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DOE OSTI2025

Defect-Engineered High-Entropy Spinel Oxide@Onion-Like Carbon Catalysts for High-Areal-Energy Rechargeable Zinc–Air Batteries

Rechargeable zinc-air batteries (ReZAB) have emerged as the next-generation batteries with several advantages over the conventional lithium-ion battery. In this work, single nanocrystals of inverse-type high-entropy spinel oxides (HESOx, particle size of 10−12 nm) confined in highly curved defective onion-like carbons (HESOx/OLC AT ) as efficient electrocatalysts for oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and ReZAB, have been synthesized. The HESOx materials were thoroughly characterized using several analytical techniques, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), Raman, and electron paramagnetic resonance (EPR). HESOx/OLC AT catalyst was tested for ReZAB using literature-recommended parameters that would allow for real technological application. These parameters include a current loading of 10 mA cm −2 and a discharge areal energy density of 35 mWh cm geometric −2 , which maps a Li-ion battery pack-level specific energy of 120 Wh kg pack −1 . HESOx/OLC AT electrocatalysts allowed for continuous discharging and charging at a current loading of 10 mA cm −2 with discharge areal energy densities between 37 and 74 mWh cm geometric −2 , thus outperforming the recommended threshold of 35 mWh cm geometric −2 . Considering that most studies (>90%) hardly meet the recommended threshold for technological application of ReZAB, the present work represents one of the top-performing electrocatalysts for ReZAB. The excellent electrocatalytic properties of defect-rich HESOx/OLC AT toward ORR/OER and ReZAB are governed by the strong electronic modulation arising from d-π hybridization, the availability of multiple catalytic sites for intermediates, and weakened d-band centers of the rate-determining intermediates (i.e., *O adsorption for ORR and *OOH formation for OER) compared to the pristine HESOx. This work introduces an effective approach for the design and synthesis of single nanocrystals of high-entropy electrocatalysts for the development of low-cost, robust, and technologically relevant rechargeable zinc−air batteries.

25 ENERGY STORAGE↗

DOE OSTI2020

The Incorporation of Pump-and-Treat Data in the New Tracking Restoration and Closure (TRAC)Web-Based Mapping Tool - 20339

Groundwater pump-and-treat (P and T) systems are a common remediation strategy for sites with contaminated groundwater within the U.S. Department of Energy (DOE) Office of Environmental Management (EM). Currently, there are six DOE-EM sites with active P and T systems, but integrated information on individual systems is only primarily available in separate annual reports. To provide a broad view of both current and historical P and T operations, data has been collected on all of the P and T systems. This summary information not only includes capital and average annual costs, but also identifies contaminants treated and forecasted P and T closure dates. Principal contaminants of concern treated with P and T systems include trichloroethylene, chromium (VI), strontium-90, technetium-99, and uranium. DOE-EM is continuing to create a web-based mapping tool that compiles information on groundwater contaminants, remediation strategies and, current data related to plumes and cleanup progress within all DOE-EM sites. The information collected on P and T systems will be added to the TRAC (Tracking Restoration and Closure) tool using interactive maps to quickly access and share information. This information sharing supports the transition from active to passive remediation methods and long-term monitoring approaches. TRAC can ensure that managers, stakeholders, regulators, and contractors remain up to date on cleanup progress for all sites within the complex. The information on P and T systems expands the use of TRAC and can assist in project monitoring and budget planning and support potential shifts in management plans based on plume data. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Remote Sensing-Based, 5-m, Vegetation Distributions, Kougarok Study Site, Seward Peninsula, Alaska, ca. 2009 - 2016

A multi-sensor remote sensing-based deep learning approach was developed for generating high-resolution (5~m) vegetation maps for the western Alaskan Arctic on the Seward Peninsula, Alaska. This data was developed using the fusion of hyperspectral, multispectral, and terrain datasets. The current data is located in the Kougarok watershed but we plan to expand this over the Seward Peninsula. Additional metadata and vegetation maps included as two *.pdf, one *.txt, one *.nc, and three *.tif files.The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), was a research effort to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy's Office of Biological and Environmental Research.The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska.Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy's Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2021

The Temporal and Spatial Development of dB/dt for Substorms

Ground induced currents (GICs) due to space weather are a threat to high voltage power transmission systems. However, knowledge of ground conductivity is the largest source of errors in the determination of GICs. A good proxy for GICs is dB/dt obtained from the Bx and By components of the magnetic field fluctuations. It is known that dB/dt values associated with magnetic storms can reach dangerous levels for power transmission systems. On the other hand, it is not uncommon for dB/dt values associated with substorms to exceed prior Pulkkinen and Molinski critical thresholds of 1.5 nT/s and 5 nT/s, respectively, and the temporal and spatial changes of the dB/dt associated with substorms, unlike storms, are not well understood. Using two dimensional maps of dB/dt over North America and Greenland derived from the spherical elementary currents, we investigate the temporal and spatial change of dB/dt for both a single substorm event and a two dimensional superposed epoch analysis of many substorms. Both the single event and the statistical analysis shows a sudden increase of dB/dt at substorm onset followed by an expansion poleward, westward, and eastward after the onset during the expansion phase. The area of dB/dt values exceeding the two critical thresholds from the initial onset dB/dt values showed little to no expansion equatorward. The temporal and spatial development of the dB/dt resembles the temporal and spatial change of the auroral emissions. Substorm values of dB/dt peak shortly after the auroral onset time and in at least one event exceeded 35 nT/s for a non-storm time substorm. In many of our 81 cases the area that exceeds the threshold of 1.5 nT/s is over several million square kilometers and after about 30 minutes the dB/dt values fall below the threshold level. These results address one of goals of the Space Weather Action Plan, which are to establish benchmarks for space weather events and improve modeling and prediction of their impacts on infrastructure. Plain language: The change in the ground magnetic field with respect to time (dB/dt) associated with magnetic storms (a large disturbance of the magnetic field of the earth) can reach dangerous levels for power transmission systems. On the other hand, substorms, which are a smaller more localized disturbance of the Earth’s magnetic field, are more common. It is not uncommon for substorm dB/dt values to also exceed dangerous levels and the temporal and spatial changes of the dB/dt associated with substorms, unlike storms, are not well understood. Our analysis shows a sudden increase of dB/dt at substorm onset, which peaks shortly after the start of the substorm, followed shortly after by an expansion northward, westward, and eastward after the onset.

ionospheric currents↗

DOE OSTI2023

Inference of the optical depth to reionization τ from Planck CMB maps with convolutional neural networks

The optical depth to reionization, τ, is the least constrained parameter of the cosmological Λ cold dark matter (ΛCDM) model. To date, its most precise value is inferred from large-scale polarized cosmic microwave background (CMB) power spectra from the High Frequency Instrument (HFI) aboard the Planck satellite. These maps are known to contain significant contamination by residual non-Gaussian systematic effects, which are hard to model analytically. Therefore, robust constraints on τ are currently obtained through an empirical cross-spectrum likelihood built from simulations. In this paper, we present a likelihood-free inference of τ from polarized Planck HFI maps which, for the first time, is fully based on neural networks (NNs). NNs have the advantage of not requiring an analytical description of the data and can be trained on state-of-the-art simulations, combining the information from multiple channels. By using Gaussian sky simulations and Planck SRoll2 simulations, including CMB, noise, and residual instrumental systematic effects, we trained, tested, and validated NN models considering different setups. We inferred the value of τ directly from Stokes Q and U maps at ~4° pixel resolution, without computing angular power spectra. On Planck data, we obtained τ NN = 0.0579 ± 0.0082, which is compatible with current EE cross-spectrum results but with a ~30% larger uncertainty, which can be assigned to the inherent nonoptimality of our estimator and to the retraining procedure applied to avoid biases. While this paper does not improve on current cosmological constraints on τ, our analysis represents a first robust application of NN-based inference on real data, and highlights its potential as a promising tool for complementary analysis of near-future CMB experiments, also in view of the ongoing challenge to achieve the first detection of primordial gravitational waves.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Direct density modulation of photo-assisted field emission from an RF cold cathode

This paper explores direct density modulation of high-current electron beam emission from an RF cold cathode using optical excitation. We theoretically study the photo-assisted field emission of periodically bunched electron beams of various pulse shapes under the combined excitation of an RF field and an optical field, using an exact quantum model. Both continuous-wave (CW) and pulsed optical fields are considered. The emission current pulse amplitude, pulse width, electron number density per pulse, as well as pulse shape and its harmonic contents are investigated in detail. For CW photon sources in the UV to NIR range (i.e., 200–1200 nm), increasing the optical intensity under an RF bias tends to change the current pulse from a Gaussian to sinusoidal-like shape, thus offering strong flexibility to control the frequency components in beam current emission. Pulsed photon sources combined with an RF field can produce sharp, high-current electron bunches with pulse duration comparable with or even less than that of the optical pulse. A contour map of the density modulation depth is constructed for different combinations of RF and laser fields. The results provide insight into unlocking new opportunities to achieve direct density modulation during electron current emission by optical means.

Physics↗

DOE OSTI2018

Exploring the posterior surface of the large scale structure reconstruction

The large scale structure (LSS) of the universe is generated by the linear density gaussian modes, which are evolved into the observed nonlinear LSS. Given a set of data the posterior surface of the modes is convex in the linear regime, leading to a unique global maximum (MAP), but this is no longer guaranteed in the nonlinear regime. In this paper we investigate the nature of posterior surface using the recently developed MAP reconstruction method, with a simplified but realistic N-body simulation as the forward model. The reconstruction method uses optimization with analytic gradients from back-propagation through the simulation. For low noise cases we recover the initial conditions well into the nonlinear regime (k~ 1 h/Mpc) nearly perfectly. We show that the large scale modes can be recovered more precisely than the linear expectation, which we argue is a consequence of nonlinear mode coupling. For noise levels achievable with current and planned LSS surveys the reconstruction cannot recover very small scales due to noise. We see some evidence of non-convexity, specially for smaller scales where the non-injective nature of the mappings: several very different initial conditions leading to the same near perfect final data reconstruction. We investigate the nature of these phenomena further using a 1-d toy gravity model, where many well separated local maximas are found to have identical data likelihood but differ in the prior. We also show that in 1-d the prior favors some solutions over the true solution, though no clear evidence of these in 3-d. Our main conclusion is that on very small scales and for a very low noise the posterior surface is multi-modal and the global maximum may be unreachable with standard methods, while for realistic noise levels in the context of the current and next generation LSS surveys MAP optimization method is likely to be nearly optimal.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1981

Investigation from Japanese MAGSAT Team. Part A. Crustal structure near Japan and in Antarctic station. Part B. Electric currents and hydromagnetic waves in the ionosphere and the magnetosphere

Preliminary results of MAGSAT data analysis are described. Regional anomaly maps (deviations from the MGST model field) for X,Y,Z, and F in the area of 115 to 155 deg E and 20 to 60 deg N were obtained. A similar map for the geomagnetic total force anomaly in the vicinity of Japan showed that the observed anomaly can be explained by the difference in crustal magnetization between the Japan Sea and the Japan Island, which reflects a difference of 25 km in the thickness of the magnetized layer. The MAGSAT record of a sudden commencement of a magnetic storm above the South Atlantic Ocean showed a reverse impulse particularly in the D-component. Results relating to toroidal currents in the ionosphere, transverse and parallel perturbations over the polar regions, the relationship between field aligned currents and precipitating electrons, and the calculation of the subsatellite electric field are also discussed.

Fukushima, N.↗

DOE OSTI2026

Coupled Interfacial Kinetics and Transport Resistances Govern High-Current Behavior in Bipolar Membranes

Bipolar membranes (BPMs) enable electrochemical systems that operate across large pH gradients; however, high-current operation is often limited by voltage losses whose origins remain difficult to resolve in membrane−electrode assemblies. Here, we combine electrochemical impedance spectroscopy with distribution of relaxation times (EIS–DRT) analysis and operando synchrotron X-ray diffraction to examine interfacial polarization, membrane hydration, and transport in commercial and synthesized BPMs. EIS–DRT isolates the BPM-associated interfacial contribution and shows that the commercial BPM exhibits larger water-dissociation-associated overpotentials than the synthesized BPM. Operando hydration mapping shows that both membranes retain water at the bipolar junction during high-current operation, while anode-adjacent hydration gradients are more pronounced in the commercial membrane. These results indicate that high-current voltage losses are not governed by junction water starvation alone but by coupled interfacial polarization and transport resistances.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Ensemble Estimation of Historical Evapotranspiration for the Conterminous U.S.

Abstract Evapotranspiration (ET) is the largest component of the water budget, accounting for the majority of the water available from precipitation. ET is challenging to quantify because of the uncertainties associated with the many ET equations currently in use, and because observations of ET are uncertain and sparse. In this study, we combine information provided by available ET data and equations to produce a new monthly data set for ET for the conterminous U.S. (CONUS). These maps are produced from 1895 to 2018 at an 800 m spatial scale, marking a finer resolution than currently available products over this time period. In our approach, the relative performance of a suite of ET equations is assessed using water balance, flux tower, and remotely sensed ET estimates. At the observation locations, we use error distributions to quantify relative weights for the equations and use these in a modified Bayesian model averaging weighted ensemble approach. The relative weights are spatially generalized using a random forest regression, which is applied to wall‐to‐wall explanatory variable maps to generate CONUS‐wide relative weight maps and ensemble estimates. We assess the performance of the ensemble using a reserved subset of the observations and compare this performance against other national‐scale map products for historical to modern ET. The ensemble ET maps are shown to provide an improved accuracy over the alternative comparison products. These ET maps could be useful for a variety of hydrologic modeling and assessment applications that benefit from a long record, such as the study of periods of water scarcity through time.

Environmental Sciences & Ecology↗

DOE OSTI2019

110th Anniversary: Bridging the Time and Length Scales of Process Systems with Data

Here we report on the role of data as a "bridge" connecting the different time/length scales of chemical processes in mathematical modeling and multi-scale, integrated decision making. We argue that this is a fitting role of "big data" in the chemical industry, an area that comprises complicated yet deterministic physical systems. Such systems can be described using physical and chemical laws that are generally well-understood. Accordingly, data and data analysis are less likely to provide the unexpected and/or surprising insights that they have generated in other sectors (e.g., the transactional economy, social sciences). Nevertheless, historical operating data (which are often plentiful and available at little cost) can be converted to very useful information for multi-scale mathematical modeling of chemical processes. Several examples of integration are provided, mapped on the continuum of time and length scales of process systems. Current research challenges and potential directions for future work are discussed.

42 ENGINEERING↗

DOE OSTI2019

Time-resolved XUV ARPES with tunable 24–33 eV laser pulses at 30 meV resolution

Abstract High harmonic generation of ultrafast laser pulses can be used to perform angle-resolved photoemission spectroscopy (ARPES) to map the electronic band structure of materials with femtosecond time resolution. However, currently it is difficult to reach high momenta with narrow energy resolution. Here, we combine a gas phase extreme ultraviolet (XUV) femtosecond light source, an XUV monochromator, and a time-of-flight electron analyzer to develop XUV-based time-resolved ARPES. Our technique can produce tunable photon energy between 24–33 eV with an unprecedented energy resolution of 30 meV and time resolution of 200 fs. This technique enables time-, energy- and momentum-resolved investigation of the nonequilibrium dynamics of electrons in materials with a full access to their first Brillouin zone. We evaluate the performance of this setup through exemplary measurements on various quantum materials, including WTe 2 , WSe 2 , TiSe 2 , and Bi 2 Sr 2 CaCu 2 O 8+δ .

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Pre-conditioned BFGS-based uncertainty quantification in elastic full-waveform inversion

SUMMARY Full-waveform inversion has become an essential technique for mapping geophysical subsurface structures. However, proper uncertainty quantification is often lacking in current applications. In theory, uncertainty quantification is related to the inverse Hessian (or the posterior covariance matrix). Even for common geophysical inverse problems its calculation is beyond the computational and storage capacities of the largest high-performance computing systems. In this study, we amend the Broyden–Fletcher–Goldfarb–Shanno (BFGS) algorithm to perform uncertainty quantification for large-scale applications. For seismic inverse problems, the limited-memory BFGS (L-BFGS) method prevails as the most efficient quasi-Newton method. We aim to augment it further to obtain an approximate inverse Hessian for uncertainty quantification in FWI. To facilitate retrieval of the inverse Hessian, we combine BFGS (essentially a full-history L-BFGS) with randomized singular value decomposition to determine a low-rank approximation of the inverse Hessian. Setting the rank number equal to the number of iterations makes this solution efficient and memory-affordable even for large-scale problems. Furthermore, based on the Gauss–Newton method, we formulate different initial, diagonal Hessian matrices as pre-conditioners for the inverse scheme and compare their performances in elastic FWI applications. We highlight our approach with the elastic Marmousi benchmark model, demonstrating the applicability of pre-conditioned BFGS for large-scale FWI and uncertainty quantification.

58 GEOSCIENCES↗

DOE OSTI2024

Nature versus nurture: distinguishing effects from stellar processing and chemical evolution on carbon and nitrogen in red giant stars

ABSTRACT The surface [C/N] ratios of evolved giants are strongly affected by the first dredge-up (FDU) of nuclear-processed material from stellar cores. C and N also have distinct nucleosynthetic origins and serve as diagnostics of mixing and mass-loss. We use subgiants to find strong trends in the birth [C/N] with [Fe/H], which differ between the low-α and high-α populations. We demonstrate that these birth trends have a strong impact on the surface abundances after the FDU. This effect is neglected in current stellar models, which use solar-scaled C and N. We map out the FDU as a function of evolutionary state, mass, and composition using a large and precisely measured asteroseismic data set in first-ascent red giant branch (RGB) and core He-burning, or red clump (RC), stars. We describe the domains where [C/N] is a useful mass diagnostic and find that the RC complements the RGB and extends the range of validity to higher mass. We find evidence for extra mixing on the RGB below [Fe/H] = −0.4, matching literature results, for high-α giants, but there is no clear evidence of mixing in the low-α giants. The predicted signal of mass-loss is weak and difficult to detect in our sample. We discuss implications for stellar physics and stellar population applications.

Roberts, John D. (ORCID:0000000228545796)↗

DOE OSTI2022

ESS-DIVE Reporting Format for Amplicon Abundance Table

While standardized sequencing data is available in public repositories and efforts such as MIxS for common sample collection and processing metadata are well established, the lack of common bioinformatic processing metadata has hindered the ability to do large-scale metaanalyses and the potential for data re-use by non-experts such as ecosystem, watershed, or earth system modelers. To address this need for Department of Energy researchers, we have developed an amplicon reporting format which captures both sample preparation and bioinformatic processing metadata and stores processed amplicon data as a paired abundance table and sequencing file to maximize the potential for re-use of these data. To aid in the adoption of accessible and reproducible analysis workflows, this reporting format was developed in concert with amplicon functionality within the Department of Energy’s Systems Biology Knowledgebase (KBase) to ensure common data and metadata requirements and facilitate seamless transfer between these platforms.This dataset contains support documentation for the amplicon reporting format (README.md and instructions.md), templates for both bioinformatic and sequencing metadata (amplicon_bioinformatic_metadata_template_2021_10_03.csv and amplicon_sequencing_metadata_template_2021_10_03.csv), a crosswalk indicating how this reporting format relates to the current MIxS format (ESSDIVE-MIxS_crosswalk.csv), a list of available instrument terms (amplicon_seq_instrument_terms_2021_10_03.csv), a map between QIIME2 parameter settings and metadata fields (amplicon_qiime2_plugin_metadata_map.csv), a data dictionary (amplicon_CSV_dd.csv), and file-level metadata (amplicon_FLMD.csv).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Synchrotron Based Microstructural Characterization Method Development for Pu Oxides

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2019

Synchrotron Based Microstructural Characterization Method Development for Pu Oxides

Identification of new plutonium oxide signatures is a high priority focus area of the technical nuclear forensics and nonproliferation communities. Comprehensive materials science studies of plutonium oxide are needed to advance the understanding of the microcrystalline properties and their relationship to macro-scale morphologies and signatures. Plutonium oxide particle growth is depenedent on the microcrystalline strucutures, grain size, and orientation. Microcrystalline structures have been found to vary for plutonium oxide based on the oxidation state of plutonium, concentration of reactants, and the physiochemical conditions of precipitation. Empirical observation confirms the relationship between processing conditions and particle morphology. High sensitivity, non destructive analysis of individual microcrystalline grains requires the use of bright sources of X-rays produced by synchrotron radiation, such as those at the Advanced Photon Source. The light source can reveal higher resolution crystallographic mapping, more sensitive chemical analysis, and higher fidelity morphological information than any current methods at SRNL Progress of FY19 was the analysis of the synchrotron data. Areas of focus included XANES oxidation state and EXAFS to measure bond distances with modeling. Most measurements for XANES indicated that the plutonium was in the +4 oxidation state, however, some indicated that there could also be a +5 oxidation state. The EXAFS measurements showed typical Pu – O bonding distance of 2.33 and Pu – Pu bonding distances of 3.81 A; however, some samples also showed that there could be shorter Pu – O distances of approximately 1.81 A, indicative of plutonium in the +5 oxidation state.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Electrically Engaged UnduLation (EEL) Marine Energy System

Current technologies at the forefront of instrumentation for ocean observation through acoustic mapping are powered by batteries that cannot achieve the lasting durations required for high-resolution measurements. Pyro-E has designed an Electrically Engaged unduLation (EEL) system capable of in situ energy harvest and deployment in sub-sea configurations. By extracting kinetic energy from the ocean, EEL proposes to provide power output ranging from 1 mW to 1,000 mW. Such a magnitude of power can sustain active instrumentation with onboard processing of data and over-the-horizon telemetry. Pyro-E and Oak Ridge National Laboratory have utilized software tools and powerful computing resources to develop a techno-economic design of the EEL capable of harvesting 5 W. The material response of the EEL under simulated hydromechanical loads is described through time-accurate predictions. All physical tests were conducted by Pyro-E to guide simulations at Oak Ridge National Laboratory.

16 TIDAL AND WAVE POWER↗