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At least 1,207 records · Page 67
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Reduction of spectral interferences and noise effects in laser ablation molecular isotopic spectrometry with partial least square regression – a computer simulation study

The fundamental analytical accuracies and precisions attainable by laser ablation molecular isotopic spectrometry (LAMIS), with emphasis on the impacts from spectral interferences and measurement noise, were investigated by means of computer simulation. The study focused on the analysis of a minor isotope at sub- to single-percentage abundance level. With a natural abundance about 1.1% for 13 C, the C 2 Swan band (d 3 II g - a 3 II u ) with Δν = + 1 was selected as a representative system. The characteristics (e.g., noise amplitude and distribution, signal strength, and signal-to-background ratio) of the simulated spectra were experimentally characterized. Partial least square (PLS) regression was used to extract isotopic information from the simulated molecular spectra. In the absence of any spectral interference and with the use of a calibration set consisting of eleven isotopic standards, the theoretical accuracies and precisions with signal accumulation from 100 laser shots are about 0.002% and 0.001%, respectively, in absolute percentage abundance of 13 C. The theoretical analytical accuracies slightly degrade, but are adequate for many applications, to 0.004% and 0.008% respectively, for calibrations involving only three and two isotopic standards. It was found that PLS regression is not only immune to both source-flicker and photon-shot noise, but is also effective in differentiating the spectral patterns from the analyte against those from spectral interferences. The influences of spectral interference from single or multiple atomic emission lines were simulated, and new ways to minimize their impacts were formulated and demonstrated. It was found that the wavelength range selected for the computation of the normalization factor should not contain any spectral-interfering peak, and a properly chosen wavelength range increases the tolerance of spectral interference by at least one order of magnitude. With matrix-matched calibration standards, the precisions (expressed as RSDs of the determined 13 C isotopic abundances) degrade from ~ 1% in the absence of spectral interference, to ~ 3&#8240, 10&#8240 and 20&#8240 with multiple spectral-interfering peaks that are 10 ×, 100 × and 1000 ×, respectively, stronger than the molecular bandhead of the analyte. The study concluded that PLS regression is a powerful and indispensable tool for extraction of isotopic information from LAMIS spectra.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

The distribution of satellites around massive galaxies at 1 < z < 3 in ZFOURGE/CANDELS: Dependence on star formation activity

We study the statistical distribution of satellites around star-forming and quiescent central galaxies at 1 < z < 3 using imaging from the FourStar Galaxy Evolution Survey and the Cosmic Assembly Near-IR Deep Extragalactic Legacy Survey. The deep near-IR data select satellites down to log (M/M {sub ☉}) > 9 at z < 3. The radial satellite distribution around centrals is consistent with a projected Navarro-Frenk-White profile. Massive quiescent centrals, log (M/M {sub ☉}) > 10.78, have ∼2 times the number of satellites compared to star-forming centrals with a significance of 2.7σ even after accounting for differences in the centrals' stellar-mass distributions. We find no statistical difference in the satellite distributions of intermediate-mass quiescent and star-forming centrals, 10.48 < log (M/M {sub ☉}) < 10.78. Compared to the Guo et al. semi-analytic model, the excess number of satellites indicates that quiescent centrals have halo masses 0.3 dex larger than star-forming centrals, even when the stellar-mass distributions are fixed. We use a simple toy model that relates halo mass and quenching, which roughly reproduces the observed quenched fractions and the differences in halo mass between star-forming and quenched galaxies only if galaxies have a quenching probability that increases with halo mass from ∼0 for log (M{sub h} /M {sub ☉}) ∼ 11 to ∼1 for log (M{sub h} /M {sub ☉}) ∼ 13.5. A single halo-mass quenching threshold is unable to reproduce the quiescent fraction and satellite distribution of centrals. Therefore, while halo quenching may be an important mechanism, it is unlikely to be the only factor driving quenching. It remains unclear why a high fraction of centrals remain star-forming even in relatively massive halos.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Tunable Oxygen Reduction Electrocatalysis by Phenazine-Modified Carbons (Final Report)

This project aims to systematically investigate the fundamental interfacial chemistry that underlies the four-electron, four-proton oxygen reduction reaction (ORR) mediated by heteroatom-doped graphitic carbon electrodes. Heteroatom-doped (Fe, N, etc.) graphitic carbons have emerged as a rich class of materials that are promising ORR catalysts in low temperature fuel cells because of their earth-abundant elements, extremely low cost, environmental harmlessness, and high tolerance to impurities in the fuel stream. However, despite decades of research, systematic efforts to improve the activity, selectivity, and durability of these catalysts has been hampered both by a complex heterogeneous distribution of potential N- and Fe-dopant active sites and by the inability to tune the local electronic structure and environment of the active site with molecular precision. Understanding the fundamental chemistry that influences the turnover-limiting and selectivity determining steps for ORR and other multielectron/multiproton electrocatalytic transformations requires new and innovative methods to prepare heteroatom active sites with molecular precision on carbon surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

A comparison of Ti-6Al-4V in-situ alloying in Selective Laser Melting using simply-mixed and satellited powder blend feedstocks

Highlights: • Satelliting mixing is proposed for preparing powder feedstocks for AM. • Satelliting allows the creation of blended feedstocks of improved homogeneity. • Sample homogeneity is affected by particle size distribution and powder mixing technique. - Abstract: In-situ alloying within laser powder-bed fusion, specifically Selective Laser Melting (SLM), has been investigated for the formulation of novel alloys from elemental powders to extend the benefits offered by these technologies. Inadequate preparation of the powder feedstock prior to in-situ alloying can yield inhomogeneous microstructures, often deteriorating the mechanical performance of the deposited parts. The present work was designed to assess the use of the ‘satelliting’ method to create powder feedstocks for in-situ laser powder-bed fusion. The research was carried out on Ti-6Al-4V. Ti-6Al-4V feedstocks obtained by mixing or satelliting elemental powders were investigated and compared to a reference pre-alloyed material. The processability of the different feedstocks was assessed by comparing the microstructure of the deposits originating from the different powder blends. Results show that the powder percolation and particle size distribution of the feedstocks translate in deposited microstructures exhibiting different porosity, elemental segregation, and average grain size, revealing the impact of the powder blend characteristics on the laser energy absorbance and solidification of the alloy. This study provides fundamental insights of how to formulate powder feedstock and aims to support future research activities on the design and development of new alloys for use in powder-based additive manufacturing.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Precision measurement of transverse velocity distribution of a strontium atomic beam

We measure the transverse velocity distribution in a thermal Sr atomic beam precisely by velocity-selective saturated fluorescence spectroscopy. The use of an ultrastable laser system and the narrow intercombination transition line of Sr atoms mean that the resolution of the measured velocity can reach 0.13 m/s, corresponding to 90 μK in energy units. The experimental results are in very good agreement with the results of theoretical calculations. Based on the spectroscopic techniques used here, the absolute frequency of the intercombination transition of {sup 88}Sr is measured using an optical-frequency comb generator referenced to the SI second through an H maser, and is given as 434 829 121 318(10) kHz.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS2010

Coherent Frequency Reference System for the NASA Deep Space Network

The NASA Deep Space Network (DSN) requires state-of-the-art frequency references that are derived and distributed from very stable atomic frequency standards. A new Frequency Reference System (FRS) and Frequency Reference Distribution System (FRD) have been developed, which together replace the previous Coherent Reference Generator System (CRG). The FRS and FRD each provide new capabilities that significantly improve operability and reliability. The FRS allows for selection and switching between frequency standards, a flywheel capability (to avoid interruptions when switching frequency standards), and a frequency synthesis system (to generate standardized 5-, 10-, and 100-MHz reference signals). The FRS is powered by redundant, specially filtered, and sustainable power systems and includes a monitor and control capability for station operations to interact and control the frequency-standard selection process. The FRD receives the standardized 5-, 10-, and 100-MHz reference signals and distributes signals to distribution amplifiers in a fan out fashion to dozens of DSN users that require the highly stable reference signals. The FRD is also powered by redundant, specially filtered, and sustainable power systems. The new DSN Frequency Distribution System, which consists of the FRS and FRD systems described here, is central to all operational activities of the NASA DSN. The frequency generation and distribution system provides ultra-stable, coherent, and very low phase-noise references at 5, l0, and 100 MHz to between 60 and 100 separate users at each Deep Space Communications Complex.

Tucker, Blake C.↗
NASA NTRS1987

An interim reference model for the middle atmosphere water vapor distribution

Nimbus 7 LIMS data are used to determine monthly and seasonal zonal mean reference stratospheric profiles over selected latitude bands, and other ground and airborne microwave data are combined with the LIMS data to construct an interim reference profile from the tropopause to 80 km for the midlatitude region averaged over the winter and spring periods. The present profiles indicate the presence of a hygropause near 50 mb pressure in the tropics, a relatively constant mixing ratio distribution with a height of 4.7-5 ppmv in the midlatitude and high latitude stratosphere, and a decrease in the midlatitude mesosphere to 1 ppmv at about 80 km.

Russell, J. M., III↗
NASA NTRS1985

On the Latitudinal Distribution of Debris in the Northern Hemisphere of Mars

Examination of Mariner 9 images showed evidence of debris mantling on Mars. The evidence included craters that appeared to be filled with debris and an apparent lack of small craters. Based on such data, it was suggested that a circumpolar debris mantle exists poleward of about 30N and 30S latitudes. The presence of a debris layer has important implications for the modulation over time of atmospheric pressure by the cap-regolith-atmosphere system. Preliminary efforts in providing constraints on the thickness and distribution of debris are discussed. The initial approach is to examine crater size-frequency data for selected regions on Mars, later expanding the study to include an inventory of aeolian features and other direct indicators of debris deposition. The crater size-frequency distributions for ten regions between latitudes 20N and 80N and covering a range of longitudes were discovered. Crater data were derived from Viking Orbiter images with resolutions of between 26 and 75 meters/pixel.

Guinness, E. A.↗
DOE OSTI2015

MAPPING THE GALAXY COLOR–REDSHIFT RELATION: OPTIMAL PHOTOMETRIC REDSHIFT CALIBRATION STRATEGIES FOR COSMOLOGY SURVEYS

Calibrating the photometric redshifts of ≳10{sup 9} galaxies for upcoming weak lensing cosmology experiments is a major challenge for the astrophysics community. The path to obtaining the required spectroscopic redshifts for training and calibration is daunting, given the anticipated depths of the surveys and the difficulty in obtaining secure redshifts for some faint galaxy populations. Here we present an analysis of the problem based on the self-organizing map, a method of mapping the distribution of data in a high-dimensional space and projecting it onto a lower-dimensional representation. We apply this method to existing photometric data from the COSMOS survey selected to approximate the anticipated Euclid weak lensing sample, enabling us to robustly map the empirical distribution of galaxies in the multidimensional color space defined by the expected Euclid filters. Mapping this multicolor distribution lets us determine where—in galaxy color space—redshifts from current spectroscopic surveys exist and where they are systematically missing. Crucially, the method lets us determine whether a spectroscopic training sample is representative of the full photometric space occupied by the galaxies in a survey. We explore optimal sampling techniques and estimate the additional spectroscopy needed to map out the color–redshift relation, finding that sampling the galaxy distribution in color space in a systematic way can efficiently meet the calibration requirements. While the analysis presented here focuses on the Euclid survey, similar analysis can be applied to other surveys facing the same calibration challenge, such as DES, LSST, and WFIRST.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Dynamic development of geochemical reaction fronts during hydraulic stimulation of shale

Injection of acidic hydraulic fracture fluid (HFF) into shale formations for unconventional oil/gas production results in chemical reactions in the shale matrix that can alter fluid transport. Here, we report the results of set of experiments designed to evaluate the impact of calcite dissolution as a function of carbonate mineral content on matrix chemical reactivity and pore-space modification concomitant with imbibition. In this study, we tracked acidic HFF transport in four samples of Wolfcamp shale with calcite contents varying from 4% to 59% by monitoring the rate and spatial extent of bromide tracer transport using synchrotron-based X-ray fluorescence microprobe (XFM) imaging. Concurrently, we also carried out XFM imaging of the spatial distribution of Ca in the Wolfcamp shale cores (as a proxy of calcite distribution). Our approach thus yields a direct record of time-resolved selective ion transport resulting from the penetration of acidic HFF and the associated mineral transformations in the shale cores. We show that the variability in calcite content of Wolfcamp shale samples can directly affect the rate and spatial extent of imbibition. Although reaction of the acidic HFF with carbonates in shales enhances calcite dissolution and increases porosity, the spatial extent of calcite dissolution in the shale matrix is limited due to a rapid neutralization of pH. The relative abundance and spatial distribution of calcite control the chemical saturation state of the HFF progressing into the matrix. As a result, calcite has a major impact on the spatial extent and rate of matrix alteration and thus on HFF transport during subsurface reservoir stimulation. Consequently, increased calcite content in the shale matrix inhibits the spatial extent of the pore-volume increase and, by extension, the spatial extent and rate of imbibition. Our results thus show that the overall rates of calcite dissolution approach the rates of acidic HFF transport (i.e., Damköhler number ~1), which could contribute to the efficiency of subsurface reservoir stimulation. A better understanding of HFF-calcite reaction rates is crucial for improving the prediction and optimization of fluid transport across HFF-shale interfaces during hydraulic fracturing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Microwave-assisted conversion of methane over H-(Fe)-ZSM-5: Evidence for formation of hot metal sites

We report microwave-assisted catalysis offers great promise as an “intensified” technology for chemical processing. The present study investigates microwave-assisted direct conversion of methane with focus on the design and evaluation of microwave-sensitive H-(Fe)ZSM-5 catalysts for the existence of hotspot formation. Isomorphous substituted H-(Fe)ZSM-5 catalysts are tuned to identify key design parameters that control their microwave sensitivity. Increasing the amount of Al and Fe substitution in the zeolite lattice is found to result in higher microwave sensitivity due to improved dielectric properties and hence facilitated microwave heating of the catalyst bed. Comparison between the performance of these catalysts in a conventional thermally-heated (CH) fixed-bed and a microwave (MW) reactor allows identification of the effect of microwave irradiation on the catalyst activity. Methane conversion is drastically enhanced at MW conditions (from 3% at CH conditions to 40% at MW conditions), indicating accelerated methane activation over the metal site and hence suggesting a hot metal site despite much lower catalyst bulk temperature measured in the microwave reactor. The existence of metal hotspot formation is further supported by the reaction product distribution and spent catalyst analysis. At MW conditions, C 2 (ethane and ethylene) and coke (mainly carbon nanotubes and nanofibers) selectivity are much higher at the cost of aromatics make compared to CH conditions. This can be explained by reduced aromatization activity at the Brønsted acid sites of the zeolite due to its lower relative temperature of the zeolite. The much-enhanced metal aggregation observed in the spent catalyst from the MW reactor along with the distribution of coke species further confirms the existence of selective heating (i.e. hotspot formation) occurring at the active metal site in the catalyst at MW conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Migration of Al within dealuminated beta extruded catalysts influences olefin distribution during ethanol upgrading

Zeolites serve as essential catalytic platforms for many industrial processes, including emerging ethanol-to-olefins (ETO) upgrading technologies. Although metal-loaded (Cu, Zn, Y) dealuminated beta (deAlBeta) zeolite powders are promising catalysts for direct ETO conversion with high selectivity to butene-rich C3+ olefins necessary for production of sustainable aviation fuels (SAF), development of these materials as shaped technical bodies through the incorporation of binders is required for scale-up and commercial viability. Here, we report the ethanol upgrading performance of Cu-Zn-Y/deAlBeta extruded catalysts formulated with either alumina or kaolin clay binders. Both extrudates exhibit high ethanol dehydration reactivity which competes with the initial ethanol dehydrogenation step in the direct ETO reaction network. Consequently, elevated selectivity to dehydration side products (ethylene, diethyl ether) at ∼100% ethanol conversion is observed on Cu-Zn-Y/deAlBeta extrudates compared to the powder catalyst, which inhibits production of desired C3+ olefins. Utilizing microscopy and spectroscopic characterizations, we attribute this to Al migration from binder to zeolite particles within the extrudates, thus re-aluminating the zeolite and generating Brønsted acid sites active for dehydration reactions. This work elucidates the effects of binder incorporation on ETO product distributions and emphasizes that binder selection must be carefully considered during design of extruded zeolite catalysts.

Jacobs, Hunter [ORNL] (ORCID:000000016190874X)↗
NASA NTRS1988

Measurements of selected C2-C5 hydrocarbons in the troposphere - Latitudinal, vertical, and temporal variations

The tropospheric distribution of 1077 C2-C5 hydrocarbon samples was determined. Shipboard measurements obtained over the eastern Pacific Ocean reveal large north-to-south gradients for most nonmethane hydrocarbons (NMHCs). The results show that NMHC concentrations can decrease by a factor of two or more during the passage of cold fronts in winter and spring, and that upper tropospheric concentrations were lower than those in the lower troposphere.

Singh, Hanwant B.↗
NASA NTRS1994

Crustal Magnetic Anomalies

This Quadrennial Report departs in format from its predecessors.....we instead focus our discussion on only a few selected topics.

magnetization distributions↗
DOE OSTI2013

SATELLITES IN MILKY-WAY-LIKE HOSTS: ENVIRONMENT DEPENDENCE AND CLOSE PAIRS

Previous studies showed that an estimate of the likelihood distribution of the Milky Way (MW) halo mass can be derived using the properties of the satellites similar to the Large and Small Magellanic Clouds (LMC and SMC). However, it would be straightforward to interpret such an estimate only if the properties of the Magellanic Clouds (MCs) are fairly typical and are not biased by the environment. In this study, we explore whether the environment of the MW affects the properties of the SMC and LMC such as their velocities. To test for the effect of the environment, we compare velocity distributions for MC-sized subhalos around MW hosts in a sample selected simply by mass and in the second sample of such halos selected with additional restrictions on the distance to the nearest cluster and the local galaxy density, designed to mimic the environment of the Local Group (LG). We find that satellites in halos in the LG-like environments do have somewhat larger velocities, as compared to the halos of similar mass in the sample without environmental constraints. For example, the fraction of subhalos matching the velocity of the LMC is 23% {+-} 2% larger in the LG-like environments. We derive the host halo likelihood distribution for the samples in the LG-like environment and in the control sample and find that the environment does not significantly affect the derived likelihood. We use the updated properties of the SMC and LMC to derive the constraint on the MW halo mass of log(M{sub 200}/M{sub Sun }) = 12.06{sub -0.19}{sup +0.31} (90% confidence interval). We also explore the incidence of close pairs with relative velocities and separations similar to those of the LMC and SMC and find that such pairs are quite rare among {Lambda}CDM halos. Only 2% of halos in the MW mass range have a relatively close pair ({Delta}r < 40 kpc and {Delta}s < 160 km s{sup -1}) of subhalos with circular velocities v{sub circ} > 50 km s{sup -1}. Pairs with masses and separations similar to those of the LMC and SMC ({Delta}r{sub MC} = 23.4 {+-} 10 kpc and {Delta}s{sub MC} = 128 {+-} 32 km s{sup -1}) are found only in one out of Almost-Equal-To 30, 000 MW-sized halos. Interestingly, the halo mass likelihood distribution for host halos constrained to have MC-like close pairs of subhalos is quite different from the global likelihood from which the MW halo mass constraint discussed above was derived. Taking into account the close separation of the MCs in the Busha et al. method results in the shift of the MW halo mass estimate to smaller masses, with the peak shifting approximately by a factor of two.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2019

Successful Decontamination of 99 TcO 4 - in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets

99 Tc contamination at legacy nuclear sites is a serious and unsolved environmental issue. The selective remediation of 99 TcO 4 - in the presence of a large excess of NO 3 - and SO 4 2- from natural waste systems represents a significant scientific and technical challenge, since anions with a higher charge density are often preferentially sorbed by traditional anion exchange materials. We present a solution to this challenge based on a stable cationic metal-organic framework, SCU-102 (Ni 2 (tipm) 3 (NO 3 ) 4 ), which exhibits fast sorption kinetics, a large capacity (291 mg g 1 ), a high distribution coefficient, and, most importantly, a record-high TcO 4 - uptake selectivity. This material can almost quantitatively remove TcO 4 - in the presence of a large excess of NO 3 - and SO 4 2- . Finally, decontamination experiments confirm that SCU-102 represents the optimal Tc scavenger with the highest reported clean-up efficiency, while first-principle simulations reveal that the origin of the selectivity is the recognition of TcO 4 - by the hydrophobic pockets of the structure.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗