Abstract: Due to a beneficial balance of computational cost and accuracy, real-time time-dependent density-functional theory has emerged as a promising first-principles framework to describe electron real-time dynamics. Here we discuss recent implementations around this approach, in particular in the context of complex, extended systems. Results include an analysis of the computational cost associated with numerical propagation and when using absorbing boundary conditions. We extensively explore the shortcomings for describing electron–electron scattering in real time and compare to many-body perturbation theory. Modern improvements of the description of exchange and correlation are reviewed. In this work, we specifically focus on the Qb@ll code, which we have mainly used for these types of simulations over the last years, and we conclude by pointing to further progress needed going forward. Graphical abstract: [Figure not available: see fulltext.].
Soil organic carbon (SOC) changes under future climate warming are difficult to quantify in situ. Here we apply an innovative approach combining space-for-time substitution with meta-analysis to SOC measurements in 113,013 soil profiles across the globe to estimate the effect of future climate warming on steady-state SOC stocks. We find that SOC stock will reduce by 6.0 ± 1.6% (mean±95% confidence interval), 4.8 ± 2.3% and 1.3 ± 4.0% at 0–0.3, 0.3–1 and 1–2 m soil depths, respectively, under 1 °C air warming, with additional 4.2%, 2.2% and 1.4% losses per every additional 1 °C warming, respectively. The largest proportional SOC losses occur in boreal forests. Existing SOC level is the predominant determinant of the spatial variability of SOC changes with higher percentage losses in SOC-rich soils. Our work demonstrates that warming induces more proportional SOC losses in topsoil than in subsoil, particularly from high-latitudinal SOC-rich systems.
This report updates the Regional Disruption Economic Impact Model (RDEIM) GDP-based model described in Bixler et al. (2020) used in the MACCS accident consequence analysis code. MACCS is the U.S. Nuclear Regulatory Commission (NRC) used to perform probabilistic health and economic consequence assessments for atmospheric releases of radionuclides. It is also used by international organizations, both reactor owners and regulators. It is intended and most commonly used for hypothetical accidents that could potentially occur in the future rather than to evaluate past accidents or to provide emergency response during an ongoing accident. It is designed to support probabilistic risk and consequence analyses and is used by the NRC, U.S. nuclear licensees, the Department of Energy, and international vendors, licensees, and regulators. The update of the RDEIM model in version 4.2 expresses the national recovery calculation explicitly, rather than implicitly as in the previous version. The calculation of the total national GDP losses remains unchanged. However, anticipated gains from recovery are now allocated across all the GDP loss types – direct, indirect, and induced – whereas in version 4.1, all recovery gains were accounted for in the indirect loss type. To achieve this, we’ve introduced new methodology to streamline and simplify the calculation of all types of losses and recovery. In addition, RDEIM includes other kinds of losses, including tangible wealth. This includes loss of tangible assets (e.g., depreciation) and accident expenditures (e.g., decontamination). This document describes the updated RDEIM economic model and provides examples of loss and recovery calculation, results analysis, and presentation. Changes to the tangible cost calculation and accident expenditures are described in section 2.2. The updates to the RDEIM input-output (I-O) model are not expected to affect the final benchmark results Bixler et al. (2020), as the RDEIM calculation for the total national GDP losses remains unchanged. The reader is referred to the MACCS revision history for other cost modelling changes since version 4.0 that may affect the benchmark. RDEIM has its roots in a code developed by Sandia National Laboratories for the Department of Homeland Security to estimate short-term losses from natural and manmade accidents, called the Regional Economic Accounting analysis tool (REAcct). This model was adapted and modified for MACCS. It is based on I-O theory, which is widely used in economic modeling. It accounts for direct losses to a disrupted region affected by an accident, indirect losses to the national economy due to disruption of the supply chain, and induced losses from reduced spending by displaced workers. RDEIM differs from REAcct in in its treatment and estimation of indirect loss multipliers, elimination of double-counting associated with inter-industry trade in the affected area, and that it is intended to be used for extended periods that can occur from a major nuclear reactor accident, such as the one that occurred at the Fukushima Daiichi site in Japan. Most input-output models do not account for economic adaptation and recovery, and in this regard RDEIM differs from its parent, REAcct, because it allows for a user-definable national recovery period. Implementation of a recovery period was one of several recommendations made by an independent peer review panel to ensure that RDEIM is state-of-practice. For this and several other reasons, RDEIM differs from REAcct.
This study explores the effect of surface re-finishing on the corrosion behavior of electron beam manufactured (EBM) Ti-G5 (Ti-6Al-4V), including the novel application of an electron beam surface remelting (EBSR) technique. Specifically, the relationship between material surface roughness and corrosion resistance was examined. Surface roughness was tested in the as-printed (AP), mechanically polished (MP), and EBSR states and compared to wrought (WR) counterparts. Electrochemical measurements were performed in chloride-containing media. It was observed that surface roughness, rather than differences in the underlying microstructure, played a more significant role in the general corrosion resistance in the environment explored here. While both MP and EBSR methods reduced surface roughness and enhanced corrosion resistance, mechanical polishing has many known limitations. The EBSR process explored herein demonstrated positive preliminary results. The surface roughness (Ra) of the EBM-AP material was considerably reduced by 82%. Additionally, the measured corrosion current density in 0.6 M NaCl for the EBSR sample is 0.05 µA cm−2, five times less than the value obtained for the EBM-AP specimen (0.26 µA cm−2).
The extreme miniaturization of a cold-atom interferometer accelerometer requires the development of novel technologies and architectures for the interferometer subsystems. Here, we describe several component technologies and a laser system architecture to enable a path to such miniaturization. We developed a custom, compact titanium vacuum package containing a microfabricated grating chip for a tetrahedral grating magneto-optical trap (GMOT) using a single cooling beam. In addition, we designed a multi-channel photonic-integrated-circuit-compatible laser system implemented with a single seed laser and single sideband modulators in a time-multiplexed manner, reducing the number of optical channels connected to the sensor head. In a compact sensor head containing the vacuum package, sub-Doppler cooling in the GMOT produces 15 μK temperatures, and the GMOT can operate at a 20 Hz data rate. We validated the atomic coherence with Ramsey interferometry using microwave spectroscopy, then demonstrated a light-pulse atom interferometer in a gravimeter configuration for a 10 Hz measurement data rate and T = 0–4.5 ms interrogation time, resulting in Δg/g = 2.0 × 10−6. This work represents a significant step towards deployable cold-atom inertial sensors under large amplitude motional dynamics.
This report provides recommendations to improve the assessment method of the Federal Radiological Monitoring and Assessment Center (FRMAC) for the ingestion of crops contaminated with radionuclides. The current FRMAC method of calculating investigation levels (ILs) and crop derived response levels (DRLs) is detailed. Recommended modifications to these calculations are presented based on the following aspects: handling radionuclide mixtures, no immediate equilibrium, washing of contaminated crops, and updated dietary intake rates.
The Strategic Petroleum Reserve (SPR) is the world's largest supply of emergency crude oil. The reserve consists of four sites in Louisiana and Texas. Each site stores crude in deep, underground salt caverns. It is the mission of the SPR's Enhanced Monitoring Program to examine all available data to inform our understanding of each site. This report discusses the monitoring data, processes, and results for each of the four sites for fiscal year 2022.
Integrated computational materials engineering (ICME) models have been a crucial building block for modern materials development, relieving heavy reliance on experiments and significantly accelerating the materials design process. However, ICME models are also computationally expensive, particularly with respect to time integration for dynamics, which hinders the ability to study statistical ensembles and thermodynamic properties of large systems for long time scales. To alleviate the computational bottleneck, we propose to model the evolution of statistical microstructure descriptors as a continuous-time stochastic process using a non-linear Langevin equation, where the probability density function (PDF) of the statistical microstructure descriptors, which are also the quantities of interests (QoIs), is modeled by the Fokker-Planck equation. We discuss how to calibrate the drift and diffusion terms of the Fokker-Planck equation from the theoretical and computational perspectives. The calibrated Fokker-Planck equation can be used as a stochastic reduced-order model to simulate the microstructure evolution of statistical microstructure descriptors PDF. Considering statistical microstructure descriptors in the microstructure evolution as QoIs, we demonstrate our proposed methodology in three integrated computational materials engineering (ICME) models: kinetic Monte Carlo, phase field, and molecular dynamics simulations.
Mobile sources is a term most commonly used to describe radioactive sources that are used in applications requiring frequent transportation. Such radioactive sources are in common use world-wide where typical applications include radiographic non-destructive evaluation (NDE) and oil and gas well logging, among others requiring lesser amounts of radioactivity. This report provides a general overview of mobile sources used for well logging and industrial radiography applications including radionuclides used, equipment, and alternative technologies. Information presented here has been extracted from a larger study on common mobile radiation sources and their use.
The growing demand for bandwidth makes photonic systems a leading candidate for future telecommunication and radar technologies. Integrated photonic systems offer ultra-wideband performance within a small footprint, which can naturally interface with fiber-optic networks for signal transmission. However, it remains challenging to realize narrowband (∼MHz) filters needed for high-performance communications systems using integrated photonics. In this paper, we demonstrate all-silicon microwave-photonic notch filters with 50× higher spectral resolution than previously realized in silicon photonics. This enhanced performance is achieved by utilizing optomechanical interactions to access long-lived phonons, greatly extending available coherence times in silicon. We use a multi-port Brillouin-based optomechanical system to demonstrate ultra-narrowband (2.7 MHz) notch filters with high rejection (57 dB) and frequency tunability over a wide spectral band (6 GHz) within a microwave-photonic link. We accomplish this with an all-silicon waveguide system, using CMOS-compatible fabrication techniques.
Hydrogen is an attractive option for energy storage because it can be produced from renewable sources and produces environmentally benign byproducts. However, the volumetric energy density of molecular hydrogen at ambient conditions is low compared to other storage methods like batteries, so it must be compressed to attain a viable energy density for applications such as transportation. Nanoporous materials have attracted significant interest for gas storage because they can attain high storage density at lower pressure than conventional compression. In this work, we examine how to improve the cryogenic hydrogen storage capacity of a series of porous aromatic frameworks (PAFs) by controlling the pore size and increasing the surface area by adding functional groups. We also explore tradeoffs in gravimetric and volumetric measures of the hydrogen storage capacity and the effects of temperature swings using grand canonical Monte Carlo simulations. We also consider the effects of adding functional groups to the metal–organic framework NU-1000 to improve its hydrogen storage capacity. We find that highly flexible alkane chains do not improve the hydrogen storage capacity in NU-1000 because they do not extend into the pores; however, rigid chains containing alkyne groups do increase the surface area and hydrogen storage capacity. Finally, we demonstrate that the deliverable capacity of hydrogen in NU-1000 can be increased from 40.0 to 45.3 g/L (at storage conditions of 100 bar and 77 K and desorption conditions of 5 bar and 160 K) by adding long, rigid alkyne chains into the pores.
The effect of crystallography on transgranular chloride-induced stress corrosion cracking (TGCISCC) of arc welded 304L austenitic stainless steel is studied on >300 grains along crack paths. Schmid and Taylor factor mismatches across grain boundaries (GBs) reveal that cracks propagate either from a hard to soft grain, which can be explained merely by mechanical arguments, or soft to hard grain. In the latter case, finite element analysis reveals that TGCISCC will arrest at GBs without sufficient mechanical stress, favorable crystallographic orientations, or crack tip corrosion. GB type does not play a significant role in determining TGCISCC cracking behavior nor susceptibility. TGCISCC crack behaviors at GBs are discussed in the context of the competition between mechanical, crystallographic, and corrosion factors.
Advances in machine learning (ML) have enabled the development of interatomic potentials that promise the accuracy of first principles methods and the low-cost, parallel efficiency of empirical potentials. However, ML-based potentials struggle to achieve transferability, i.e., provide consistent accuracy across configurations that differ from those used during training. In order to realize the promise of ML-based potentials, systematic and scalable approaches to generate diverse training sets need to be developed. This work creates a diverse training set for tungsten in an automated manner using an entropy optimization approach. Subsequently, multiple polynomial and neural network potentials are trained on the entropy-optimized dataset. A corresponding set of potentials are trained on an expert-curated dataset for tungsten for comparison. The models trained to the entropy-optimized data exhibited superior transferability compared to the expert-curated models. Furthermore, the models trained to the expert-curated set exhibited a significant decrease in performance when evaluated on out-of-sample configurations.
Spin–orbit effects, inherent to electrons confined in quantum dots at a silicon heterointerface, provide a means to control electron spin qubits without the added complexity of on-chip, nanofabricated micromagnets or nearby coplanar striplines. Here, we demonstrate a singlet–triplet qubit operating mode that can drive qubit evolution at frequencies in excess of 200 MHz. This approach offers a means to electrically turn on and off fast control, while providing high logic gate orthogonality and long qubit dephasing times. We utilize this operational mode for dynamical decoupling experiments to probe the charge noise power spectrum in a silicon metal-oxide-semiconductor double quantum dot. In addition, we assess qubit frequency drift over longer timescales to capture low-frequency noise. We present the charge noise power spectral density up to 3 MHz, which exhibits a 1/fα dependence consistent with α ~ 0.7, over 9 orders of magnitude in noise frequency.
Although gold remains a preferred surface finish for components used in high-reliability electronics, rapid developments in this area have left a gap in the fundamental understanding of solder joint gold (Au) embrittlement. Furthermore, as electronic designs scale down in size, the effect of Au content is not well understood on increasingly smaller solder interconnections. As a result, previous findings may have limited applicability. The current study focused on addressing these gaps by investigating the interfacial microstructure that evolves in 63Sn-37Pb solder joints as a function of Au layer thickness. Those findings were correlated to the mechanical performance of the solder joints. Increasing the initial Au concentration decreased the mechanical strength of a joint, but only to a limited degree. Kirkendall voids were the primary contributor to low-strength joints, while brittle fracture within the intermetallic compounds (IMC) layers is less of a factor. The Au embrittlement mechanism appears to be self-limiting, but only once mechanical integrity is degraded. Sufficient void evolution prevents continued diffusion from the remaining Au.
The interaction of an intense laser with a solid foil target can drive ∼ TV/m electric fields, accelerating ions to MeV energies. In this study, we experimentally observe that structured targets can dramatically enhance proton acceleration in the target normal sheath acceleration regime. At the Texas Petawatt Laser facility, we compared proton acceleration from a 1μm flat Ag foil, to a fixed microtube structure 3D printed on the front side of the same foil type. A pulse length (140–450 fs) and intensity ((4–10) × 10 20 W/cm2) study found an optimum laser configuration (140 fs, 4 × 10 20 W/cm2), in which microtube targets increase the proton cutoff energy by 50% and the yield of highly energetic protons (> 10 MeV) by a factor of 8×. When the laser intensity reaches 10 21 W/cm2, the prepulse shutters the microtubes with an overcritical plasma, damping their performance. 2D particle-in-cell simulations are performed, with and without the preplasma profile imported, to better understand the coupling of laser energy to the microtube targets. The simulations are in qualitative agreement with the experimental results, and show that the prepulse is necessary to account for when the laser intensity is sufficiently high.
Picuris Pueblo is a small tribal community in Northern New Mexico consisting of about 306 members and 86 homes. Picuris Pueblo has made advances with renewable energy implementation, including the installation of a 1 megawatt photovoltaic (PV) array. This array has provided the tribe with economic and other benefits that contribute toward the tribe's goal of tribal sovereignty. The tribe is seeking to implement more PV generation as well as battery energy storage systems. Picuris Pueblo is considering different implementation methods, including the formation of a microgrid system. This report studies the potential implementation of a PV and battery storage microgrid system and the associated benefits and challenges. The benefits of a microgrid system include cost savings, increased resiliency, and increased tribal sovereignty and align with the tribe's goals of becoming energy independent and lowering the cost of electricity.
Clays are known for their small particle sizes and complex layer stacking. We show here that the limited dimension of clay particles arises from the lack of long-range order in low-dimensional systems. Because of its weak interlayer interaction, a clay mineral can be treated as two separate low-dimensional systems: a 2D system for individual phyllosilicate layers and a quasi-1D system for layer stacking. The layer stacking or ordering in an interstratified clay can be described by a 1D Ising model while the limited extension of individual phyllosilicate layers can be related to a 2D Berezinskii–Kosterlitz–Thouless transition. This treatment allows for a systematic prediction of clay particle size distributions and layer stacking as controlled by the physical and chemical conditions for mineral growth and transformation. Clay minerals provide a useful model system for studying a transition from a 1D to 3D system in crystal growth and for a nanoscale structural manipulation of a general type of layered materials.
Migration of seismic events to deeper depths along basement faults over time has been observed in the wastewater injection sites, which can be correlated spatially and temporally to the propagation or retardation of pressure fronts and corresponding poroelastic response to given operation history. The seismicity rate model has been suggested as a physical indicator for the potential of earthquake nucleation along faults by quantifying poroelastic response to multiple well operations. Our field-scale model indicates that migrating patterns of 2015–2018 seismicity observed near Venus, TX are likely attributed to spatio-temporal evolution of Coulomb stressing rate constrained by the fault permeability. Even after reducing injection volumes since 2015, pore pressure continues to diffuse and steady transfer of elastic energy to the deep fault zone increases stressing rate consistently that can induce more frequent earthquakes at large distance scales. Sensitivity tests with variation in fault permeability show that (1) slow diffusion along a low-permeability fault limits earthquake nucleation near the injection interval or (2) rapid relaxation of pressure buildup within a high-permeability fault, caused by reducing injection volumes, may mitigate the seismic potential promptly.
Hydrogen produced through low-temperature water electrolysis using anion exchange membranes (AEM) combines the benefits of liquid-electrolyte alkaline electrolysis and solid-polymer proton exchange membrane electrolysis. The anion conductive ionomers in the oxygen-producing anode and hydrogen-producing cathode are a critical part of the three-dimensional electrodes. The ionomer in the hydrogen-producing cathode facilitates hydroxide ion conduction from the cathode catalyst to the anode catalyst, and water transport from the anode to the cathode catalyst through the AEM. This ionomer also binds the catalyst particles to the porous transport layer. In this study, the cathode durability was improved by use of a self-adhesive cathode ionomer to chemically bond the cathode catalyst particles to the porous transport layer. It was found that the cathode ionomers with high ion exchange capacity (IEC) were more effective than low IEC ionomers because of the need to transport water to the cathode catalyst and transport hydroxide away from the cathode. The cathode durability was improved by using ionomers which were soluble in the spray-coated cathode ink. Optimization of the catalyst and ionomer content within the cathode led to electrolysis cells which were both mechanically durable and operated at low voltage.
As part of the project “Designing Resilient Communities (DRC): A Consequence-Based Approach for Grid Investment,” funded by the United States (US) Department of Energy’s (DOE) Grid Modernization Laboratory Consortium (GMLC), Sandia National Laboratories (Sandia) is partnering with a variety of government, industry, and university participants to develop and test a framework for community resilience planning focused on modernization of the electric grid. This report provides a summary of the section of the project focused on hardware demonstration of “resilience nodes” concept.
We report the method-of-moments implementation of the electric-field integral equation (EFIE) yields many code-verification challenges due to the various sources of numerical error and their possible interactions. Matters are further complicated by singular integrals, which arise from the presence of a Green's function. To address these singular integrals, an approach is presented in wherein both the solution and Green's function are manufactured. Because the arising equations are poorly conditioned, they are reformulated as a set of constraints for an optimization problem that selects the solution closest to the manufactured solution. In this paper, we demonstrate how, for such practically singular systems of equations, computing the truncation error by inserting the exact solution into the discretized equations cannot detect certain orders of coding errors. On the other hand, the discretization error from the optimal solution is a more sensitive metric that can detect orders less than those of the expected convergence rate.
Shuttling ions at high speed and with low motional excitation is essential for realizing fast and high-fidelity algorithms in many trapped-ion-based quantum computing architectures. Achieving such performance is challenging due to the sensitivity of an ion to electric fields and the unknown and imperfect environmental and control variables that create them. Here we implement a closed-loop optimization of the voltage waveforms that control the trajectory and axial frequency of an ion during transport in order to minimize the final motional excitation. The resulting waveforms realize fast round-trip transport of a trapped ion across multiple electrodes at speeds of 0.5 electrodes per microsecond (35 m·s−1 for a one-way transport of 210 μm in 6 μs) with a maximum of 0.36 ± 0.08 mean quanta gain. This sub-quanta gain is independent of the phase of the secular motion at the distal location, obviating the need for an electric field impulse or time delay to eliminate the coherent motion.
Heavy metals released from kerogen to produced water during oil/gas extraction have caused major enviromental concerns. To curtail water usage and production in an operation and to use the same process for carbon sequestration, supercritical CO2 (scCO2) has been suggested as a fracking fluid or an oil/gas recovery agent. It has been shown previously that injection of scCO2 into a reservoir may cause several chemical and physical changes to the reservoir properties including pore surface wettability, gas sorption capacity, and transport properties. Using molecular dynamics simulations, we here demonstrate that injection of scCO2 might lead to desorption of physically adsorbed metals from kerogen structures. This process on one hand may impact the quality of produced water. On the other hand, it may enhance metal recovery if this process is used for in-situ extraction of critical metals from shale or other organic carbon-rich formations such as coal.