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DOE OSTI2024

Measurement of coherent vibrational dynamics with X-ray Transient Absorption Spectroscopy simultaneously at the Carbon K- and Chlorine L 2,3 - edges

X-ray Transient Absorption Spectroscopy (XTAS) is a powerful probe for ultrafast molecular dynamics. The evolution of XTAS signal is controlled by the shapes of potential energy surfaces of the associated core-excited states, which are difficult to directly measure. Here, we study the vibrational dynamics of Raman activated CCl 4 with XTAS targeting the C 1s and Cl 2p electrons. The totally symmetric stretching mode leads to concerted elongation or contraction in bond lengths, which in turn induce an experimentally measurable red or blue shift in the X-ray absorption energies associated with inner-shell electron excitations to the valence antibonding levels. The ratios between slopes of different core-excited potential energy surfaces (CEPESs) thereby extracted agree very well with Restricted Open-Shell Kohn-Sham calculations. The other, asymmetric, modes do not measurably contribute to the XTAS signal. The results highlight the ability of XTAS to reveal coherent nuclear dynamics involving < 0.01 Å atomic displacements and also provide direct measurement of forces on CEPESs.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Si Microwire-Array Photocathodes Decorated with Cu Allow CO 2 Reduction with Minimal Parasitic Absorption of Sunlight

High loadings of Cu were integrated on the light-facing side of Si microwire arrays used under simulated sunlight for the photoelectrochemical reduction of CO 2 (aq) to hydrocarbons in 0.10 M KHCO 3 (aq). Radial-junction n + p-Si microwire arrays decorated with Cu exhibited absolute photocurrent densities comparable to an uncovered Si surface. Moreover, with respect to a Cu foil electrode, the positive shift in the onset potential for hydrocarbon formation at n + p-Si/Cu microwire arrays was equal to or greater than the photovoltage of the semiconductor alone. Selective electrodeposition of Cu on the tips and sidewalls of Si microwires was responsible for the minimal parasitic reflection and absorption exhibited by the catalyst, such that light-limited, absolute current densities >25 mA·cm –2 were sustained for 48 h under simulated sunlight. Photoelectrodes prepared from semiconductors with low diode quality factors and electrocatalysts with large Tafel slopes are shown to benefit from increased microstructured surface area. Si microwire arrays are thus suitable for photoelectrochemical reactions requiring high loadings of metallic and reflective electrocatalysts.

25 ENERGY STORAGE↗

NASA NTRS1975

Basic research and data analysis for the earth and ocean physics applications program and for the National Geodetic Satellite program

Data acquisition using single image and seven image data processing is used to provide a precise and accurate geometric description of the earth's surface. Transformation parameters and network distortions are determined, Sea slope along the continental boundaries of the U.S. and earth rotation are examined, along with close grid geodynamic satellite system. Data are derived for a mathematical description of the earth's gravitational field; time variations are determined for geometry of the ocean surface, the solid earth, gravity field, and other geophysical parameters.

Source record↗

NASA NTRS2008

Landing Site Dispersion Analysis and Statistical Assessment for the Mars Phoenix Lander

The Mars Phoenix Lander launched on August 4, 2007 and successfully landed on Mars 10 months later on May 25, 2008. Landing ellipse predicts and hazard maps were key in selecting safe surface targets for Phoenix. Hazard maps were based on terrain slopes, geomorphology maps and automated rock counts of MRO's High Resolution Imaging Science Experiment (HiRISE) images. The expected landing dispersion which led to the selection of Phoenix's surface target is discussed as well as the actual landing dispersion predicts determined during operations in the weeks, days, and hours before landing. A statistical assessment of these dispersions is performed, comparing the actual landing-safety probabilities to criteria levied by the project. Also discussed are applications for this statistical analysis which were used by the Phoenix project. These include using the statistical analysis used to verify the effectiveness of a pre-planned maneuver menu and calculating the probability of future maneuvers.

Bonfiglio, Eugene P.↗

DOE OSTI2020

Direct Demonstration of Unified Brønsted-Evans-Polanyi Relationships for Proton-Coupled Electron Transfer Reactions on Transition Metal Surfaces

Brønsted-Evans-Polanyi (BEP) relationships, which relate elementary reaction barriers to reaction thermodynamics, have long been discussed in electrochemical science, but demonstration of their existence in heterogeneous electrocatalysis, across many different catalyst surfaces and voltages, is lacking. In this contribution, the BEP model is demonstrated to describe both multiple catalyst surfaces and variable voltages in electrochemical environments. For proton-coupled electron transfer (PCET) to surface nitrogen (N*) and nitric oxide (NO*), reaction energies and activation barriers are calculated using Density Functional Theory (DFT) on a parallel plate capacitor model at three different potentials and for nine different transition metal surfaces. Linear BEP relations that describe all potentials and catalyst surfaces are obtained for these elementary reactions, and the slopes of the correlations are shown to be directly related to the fractional coordinate of the transition states (FCTS) of the reactions. The results, which are explained in terms of Marcus Theory, prove a direct equivalence between unified BEP coefficients, describing both variable catalyst surfaces and voltages, and electrochemical symmetry factors and provide a straightforward means of estimating this quantify for PCET reactions on transition metal surfaces. The resulting relationships, in turn, could lead to predictions of electrocatalytic reactivity trends of enhanced accuracy and efficiency.

Electrochemistry↗

DOE OSTI2016

The Influence of Fe Substitution in Lanthanum Calcium Cobalt Oxide on the Oxygen Evolution Reaction in Alkaline Media

The effect due to systematic substitution of cobalt by iron in La 0.6 Ca 0.4 Co 1-x Fe x O 3 towards the oxygen evolution reaction(OER) in alkaline media has been investigated. We synthesized these compounds by a facile glycine-nitrate synthesis and the phase formation was confirmed by X-ray diffraction and Neutron Diffraction elemental analysis. The apparent OER activity was evaluated by quasi steady state current measurements in alkaline media using a traditional three-electrode cell. X-ray photoelectron spectroscopy shows iron substitution causes an increase in the surface concentration of various cobalt oxidation states. Tafel slope in the vicinity of 60 mV/decade and electrochemical reaction order towards OH- near unity were achieved for the unsubstituted La 0.6 Ca 0.4 CoO 3 . Moreover, a decrease in the Tafel slope to 49 mV/decade was observed when iron is substituted in high amounts in the perovskite structure. The area specific current density showed dependence on the Fe fraction, however the relationship of specific current density with Fe fraction is not linear. High Fe substitutions, La 0.6 Ca 0.4 Co 0.2 Fe 0.8 O 3 and La 0.6 Ca 0.4 Co 0.1 Fe 0.9 O 3 showed higher area specific activity towards OER than La 0.6 Ca 0.4 CoO 3 or La 0.6 Ca 0.4 FeO 3 . Finally, we believe iron inclusion in the cobalt sites of the perovskite helps decrease the electron transfer barrier and facilitates the formation of cobalt-hydroxide at the surface. Possible OER mechanisms based on the observed kinetic parameters will be discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1989

Multicolor surface photometry of powerful radio galaxies. II - Morphology and stellar content

Results on the morphology, photometric structure, and colors of 72 powerful radio galaxies (PRGs) are presented. It is found that galaxy interactions and mergers play an important role in the PRG phenomenon. Over 50 percent of the sample galaxies display optical morphological deviations from elliptical symmetry at high levels of surface brightness. About 20 percent of the galaxies have a second nucleus less than 10 kpc in projection from the main nucleus. The fraction of PRGs in a common envelope with neighboring galaxies is even larger. Surface brightness profiles for galaxies with weak or no emission lines are typically shallower in slope than normal radio-quiet elliptical galaxies, but similar to the brightest cluster galaxies. Surface brightness profiles for strong emission (SE) galaxies are more diverse in form. The SE PRGs have unusually blue average colors relative to giant elliptical galaxies. These colors are spatially extended and not merely due to light from a bright nucleus or extended emission-line gas.

Smith, Eric P.↗

NASA NTRS1980

Optical image and laser slope meter intercomparisons of high-frequency waves

Spectral analyses of optical images of the ocean surface, obtained by a digital video system, are presented and compared with wave data measured simultaneously by the JPL Waverider-mounted laser slope meter. The image analyses, which incorporate several new ideas, provide two-dimensional wave number spectra of slope, covering wavelengths from 10 cm to 10 m. These slope spectra are converted to wave height spectra by a new technique which includes the effects of sky radiance gradients. Space-time spectra are also presented for waves whose frequencies are less than 2 Hz. The JPL slope frequency spectra are compared with image wave number spectra which have been converted to frequency spectra by use of the gravity wave dispersion relation. Results of comparisons between the frequency spectra obtained from the two different measurements show reasonable agreement for frequencies less than 3 Hz.

Lubard, S. C.↗

NASA NTRS1992

Distribution of Reynolds stress carried by mesoscale variability in the Antarctic Circumpolar Current

Satellite altimeter data collected by the Geosat Exact Repeat Mission were used to investigate turbulent stress resulting from the variability of surface geostrophic currents in the Antarctic Circumpolar Current. The altimeter measured sea level along the subsatellite track. The variability of the along-track slope of sea level is directly proportional to the variability of surface geostrophic currents in the cross-track direction. Because the grid of crossover points is dense at high latitudes, the satellite data could be used for mapping the temporal and spatial variability of the current. Two and a half years of data were used to compute the statistical structure of the variability. The statistics included the probability distribution functions for each component of the current, the time-lagged autocorrelation functions of the variability, and the Reynolds stress produced by the variability. The results demonstrate that stress is correlated with bathymetry. In some areas the distribution of negative stress indicate that eddies contribute to an acceleration of the mean flow, strengthening the hypothesis that baroclinic instability makes important contributions to strong oceanic currents.

Johnson, Thomas J.↗

NASA NTRS1993

Geology and surface characteristics of Bell Regio, Venus

Bell Regio is a broad topographic rise located at approximately 30 deg N, 45 deg E which extends approximately 1500 km in the N-S direction and is characterized by extensive volcanism. The geology and surface characteristics of Bell Regio are examined in order to understand the geologic evolution of the region and the surface characteristics of the major volcanic units. Relationships between Magellan SAR backscatter values and altimeter-derived ring slope data are analyzed, and terrestrial SAR data are used to suggest possible surface morphologies.

Campbell, Bruce A.↗

NASA NTRS1995

Distribution and nature of UV absorbers on Triton's surface

Substantial evidence suggests that a UV spectrally Absorbing Material (UV-SAM) exists on Triton's surface. This evidence is found in the positive slope in Triton's spectrum from the UV to the near-IR, and the increasing contrast in Triton's light curve in the blue and UV. Although it is now widely-thought that UV-SAMs exist on Triton, little is known about their distribution and spectral properties. The goal of this NDAP Project is to determine the spatial distribution and geological context of the UV-SaM material. We hope to determine if UV-SAMs on Triton are correlated with geologic wind streaks, craters, calderas, geomorphic/topographic units, regions containing (or lacking) volatile frosts, or some other process (e.g., magnetospheric interactions). Once the location and distribution of UV-SAMs has been determined, further constraints on their composition cable made by analyzing the spectrographic data set. To accomplish these goals, various data sets will be used, including Voyager 2 UV and visible images of Triton's surface, IUE and HST spectra of Triton, and a geologic map of the surface based on voyager 2 and spectrophotometric data. The results of this research will be published in the planetary science literature.

Stern, S. Alan↗

NASA NTRS1994

Distribution and nature of UV absorbers on Triton's surface

Substantial evidence suggests that a UV Spectrally Absorbing Material (UV-SAM) exists on Triton's surface. This evidence is found in the positive slope in Triton's spectrum from the UV to the near-IR, and the increasing contrast in Triton's light curve in the blue and UV. Although it is now widely-thought that UV-SAM's exist on Triton, little is known about their distribution and spectral properties. The goal of this NDAP Project is to determine the spatial distribution and geological context of the UV-SAM material. We hope to determine if UV-SAM's on Triton are correlated with geologic wind streaks, craters, calderas, geomorphic/topographic units, regions containing (or lacking) volatile frosts, or some other process (e.g., magnetospheric interactions). Once the location and distribution of UV-SAM's has been determined, further constraints on their composition can be made by analyzing the spectrographic data set. To accomplish these goals, various data sets will be used, including Voyager 2 UV and visible images of Triton's surface, IUE and HST spectra of Triton, and a geologic map of the surface based on Voyager 2 and spectrophotometric data. The results of this research will be published in the planetary science literature.

Stern, S. Alan↗

NASA NTRS1995

Distribution and nature of UV absorbers on Trition's surface

Substantial evidence suggests that a UV (ultraviolet) Spectrally Absorbing Material (UV-SAM) exists on Triton's surface. This evidence is found in the positive slope in Triton's spectrum from the UV to the near-IR, and the increasing contrast in Triton's light curve in the blue and UV. Although it is now widely-thought that UV-SAM's exist on Triton, little is known about their distribution and spectral properties. The goal of this NDAP Project is to determine the spatial distribution and geological context of the UV-SAM material. We hope to determine if UV-SAM's on Triton are correlated with geologic wind streaks, craters, calderas, geomorphic/topographic units, regions containing (or lacking) volatile frosts, or some other process (e.g., magnetospheric interactions). Once the location and distribution of UV-SAM's has been determined, further constraints on their composition can be made by analyzing the spectrographic data set. To accomplish these goals, various data sets will be used, including Voyager 2 UV and visible images of Triton's surface, IUE and HST spectra of Triton, and a geologic map of the surface based on Voyager 2 and spectrophotometric data. The results of this research will be published in the planetary science literature.

Stern, S. Alan↗

DOE OSTI2017

Dome of magnetic order inside the nematic phase of sulfur-substituted FeSe under pressure

The pressure dependence of the structural, magnetic, and superconducting transitions and of the superconducting upper critical field were studied in sulfur-substituted Fe ( Se 1 - x S x ) . We performed resistance measurements on single crystals with three substitution levels ( x = 0.043 , 0.096, 0.12) under hydrostatic pressures up to 1.8 GPa and in magnetic fields up to 9 T and were compared to data on pure FeSe. Our results illustrate the effects of chemical and physical pressure on Fe ( Se 1 - x S x ). Furthermore, on increasing sulfur content, magnetic order in the low-pressure range is strongly suppressed to a small domelike region in the phase diagrams. But, T s is much less suppressed by sulfur substitution, and T c of Fe ( Se 1 - x S x ) exhibits similar nonmonotonic pressure dependence with a local maximum and a local minimum present in the low-pressure range for all x . The local maximum in T c coincides with the emergence of the magnetic order above T c . At this pressure the slope of the upper critical field decreases abruptly, which may indicate a Fermi-surface reconstruction. The minimum of T c correlates with a broad maximum of the upper critical field slope normalized by T c .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Interferometric SAR modelling of near surface data to improve geological model in the Surat Basin, Australia

Here we present a study on geophysical inverse modelling for subsurface structural properties of an unconventional hydrocarbon site that was monitored previously by Interferometric Synthetic Aperture Radar (InSAR) technology for surface deformation. A static three-dimensional geomodel along with extracted property maps replicates the depth of each underlying stratigraphic unit and structural feature with the density of each geological layer. We examine the hypothesis that integration of elastic properties of each formation layer with InSAR observations in a stratified elastic medium will lead to a viscoelastic geophysical inverse problem that can be solved to estimate fractional volume change at the reservoir level. Moreover, we examine synthetic scenarios in which the elastic properties of the formations are perturbed before determining the resulting impact on the rate of surface deformation. The results show that although the slope of underlying formations, their density and depth can define the extent and pattern of a deformation signal, their properties have a marginal impact on volumetric change compared to the dense network of shallow depth Coal Seam Gas (CSG) mining wells. Besides, it is also demonstrated that the inversion of InSAR deformation maps can resolve the uncertainties associated with low-resolution seismic interpretation as well as filling the data gaps within seismic acquisitions. A significant contribution of this investigation to the geological basin modelling involves a) introducing a remote and non-invasive technology such as InSAR to improve geophysical mapping of subsurface structures such as faults in areas with sparse or no reflective seismic information, and b) applying a multi-layer viscoelastic geophysical source model for an unconventional hydrocarbon reservoir such as CSG.

58 GEOSCIENCES↗

DOE OSTI2024

Field, frequency, and temperature dependencies of the surface resistance of nitrogen diffused niobium superconducting radio frequency cavities

We investigate the rf performance of several single-cell superconducting radio-frequency cavities subjected to low temperature heat treatment in nitrogen environment. The cavities were treated at temperature 120 – 165 ° C for an extended period of time (24–48 h) either in high vacuum or in a low partial pressure of ultrapure nitrogen. The improvement in Q 0 with a Q rise was observed when nitrogen gas was injected at ∼ 300 ° C during the cavity cooldown from 800 ° C and held at 165 ° C , without any degradation in accelerating gradient over the baseline performance. The treatment was applied to several elliptical cavities with frequency ranging from 0.75 to 3.0 GHz, showing an improved quality factor as a result of low temperature nitrogen treatments. The Q rise feature is similar to that achieved by nitrogen alloying Nb cavities at higher temperature, followed by material removal by electropolishing. The surface modification was confirmed by the change in electronic mean free path and tuned with the temperature and duration of heat treatment. The decrease of the temperature-dependent surface resistance with increasing rf field, resulting in a Q rise, becomes stronger with increasing frequency and decreasing temperature. The data suggest a crossover frequency of ∼ 0.95 GHz above that the Q rise phenomenon occurs at 2 K. Some of these results can be explained qualitatively with an existing model of intrinsic field-dependence of the surface resistance with both equilibrium and nonequilibrium quasiparticle distribution functions. The change in the Q slope below 0.95 GHz may result from masking contribution of trapped magnetic flux to the residual surface resistance. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗

NASA NTRS2016

Characterization of the High-Albedo NEA 3691 Bede

Characterization of NEAs provides important inputs to models for atmospheric entry, risk assessment and mitigation. Diameter is a key parameter because diameter translates to kinetic energy in atmospheric entry. Diameters can be derived from the absolute magnitude, H(PA=0deg), and from thermal modeling of observed IR fluxes. For both methods, the albedo (pv) is important - high pv surfaces have cooler temperatures, larger diameters for a given Hmag, and shallower phase curves (larger slope parameter G). Thermal model parameters are coupled, however, so that a higher thermal inertia also results in a cooler surface temperature. Multiple parameters contribute to constraining the diameter. Observations made at multiple observing geometries can contribute to understanding the relationships between and potentially breaking some of the degeneracies between parameters. We present data and analyses on NEA 3691 Bede with the aim of best constraining the diameter and pv from a combination of thermal modeling and light curve analyses. We employ our UKIRT+Michelle mid-IR photometric observations of 3691 Bede's thermal emission at 2 phase angles (27&43 deg 2015-03-19 & 04-13), in addition to WISE data (33deg 2010-05-27, Mainzer+2011). Observing geometries differ by solar phase angles and by moderate changes in heliocentric distance (e.g., further distances produce somewhat cooler surface temperatures). With the NEATM model and for a constant IR beaming parameter (eta=constant), there is a family of solutions for (diameter, pv, G, eta) where G is the slope parameter from the H-G Relation. NEATM models employing Pravec+2012's choice of G=0.43, produce D=1.8 km and pv≈0.4, given that G=0.43 is assumed from studies of main belt asteroids (Warner+2009). We present an analysis of the light curve of 3691 Bede to constrain G from observations. We also investigate fitting thermophysical models (TPM, Rozitis+11) to constrain the coupled parameters of thermal inertia (Gamma) and surface roughness, which in turn affect diameter and pv. Surface composition can be related to pv. This study focuses on understanding and characterizing the dependency of parameters with the aim of constraining diameter, pv and thermal inertia for 3691 Bede.

Wooden, Diane H.↗

NASA NTRS2016

Characterization of the High-Albedo NEA 3691 Bede

magnitude↗