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At least 1,315 records · Page 73

Synthesis of monodisperse high entropy alloy nanocatalysts from core@shell nanoparticles

We report that high-entropy alloy (HEA) nanoparticles (NPs) hold great promise in electrocatalysis because of their nearly unlimited compositions, tailorable active sites, and high durability. However, the synthesis of these compositionally complex structures as monodisperse NPs remains a challenge by colloidal routes because the different rates of metal precursor reduction lead to phase separation. Here, we report the conversion of core@shell NPs into HEA NPs through annealing, with conservation of sample monodispersity. This potentially general route for high-quality HEA NPs was demonstrated by preparing PdCu@PtNiCo NPs via seed-mediated co-reduction, wherein Pt, Ni, and Co were co-deposited on PdCu seeds in solution. These multimetallic NPs were then converted to single-crystalline and single-phase PdCuPtNiCo NPs through annealing. On account of their small particle size, highly dispersed Pt/Pd content, and low elemental diffusivity, these HEA NPs were found to be a highly efficient and durable catalyst for the oxygen reduction reaction. They were also highly selective for the four-electron transfer pathway. We expect that this new synthetic strategy will facilitate the synthesis of new HEA NPs for catalysis and other applications.

36 MATERIALS SCIENCE↗

Chebyshev polynomial filtered subspace iteration in the discontinuous Galerkin method for large-scale electronic structure calculations

The Discontinuous Galerkin (DG) electronic structure method employs an adaptive local basis (ALB) set to solve the Kohn-Sham equations of density functional theory in a discontinuous Galerkin framework. The adaptive local basis is generated on-the-fly to capture the local material physics and can systematically attain chemical accuracy with only a few tens of degrees of freedom per atom. A central issue for large-scale calculations, however, is the computation of the electron density (and subsequently, ground state properties) from the discretized Hamiltonian in an efficient and scalable manner. We show in this work how Chebyshev polynomial filtered subspace iteration (CheFSI) can be used to address this issue and push the envelope in large-scale materials simulations in a discontinuous Galerkin framework. We describe how the subspace filtering steps can be performed in an efficient and scalable manner using a two-dimensional parallelization scheme, thanks to the orthogonality of the DG basis set and block-sparse structure of the DG Hamiltonian matrix. The on-the-fly nature of the ALB functions requires additional care in carrying out the subspace iterations. We demonstrate the parallel scalability of the DG-CheFSI approach in calculations of large-scale twodimensional graphene sheets and bulk three-dimensional lithium-ion electrolyte systems. In conclusion, employing 55 296 computational cores, the time per self-consistent field iteration for a sample of the bulk 3D electrolyte containing 8586 atoms is 90 s, and the time for a graphene sheet containing 11 520 atoms is 75 s.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dynamic properties of superconductors: Anderson-Bogoliubov mode and Berry phase in the BCS and BEC regimes

We analyze the evolution of the dynamics of a neutral s-wave superconductor between BCS and BEC regimes. We consider 2d case, when BCS-BEC crossover occurs already at weak coupling as a function of the ratio of the two scales – the Fermi energy E F and the bound state energy for two fermions in a vacuum, E 0 . BCS and BEC limits correspond to E F » E 0 and E F « E 0 , respectively. The chemical potential μ = E F - E 0 changes the sign between the two regimes. We use the effective action approach, derive the leading terms in the expansion of the effective action in the spatial and time derivative of the slowly varying superconducting order parameter Δ(r, τ), and express the action in terms of derivative of the phase Φ(r, τ) of Δ(r, τ) = Δe iΦ(r,τ) . The action contains (∇Φ) 2 and $\dot{Φ}$ 2 terms, which determine the dispersion of collective phase fluctuations, and iπA$\dot{Φ}$ term. For continuous Φ(r, τ), the latter reduces to the contribution from the boundary and does not affect the dynamics. We show that this longwavelength action does not change through BCS-BEC crossover. We apply our approach to a moving vortex, for which Φ is singular at the center of the vortex core, and iπA vort $\dot{Φ}$ term affects vortex dynamics. We find that this term has two contributions. One comes from the states away from the vortex core and has Avort,1 = n/2, where n is the fermion density. The other comes from electronic states inside the vortex core and has A vort,2 = -n 0 /2, where n 0 is the fermion density at the vortex core. This last term comes from the continuous part of the electronic spectrum and has no contribution from discrete levels inside the core; it also does not change if we add impurities. We interpret this term as the contribution to vortex dynamics in the continuum limit, when the spacing between energy levels ω is set to zero, while fermionic lifetime τ can be arbitrary. The total Avort = (n-n 0 )/2 determines the transversal force acting on the vortex core, πA vort $\dot{R}$ × $\hat{z}$, where $\dot{R}$ is the velocity of the vortex core and $\hat{z}$ a unit vector perpendicular to the 2d sample. The difference (n - n 0 )/2 changes through the BEC-BCS crossover as n 0 nearly compensates n in the BCS regime, but vanishes in the BEC regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Citizen Green #1 Well: Quantitative XRD & Thin Section Data

This submission includes information on quantitative x-ray diffraction measurements and thin section photography conducted on sidewall cores from the Citizen Green #1 well drilled on King Island, CA (API 07720688) as part of the WESTCARB partnership basin characterization effort. Cores were acquired with a rotary sidewall tool at a range of depths; only deeper cores were sufficiently consolidated for analysis. SidewallCoreFormationDepthNotes.xls provides details on available samples. Helium porosimetry, air permeability, and brine permeability measurements were conducted on all competent samples (~15). Samples were largely in the Mokelumne, H&T shale, and Starkey formations. All measurements were conducted at Lawrence Berkeley National Laboratory.

Thin Section↗

Electric Grid Expansion Planning with High Levels of Variable Generation

Renewables are taking a large proportion of generation capacity in U.S. power grids. As their randomness has increasing influence on power system operation, it is necessary to consider their impact on system expansion planning. To this end, this project studies the generation and transmission expansion co-optimization problem of the US Eastern Interconnection (EI) power grid with a high wind power penetration rate. In this project, the generation and transmission expansion problem for the EI system is modeled as a mixed-integer programming (MIP) problem. This study analyzed a time series creation method to capture the diversity of load and wind power across balancing regions in the EI system. The obtained time series can be easily introduced into the MIP co-optimization problem and then solved robustly through available MIP solvers. Simulation results show that the proposed time series generation method and the expansion co-optimization model and can improve the expansion result significantly after considering the diversity of wind and load across EI regions. The improved expansion plan that combines generation and transmission will aid system planners and policy makers to maximize the social welfare. This study shows that modelling load and wind variations and diversities across balancing regions will produce significantly different expansion result compared with former studies. For example, if wind is modeled in more details (by increasing the number of wind output levels) so that more wind blocks are considered in expansion planning, transmission expansion will be larger and the expansion timing will be earlier. Regarding generation expansion, more wind scenarios will slightly reduce wind generation expansion in the EI system and increase the expansion of other generation such as gas. Also, adopting detailed wind scenarios will reveal that it may be uneconomic to expand transmission networks for transmitting a large amount of wind power through a long distance in the EI system. Incorporating more details of renewables in expansion planning will inevitably increase the computational burden. Therefore, high performance computing (HPC) techniques are urgently needed for power system operation and planning optimization. As a scoping study task, this project tested some preliminary parallel computation techniques such as breaking down the simulation task into several sub-tasks based on chronology splitting or sample splitting, and then assigning these sub-tasks to different cores. Testing results show significant time reduction when a simulation task is split into several sub-tasks for parallel execution.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Evidence for Neutrino Emission from X-Ray-bright Active Galactic Nuclei with IceCube

Recently, IceCube reported neutrino emission from the Seyfert galaxy NGC 1068. Using 13.1 yr of IceCube data, we present a follow-up search for neutrino sources in the northern sky. NGC 1068 remains the most significant neutrino source among 110 preselected gamma-ray emitters while also being spatially compatible with the most significant location in the northern sky. Its energy spectrum is characterized by an unbroken power-law with spectral index γ = 3.4 ± 0.2. Consistent with previous results, the observed neutrino flux exceeds its gamma-ray counterpart by at least 2 orders of magnitude. Motivated by this disparity and the high X-ray luminosity of the source, we selected 47 X-ray-bright Seyfert galaxies from the Swift/BAT spectroscopic survey that were not included in the list of gamma-ray emitters. When testing this collection for neutrino emission, we observe a 3.3σ excess from an ensemble of 11 sources, with NGC 1068 excluded from the sample. Our results strengthen the evidence that X-ray-bright cores of active galactic nuclei are neutrino emitters.

Abbasi, R. [Loyola University, Chicago, IL (United↗

Ice nucleating particle concentrations in the Arctic during MOSAiC 2020

This data set contains ice nucleating particle (INP) measurements, using Colorado State University’s (CSU) Ice Spectrometer (IS) of samples collected during the Multidisciplinary Drifting Observatory for the Study of Arctic Climate (MOSAiC) field campaign. Samples were collected from five different media: aerosol filters, meltwater, ice cores, snow pits, and bulk sea water (BSW).

54 ENVIRONMENTAL SCIENCES↗

On the origin of Luna 24 basalts and soils

Analyses of fine-grained very low titanium (VLT) basalt from the Luna 24 drill core suggest that a single homogeneous magma is represented by the sample. In particular, the small variation in MgO contents of the fine-grained basalt, together with the tight clustering of the compositions of brown glasses (which may be pyroclastic equivalents of the VLT basalt), provides evidence for the single-magma hypothesis. The high-Mg component in the soil samples, though not obviously explainable in petrographic terms, may be derived from material similar to olivine vitrophyre and its degraded products, or from some other high-Mg VLT basalt.

Ryder, G.↗

Characterizing Urban Heat Islands of Global Settlements Using MODIS and Nighttime Lights Products

Impervious surface area (ISA) from the National Geophysical Data Center (NGDC) and land surface temperature (LST) from the Moderate Resolution Imaging Spectroradiometer (MODIS) averaged over three annual cycles (2003-2005) are used in a spatial analysis to assess the urban heat island (UHI) signature on LST amplitude and its relationship with development intensity, size, and ecological setting for more than 3000 urban settlements globally. Development intensity zones based on fractional ISA are defined for each urban area emanating outward from the urban core to the nearby nonurban rural areas and used to stratify sampling for LST. Sampling is further constrained by biome type and elevation data to ensure objective intercomparisons between zones and between cities in different biomes. We find that the ecological context and settlement size significantly influence the amplitude of summer daytime UHI. Globally, an average of 3.8 C UHI is found in cities built in biomes dominated by forests; 1.9 C UHI in cities embedded in grass shrubs biomes; and only a weak UHI or sometimes an urban heat sink (UHS) in cities in arid and semi-arid biomes. Overall, the amplitude of the UHI is negatively correlated (R = -0.66) with the difference in vegetation density between urban and rural zones represented by the MODIS normalized difference vegetation index (NDVI). Globally averaged, the daytime UHI amplitude for all settlements is 2.6 C in summer and 1.4 C in winter. Globally, the average summer daytime UHI is 4.7 C for settlements larger than 500 square kilometers compared with 2.5 C for settlements smaller than 50 square kilometers and larger than 10 square kilometers. The stratification of cities by size indicates that the aggregated amount of ISA is the primary driver of UHI amplitude, with variations between ecological contexts and latitudinal zones. More than 60% of the total LST variance is explained by ISA for urban settlements within forests at mid to high latitudes. This percentage will increase to more than 80% when only settlements in the US are examined.

Zhang, Ping↗

Ultra-Compact Imaging Spectrometer (UCIS) for In-Situ Planetary Mineralogy: Laboratory and Field Calibration

The Ultra-Compact Imaging Spectrometer (UCIS) is a miniature telescope and spectrometer system intended for mapping terrain mineralogy over distances from 1.5 m to infinity with spatial sampling of 1.35 mrad over a 33 deg field, and spectral sampling of 10 nm in the 600-2500 nm range. The core of the system has been designed for operation in a Martian environment, but can also be used in a terrestrial environment when placed inside a vacuum vessel. We report the laboratory and field calibration data that include spatial and spectral calibration, and demonstrate the use of the system.

Imaging spectroscopy↗

Density changes in amorphous silicon induced by swift heavy ions

For this study, pure and gold-doped amorphous silicon membranes were irradiated with swift heavy ions (75 MeV Ag or 1.1 GeV Au ions) and studied using small-angle x-ray scattering. The samples that were irradiated with 1.1 GeV Au ions produced a scattering pattern consistent with core-shell-type ion tracks of 2.0 ± 0.1 nm (core) and 7.0 ± 0.3 nm (total) radius irrespective of gold doping, consistent with radii previously observed. The density in the core is nearly 4% different from that of the surrounding material. The entire track (core + shell) is slightly less dense than the surrounding material, yielding an expansion or hammering constant A of 0.036 ± 0.003 nm 2 per ion track, consistent with the macroscopic “hammering” deformation. No tracks were found in samples irradiated with 75 MeV Ag ions, and no signature specific to the gold impurity doping could be observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The radio structure source of X-ray-selected BL Lacertae objects

Arcsecond-size radio structure for a complete sample of 14 X-ray-selected BL Lac objects (XBLs) from the Einstein Extended Medium-Sensitivity Survey is presented. Most objects possess radio morphologies which are similar to those of nearby Fanaroff-Riley type 1 (FR 1) radio galaxies once the effects of surface brightness dimming and beam dilution as a function of redshift are taken into account. In order to test the beamed FR 1 hypothesis for BL Lac objects, the core and extended power levels are determined for these sources and compared with samples of radio-selected BL Lac objects (RBLs) and FR 1 from galaxies from the literature. RBLs and XBLs are found to possess extended (and thus unbeamed) power levels and the largest angular sizes similar to those of the FR 1 galaxies both supporting the beaming hypothesis and a common parent population for XBLs and RBLs.

Perlman, Eric S.↗

Final Scientific/Technical Report: Characterizing the Response of the Cascadia Margin Gas Hydrate Reservoir to Bottom Water Warming Along the Upper Continental Slope

The objective of this project is to understand the response of the WA margin gas hydrate system to contemporary warming of bottom water along the upper continental slope. Through pre-cruise analysis and modeling of archive and recent geophysical and oceanographic data, we (1) inventoried bottom simulating reflectors along the WA margin and defined the upper limit of gas hydrate stability, (2) refined margin-wide estimates of heat flow and geothermal gradients, (3) characterized decadal scale temporal variations of bottom water temperatures at the upper continental slope of the Washington margin, and (4) used numerical simulations to provide quantitative estimates of how the shallow boundary of methane hydrate stability responds to modern environmental change. These pre-cruise results provided the context for a systematic geophysical and geochemical survey of methane seepage along the upper continental slope from 48° to 46°N during a 10-day field program on the R/V Thompson from October 10-19, 2014. This systematic inventory of methane emissions along this climate-sensitive margin corridor and comprehensive sediment and water column sampling program provided data and samples for Phase 3 of this project that focused on determining fluid and methane sources (deep-source vs. shallow; microbial, thermogenic, gas hydrate dissociation) within the sediment, and how they relate to contemporary intermediate water warming. During the 2014 research expedition, we sampled nine seep sites between ~470 and 520 m water depth, within the zone of predicted methane hydrate retreat over the past 40 years. We imaged 22 bubble plumes with heights commonly rising to ~300 meters below sea level with one reaching near the sea surface. We collected 22 gravity cores and 20 CTD/hydrocasts from the 9 seeps and at background locations (no acoustic evidence of seepage) within the depth interval of predicted downslope retreat of the methane hydrate stability zone. Approximately 300 pore water samples were extracted from the gravity cores, and the pore water was analyzed for a comprehensive suite of solutes, gases, and stable isotope ratios. This comprehensive geochemical dataset was used to characterize the fluid and gas source(s) at each of the seep sites surveyed. The primary results of this project are: 1) Bottom simulating reflector-derived heat flow values decrease from 95 mW/m2 10 km east of the deformation front to ~60 mW/m2 60 km landward of the deformation front, with anomalously low values of ~25 mW/m2 on a prominent mid-margin terrace off central Washington. 2) The temperature of the incoming sediment/ocean crust interface at the deformation front ranges between 164-179 oC off central Washington, and the 350 oC isotherm at the top of the subducting ocean crust occurs 95 km landward of the deformation front. Differences between BSR-derived heat flow and modeled conductive heat flow suggest mean upward fluid flow rates of 0.4 cm/yr across the margin, with local regions (e.g. fault zones) exhibiting fluid flow rates up to 3.5 cm/yr. 3) A compilation of 2122 high-resolution CTD, glider, and Argo float temperature profiles spanning the upper continental slope of the Washington margin from the years 1968 to 2013 show a long-term warming trend that ranges from 0.006-0.008 oC/yr. Based on this long-term bottom water warming, we developed a 2-D thermal model to simulate the change in sediment temperature distribution over this period, along with the downslope retreat of the methane hydrate stability field. Over the 43 years of the simulation, the thermal disturbance propagated 30 m into the sediment column, causing the base of the methane hydrate stability field to shoal ~13 m and to move ~1 km downslope. 4) A preliminary analysis of seafloor observations and mid-water column acoustic data to detect bubble plumes was used to characterize the depth distribution of seeps along the Cascadia margin. These results indicate high bubble plume densities along the continental shelf at water depths <180 m and at the upper limit of methane hydrate stability along the Washington margin. 5) The majority of the seeps cored during the 2014 research expedition on the R/V Thompson contained abundant authigenic carbonate indicating that they are locations of long-lived seepage rather than emergent seep systems related to methane hydrate dissociation. Despite the evidence for enhanced methane seepage at the upper limit of methane hydrate stability along the Washington margin, we found no unequivocal evidence for active methane hydrate dissociation as a source of fluid and gas at the seeps surveyed. The pore fluid and bottom water chemistry shows that the seeps are fed by a variety of fluid and methane sources, but that methane hydrate dissociation, if occurring, is not widespread and is only a minor source (below the detection limit of our methods). Collectively, these results provide a significant advance in our understanding of the thermal structure of the Cascadia subduction zone and the fluid and methane sources feeding seeps along the upper continental slope of the Washington-sector of the Cascadia margin. Though we did not find unequivocal evidence for methane hydrate dissociation as a source of water and methane at the upper pressure-temperature limit of methane hydrate stability at present, continued warming of North Pacific Intermediate Water in the future has the potential to impact the methane hydrate reservoir in sediments at greater depths along the slope. Thus, this study provides a strong foundation and the necessary characterization of the background state of seepage at the upper limit of methane hydrate stability for future investigations of this important process.

54 ENVIRONMENTAL SCIENCES↗

Fine structure of the late Eocene Ir anomaly in marine sediments

The Late Eocene Ir abundance profile in deep sea cores from Ocean Drilling Program Leg 113 Hole 689B on the Maude Rise off of Antarctica was studied with 410 samples continuously in 10 cm increments and measured with the Iridium Coincidence (ICS). The ICS was subsequently modified to measure 13 other elements simultaneously with the Ir. The abundance profiles of these elements were then determined in the Late Eocene Massignano section in central Italy with 250 samples (encompassing roughly 2 million years of accumulation) which were collected about every 5 cm in about 2 cm increments. These studies augmented a previous one (which included many elements) of deep sea cores from Deep Sea Drilling Project Site 592 on the Lord Howe Rise in the Tasman Sea between Australia and New Zealand. In the latter study, 50 samples (encompassing roughly 0.7 million years of accumulation) were collected continuously in 10 cm increments. The results from these studies are discussed.

Asaro, F.↗

Fossil track and thermoluminescence studies of Luna 20 material.

Track densities in 85 feldspar crystals from L-2009 range from 2,500,000 per sq cm to greater than one billion per sq cm. This track distribution represents an intermediate case between what have been previously defined as lightly and heavily irradiated soils and suggests that the Luna 20 sample consists of a mixture of a mature, heavily irradiated component with another, lightly irradiated component. Using a two-component mixing model, the age of the lightly irradiated component is about 270,000,000 yr. It is possible, but by no means certain, that this is associated with the formation of the crater Apollonius C. At about 200 C the ratio of natural thermoluminescence to that induced by a standard irradiation is similar to that in Apollo 12 and 14 cores below about 7 cm. This confirms that most of the Luna 20 sample represents subsurface material.

Crozaz, G.↗

Comparison of Statistically Modeled Contaminated Soil Volume Estimates and Actual Excavation Volumes at the Maywood FUSRAP Site - 13555

As part of the ongoing remediation process at the Maywood Formerly Utilized Sites Remedial Action Program (FUSRAP) properties, Argonne National Laboratory (Argonne) assisted the U.S. Army Corps of Engineers (USACE) New York District by providing contaminated soil volume estimates for the main site area, much of which is fully or partially remediated. As part of the volume estimation process, an initial conceptual site model (ICSM) was prepared for the entire site that captured existing information (with the exception of soil sampling results) pertinent to the possible location of surface and subsurface contamination above cleanup requirements. This ICSM was based on historical anecdotal information, aerial photographs, and the logs from several hundred soil cores that identified the depth of fill material and the depth to bedrock under the site. Specialized geostatistical software developed by Argonne was used to update the ICSM with historical sampling results and down-hole gamma survey information for hundreds of soil core locations. The updating process yielded both a best guess estimate of contamination volumes and a conservative upper bound on the volume estimate that reflected the estimate's uncertainty. Comparison of model results to actual removed soil volumes was conducted on a parcel-by-parcel basis. Where sampling data density was adequate, the actual volume matched the model's average or best guess results. Where contamination was un-characterized and unknown to the model, the actual volume exceeded the model's conservative estimate. Factors affecting volume estimation were identified to assist in planning further excavations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Bacterial endophyte communities in Pinus flexilis are structured by host age, tissue type, and environmental factors

Background and aims: Forest tree microbiomes are vital to forest dynamics, diversity, and ecosystem processes. Mature limber pines ( Pinus flexilis ) host a core microbiome of acetic acid bacteria in their foliage, but the bacterial endophyte community structure, variation, and assembly across tree ontogeny is unknown. The aims of this research were to test if the core microbiome observed in adult P. flexilis is established at the seedling stage, if seedlings host different endophyte communities in root and shoot tissues, and how environmental factors structure seedling endophyte communities. Methods: The 16S rRNA gene was sequenced to characterize the bacterial endophyte communities in roots and shoots of P. flexilis seedlings grown in plots at three elevations at Niwot Ridge, Colorado, subjected to experimental treatments (watering and heating). The data was compared to previously sequenced endophyte communities from adult tree foliage sampled in the same year and location. Results: Seedling shoots hosted a different core microbiome than adult tree foliage and were dominated by a few OTUs in the family Oxalobacteraceae , identical or closely related to strains with antifungal activity. Shoot and root communities significantly differed from each other but shared major OTUs. Watering but not warming restructured the seedling endophyte communities. Conclusions: The results indicate differences in assembly and ecological function across conifer life stages. Seedlings may recruit endophytes to protect against fungi under increased soil moisture.

16S rRNA↗

Noble gas studies on regolith materials from Apollo 14 and 15.

Abundances and isotopic compositions of the five stable noble gases, He, Ne, Ar, Kr, and Xe in soils and breccia were determined. The samples investigated included material from a range of depths in a trench and a core tube. Noble gas determinations were performed in a 6-inch all-metal mass spectrometer of high sensitivity. The grain size separates and stepwise heating experimental methods used give results that supplement each other. Calculated concentrations of spallation Xe-126 in many of the fines and gas-rich breccia are presented in a table. Bulk soil samples obtained by Apollo 14 show an inverse correlation of spallation Xe-126 with grain size.

Bogard, D. D.↗