Space Flight Center Scanning Raman Lidar (SRL). A detailed discussion of the SRL and CARL performance during the IOPs is given by others in this meeting.

Demoz, B.↗
DOE OSTI2022

SERS-based ssDNA composition analysis with inhomogeneous peak broadening and reservoir computing

Surface-enhanced Raman spectroscopy employed in conjunction with post-processing machine learning methods is a promising technique for effective data analysis, allowing one to enhance the molecular and chemical composition analysis of information rich DNA molecules. In this work, we report on a room temperature inhomogeneous broadening as a function of the increased adenine concentration and employ this feature to develop one-dimensional and two dimensional chemical composition classification models of 200 long single stranded DNA sequences. Afterwards, we develop a reservoir computing chemical composition classification scheme of the same molecules and demonstrate enhanced performance that does not rely on manual feature identification.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Exploring Mixed Ionic–Electronic-Conducting PVA/PEDOT:PSS Hydrogels as Channel Materials for Organic Electrochemical Transistors

Here, we report the preparation and evaluation of PVA/PEDOT:PSS-conducting hydrogels working as channel materials for OECT applications, focusing on the understanding of their charge transport and transfer properties. Our conducting hydrogels are based on crosslinked PVA with PEDOT:PSS interacting via hydrogen bonding and exhibit an excellent swelling ratio of ~180–200% w/w. Our electrochemical impedance studies indicate that the charge transport and transfer processes at the channel material based on conducting hydrogels are not trivial compared to conducting polymeric films. The most relevant feature is that the ionic transport through the swollen hydrogel is clearly different from the transport through the solution, and the charge transfer and diffusion processes govern the low-frequency regime. In addition, we have performed in operando Raman spectroscopy analyses in the OECT devices supported by first-principle computational simulations corroborating the doping/de-doping processes under different applied gate voltages. The maximum transconductance (gm~1.05 μS) and maximum volumetric capacitance (C*~2.3 F.cm -3 ) values indicate that these conducting hydrogels can be promising candidates as channel materials for OECT devices.

36 MATERIALS SCIENCE↗
NASA NTRS1987

Amorphous silicon deposition diagnostics using coherent anti-Stokes Raman spectroscopy

This paper reports on an in situ silicon deposition process diagnostics, using CARS performed at state-of-the-art a-Si:H film deposition conditions in a reactor designed for a-Si:H solar cell fabrication. The diagnostics procedure measures the silane depletion in an RF plasma as a function of the silane flow rate (where the relationship is linear between 50-percent depletion, at a flow rate of 5.6 sccm, and about 8-percent depletion, at 80 sccm) and the RF power (where the silane depletion is linearly dependent on the RF power in the region of 4 to 12 W). The linear RF power dependence of the silane depletion is considered to be consistent with the mechanism of silane decomposition primarily by electron impact dissociations, while the flow rate dependence is interpreted in terms of the residence time of the SiH4 molecules in the glow discharge region, where an increase of the residence time at a low flow rate results in a high depletion ratio.

Shing, Y. H.↗
NASA NTRS1992

Observation of intense Stokes and anti-Stokes lines in CH4 pumped by 355 nm of a Nd:YAG laser

The stimulated Raman scattering (SRS) and four-wave mixing (FWM) processes are studied in detail in CH4 gas pumped by the third-harmonic of Nd:YAG laser at 355 nm. The conversion efficiency and average output energy are measured for the various Stokes and anti-Stokes lines at different experimental conditions. The threshold input energy at various CH4 pressures is calculated for the unguided and capillary waveguide Raman cells. The calculated values for the capillary case are compared with the measured values at different CH4 pressures and the two results are in good agreement.

Sentrayan, K.↗
DOE OSTI2025

Raman Laser-Induced Structural Modification in CVD-Grown Monolayer MoS 2 for Multi-Purposed Nanofabrication

Molybdenum disulfide (MoS 2 ) has been extensively explored to be utilized as an electronic material in a variety of device applications. In particular, the tunability of MoS 2 enhances its electrical properties making it an intriguing candidate for field-effect transistors (FETs), while also extending beyond electrical properties to structural phase engineering. Laser-induced modifications, particularly with Raman lasers, offer a straightforward method to modulate materials via thermal processes with precise patterning control and energy-level flexibility. However, most studies on the modification of MoS 2 have focused on multilayered structures or have been conducted under low-power laser conditions, leaving the feasibility of structural modifications in monolayer MoS 2 elusive. In this study, we fundamentally elucidated the effects of high-power Raman laser irradiation on the surface of chemical vapor deposition (CVD)-grown monolayer MoS 2 under ambient conditions and uncovered the underlying mechanisms of laser-induced modifications by applying intense photon energy with highly interactive reactions. Our results revealed both etching and deposition phenomena in two discernible regions, and it can be demonstrated by intensity regimes based on the spatial distribution of laser irradiance within the laser-irradiated spot. Furthermore, phase transition was found to be inhibited due to the promoted oxidation and the deposition of hydrogenated amorphous carbon (a-C:H), and p-type doping was observed, likely occurring in the region beneath the a-C:H deposition as substitutional doping on the 2H phase of MoS 2 . To compare the thermal effects, MoS 2 modifications were further analyzed using simplified heat transfer estimations. In conclusion, these findings deepen our understanding of how Raman laser irradiation modifies MoS 2 under ambient conditions, providing guidelines for optimizing its modification processes.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Optical vibrational spectroscopic signatures of ammonium diuranate process parameters

Ammonium diuranate (ADU) is commonly encountered in the nuclear fuel cycle; however, previous investigations have shown that ADU is a complex mixture of distinct compounds. Moreover, production parameters are known to heavily influence the composition of the resulting ADU. Here, we examine four samples of ADU prepared at Oak Ridge National Laboratory (ORNL), and one sample of ADU made at Pacific Northwest National Laboratory (PNNL), with the goal of further characterizing and elucidating the effect of processing parameters such as stir rate, strike direction, and temperature on material composition. Process parameters during ADU precipitation at ORNL and PNNL were well documented, and we relate process variables to optical vibrational spectroscopic signatures observed using Raman and infrared (IR) spectroscopy. In addition, powder X-ray diffraction (PXRD) reveals differences in the solid-phase composition of ADU precipitates, but we find that the primary phase is similar to the uranyl oxyhydroxyhydrate mineral metaschoepite. Despite the significant phase contributions of a metaschoepite-like phase, spectroscopic evidence of both nitrate and ammonium are observed for all samples. To gain a more holistic understanding of spectroscopic features of process parameters in ADU, principal component analysis (PCA) is employed and results in observable signatures that relate to the stir rate used during synthesis. These results provide further information about the process-dependence of ADU precipitate composition.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1994

The Use of Spontaneous Raman Scattering for Hydrogen Leak Detection

A fiber optic probe has been built and demonstrated that utilizes back scattered spontaneous Raman spectroscopy to detect and identify gaseous species. The small probe, coupled to the laser and data acquisition equipment with optical fibers, has applications in gaseous leak detection and process monitoring. The probe design and data acquisition system are described. Raman scattering theory has been reviewed and the results of intensity calculations of hydrogen and nitrogen Raman scattering are given. Because the device is in its developmental stage, only preliminary experimental results are presented here. Intensity scans across the rotational-vibrational Raman lines of nitrogen and hydrogen are presented. Nitrogen at a partial pressure of 0.077 MPa was detected. Hydrogen at a partial pressure of 2 kPa approached the lower limit of detectability with the present apparatus. Potential instrument improvements that would allow more sensitive and rapid hydrogen detection are identified.

Degroot, Wim A.↗
DOE OSTI2023

Ethanol-fueled metal supported solid oxide fuel cells with a high entropy alloy internal reforming catalyst

High-performance metal supported solid oxide fuel cells (MS-SOFC) with an integrated high entropy alloy (HEA) internal reforming catalyst (IRC) are demonstrated for transportation applications using ethanol and methanol as fuels. Addition of the HEA IRC dramatically improves cell performance and stability when using ethanol/water blend fuel. Absence of carbon deposition predicted by thermodynamic calculations is confirmed by Raman spectroscopy analysis of posttest anodes. Optimal catalyst processing (deposition technique, loading, firing temperature) and cell operation conditions (flow rates, temperature, fuel compositions) are explored. Infiltrated HEA reforming catalyst provides a highly porous structure and low catalyst loading (6 mg cm –2 ). The designed structure and catalysts achieve small mass transport resistances in the fuel electrode (26.2 s m –1 ) and oxygen electrode (41.6 s m –1 ). The best ethanol concentration (60:40 v% ethanol: water) provides 0.83 W cm –1 at 700 °C, without carbon deposition. The ethanol-fueled MS-SOFC is operated for 500 h, including five thermal cycles. As a result, cell evolution is similar to that reported previously for hydrogen fuel; nickel aggregation and chromia deposition were the major observed changes, and carbon formation can be avoided even after long-term operation.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2020

Subthreshold Erosion of an Organic Polymer Induced by Multiple Shots of an X-Ray Free-Electron Laser

We report solids irradiated by energetic photons can be eroded in two modes, depending on the radiation intensity. High average, low-peak power sources, e.g., synchrotron radiation and high-order harmonics, induce desorption of the material at a low etch rate. In contrast, high-peak-power radiation from extreme ultraviolet and x-ray lasers usually causes a massive removal of the material even by a single shot. In this contribution, an effective material erosion is reported in PMMA exposed to multiple accumulated pulses generated by the free-electron x-ray-laser Linac Coherent Light Source (LCLS, tuned at a photon energy of 830 eV in this study, operated in Menlo Park at Stanford, CA, USA) at a fluence below the single-pulse ablation threshold. The effect is caused by polymer-chain scissions initiated by single photons carrying enough energy to break the C—C bounds. High efficiency of the erosion is supposed to occur due to a correlation of the single-photon effects. The subthreshold damage exhibits a nonlinear dose dependence resulting from a competition between chain scissions and cross-linking processes. The cross-linking is proven by Raman spectroscopy of the irradiated polymer. Two theoretical models of the x-ray free-electron-laser-induced erosion are suggested, which provide an excellent agreement with the experimental results.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS2008

Demonstration of Aerosol Property Profiling by Multi-wavelength Lidar Under Varying Relative Humidity Conditions

The feasibility of using a multi-wavelength Mie-Raman lidar based on a tripled Nd:YAG laser for profiling aerosol physical parameters in the planetary boundary layer (PBL) under varying conditions of relative humidity (RH) is studied. The lidar quantifies three aerosol backscattering and two extinction coefficients and from these optical data the particle parameters such as concentration, size and complex refractive index are retrieved through inversion with regularization. The column-integrated, lidar-derived parameters are compared with results from the AERONET sun photometer. The lidar and sun photometer agree well in the characterization of the fine mode parameters, however the lidar shows less sensitivity to coarse mode. The lidar results reveal a strong dependence of particle properties on RH. The height regions with enhanced RH are characterized by an increase of backscattering and extinction coefficient and a decrease in the Angstrom exponent coinciding with an increase in the particle size. We present data selection techniques useful for selecting cases that can support the calculation of hygroscopic growth parameters using lidar. Hygroscopic growth factors calculated using these techniques agree with expectations despite the lack of co-located radiosonde data. Despite this limitation, the results demonstrate the potential of multi-wavelength Raman lidar technique for study of aerosol humidification process.

Whiteman, D.N.↗
NASA NTRS1999

Fine Structure of the Low-Frequency Raman Phonon Bands of Single-Wall Carbon Nanotubes

The Raman spectra of singled-wall carbon nanotubes (SWNT) produced by laser and are process were studied between 5 and 500 kappa. The line width vs. temperature dependence of the low-frequency Raman bands between 150 and 200/ cm deviates from that expected for phonon decay through phonon-phonon scattering mechanism. The experimental results and their analysis provided convincing evidence that each of the low-frequency Raman lines is a superposition of several narrower Raman lines corresponding to tubes of nearly the same diameter. The application of Raman spectroscopy to probe the distribution of SWNT by both diameter and chirality is discussed.

Iliev, M. N.↗
DOE OSTI2026

Pitfalls in parameters: practical process development in chemical vapor processing of SiC

Vapor processing of high-value materials, such as silicon carbide (SiC), is of interest for many industries, including aerospace and energy production. Chemical vapor infiltration (CVI) of additively manufactured components is an especially attractive manufacturing process currently in development. Here, a novel development workflow is demonstrated with the H 2 –CH 3 SiCl 3 gas system for SiC to accelerate the process optimization of CVI SiC. A combination of calculated thermodynamics and high-throughput experimental chemical vapor deposition (CVD) coatings substantially reduced the experiments required with slow CVI processes. The computational results accurately predicted changes in the thermodynamic conditions tested, while CVD coatings – characterized by Raman spectroscopy – addressed changes in kinetic parameters. This workflow is also applicable to other vapor-processing systems, such as pyrolytic carbon, ZrC, or Si 3 N 4 .

Lamm, Benjamin W. [Oak Ridge National Laboratory (↗
NASA NTRSDate not supplied

Potential Discovery of Amphibole in Miller Range (MIL) 090292 via Raman Spectroscopy

Ungrouped carbonaceous chondrites have the potential to provide insights into processes on their parent bodies that may not be accessible through studying established groups. Miller Range (MIL) 090292 is an extensively aqueously altered ungrouped carbonaceous chondrite, which provides the potential to reveal new information about alteration processes on carbonaceous chondrite-like asteroids. The meteorite MIL090292 was initially classified as a CR1 chondrite. It experienced heavy aqueous alteration and, texturally, the meteorite is highly brecciated. MIL 090292 was reclassified as a C1 ungrouped chondrite after it was found that the Δ17O values of its magnetite grains do not plot along the CR mixing line. Furthermore, there is a lack of calcium carbonate grains in the sample, which are common in aqueously altered CRs –calcium is found in andradite and hedenbergite (which are not found in CRs) and phosphates. However, beyond this basic mineralogical information, there is a lack of knowledge about the petrogenetic history of the meteorite or its parent body.

Meteorite↗