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At least 145 records · Page 8

Data Report: UT-GOM2-1 Sediment Grain Size Measurements at Site GC 955, Holes H002 and H005

Sediment grain size measurement in marine sediments provides a record of the stratigraphic variation in grain size and thus energy regime at the time of deposition. In addition to the grain size distribution, the degree of sediment sorting can also be calculated, and together they both influence primary sediment porosity and permeability. Here we present sediment grain size results from laser diffraction particle size analysis of samples from pressure cores collected during the 2017 UT GOM2-1 Expedition. We measured both bulk sediment and organic carbon-free sediment fractions for 46 samples and organic carbon-free sediment for 5 samples at Site GC 955, Holes H002 and H005. Differences between the bulk sediment and organic carbon-free fractions reflect the relative amount and size fraction of the organic carbon. The sample results presented here represent the grain size variation of the host lithology across the Green Canyon (GC) 955 gas hydrate reservoir.

03 NATURAL GAS↗

Explosive Soot Challenge (Final Report)

This project assembled a broad ensemble of modeling and experimentation tools to study the morphological and optical properties of detonation soots in explosive fireballs. A gram-scale hemispherical high explosive was studied in a low-pressure controlled environment using in-situ experimentation with diffusely illuminated visible absorption spectroscopy, particle sizing through light scattering techniques, and post-test collections with subsequent morphological analysis. Hydrocode modeling was performed to replicate the detonation flow observations, and subsequent aerosol kinetics models provided particle size distributions and extinction coefficients from the hydrocode results. Experimentally observed soot morphologies agreed with expectation from the literature - a bimodal distribution was found, brought upon by the particles growing to a size where their inertia and fluid wakes are non-negligible. The aerosol kinetics model did not replicate the observed bimodal size distribution for lack of a coagulation kernel to represent the behavior. To recover particulate optical properties, a spectrally resolved absorption spectroscopy method termed Spectral diffuse back-illuminated extinction imaging (SBI-EI) was developed and implemented on two explosive types. Inverting the absorption spectra using a Kramers-Kronig consistent method yielded the complex index of refraction for the soots produced by the explosives. This method resulted in an unrealistic index of refraction for one of the two explosives, and this is suspected to be due to the model neglecting scattering brought upon by the large particle sizes observed. In addition to the core work, three additional studies were performed in parallel. These investigated the impact of scattering on diffuse absorption spectroscopy, studied how soots oxidate and sublimate in a well-controlled shock tube, and laid the theoretical groundwork for a new collision kernel to replicate the bimodal size distribution from the observations. Summaries of these efforts are included at the end of this report.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Framework for custom event sample augmentations for ATLAS analysis data

For HEP event processing, data is typically stored in column-wise synchronized containers, such as most prominently ROOT’s TTree, which have been used for several decades to store by now over 1 exabyte. These containers can combine row-wise association capabilities needed by most HEP event processing frameworks (e.g. Athena for ATLAS) with column-wise storage, which typically results in better compression and more efficient support for many analysis use-cases. One disadvantage is that these containers, TTree in the HEP use-case, require to contain the same attributes for each entry/row (representing events), which can make extending the list of attributes very costly in storage, even if those are only required for a small subsample of events. Since the initial design, the ATLAS software framework features powerful navigational infrastructure to allow storing custom data extensions for subsamples of events in separate, but synchronized containers. This allows adding event augmentations to ATLAS standard data products (such as DAOD-PHYS or PHYSLITE) avoiding duplication of those core data products, while limiting their size increase. For this functionality, the framework does not rely on any associations made by the I/O technology (i.e. ROOT), however it supports TTree friends and builds the associated index to allow for analysis outside of the ATLAS framework. A prototype based on the Long-Lived Particle search is implemented and preliminary results with this prototype will be presented. At this point, augmented data are stored within the same file as the core data. Storing them in separate files will be investigated in future, as this could provide more flexibility, e.g. certain sites may only want a subset of several augmentations or augmentations can be archived to tape once their analysis is complete.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Core Design Optimization of the Westinghouse Lead Fast Reactor

Westinghouse is pursuing an advanced Nuclear Power Plant design based on Lead Fast Reactor (LFR) technology for global commercialization. To achieve an optimal combination of key attributes, such as safety, sustainability, and economic competitiveness, Westinghouse and ANL partnered in developing and applying a formalized core design optimization strategy. An LFR analysis workflow was developed to automate a suite of reactor physics, fuels performance, safety, and economics simulations on a selected LFR concept. The workflow streamlines analysis of a wide range of LFR designs with different dimensions and fuel types to assess their viability and economic performance, significantly reducing human processing time and risks of processing errors. The LFR optimization exercise was defined, resulting in selection of the design constraints (geometric, neutronics, thermo-mechanical, safety, thermal-hydraulics, and economics) and performance metrics researched (minimization of both the fuels LCOE and the first core inventory cost). A total of 14 varied design parameters were considered, including assembly dimensions, coolant temperature, and enrichment distribution throughout the core. The LFR analysis workflow was connected to DAKOTA for sensitivity and optimization analyses. Due to the extremely large size of the potential LFR optimization solution space relative to the computing time required to characterize one LFR solution, a multi-stage optimization approach was proposed to breakdown the problem into several stages with more reasonable sizes. This optimization approach enabled finding various viable core solutions with different cost tradeoffs that were considered by Westinghouse and justify selection of a smaller core with multi-batch 2-year cycle length.

Stauff, Nicolas E.↗

DOE Award No.: DE-FE0023919 Phase 3 Scientific/Technical Report

This is the Phase 3 Report for the ‘Deepwater Methane Hydrate Characterization and Scientific Assessment or Genesis of Methane Hydrates in the Gulf of Mexico (GOM2)’ research project (DOE Award No. DE-FE0023919). The report summarizes activities from January 16, 2018 to September 30, 2019. The project is led by the University of Texas at Austin (UT). The objective is to gain insight into the nature, formation, occurrence and physical properties of methane hydrate-bearing sediments for the purpose of methane hydrate resource appraisal through the planning and execution of drilling, coring, logging, testing and analytical activities that assess the geologic occurrence, regional context, and characteristics of marine methane hydrate deposits in the Gulf of Mexico outer continental shelf (OCS). We determined that it would not be possible to pursue the project with the International Ocean Discovery Program (IODP) and then developed a revised science and operations plan to maximize the science using a commercial vessel within the budget that is available. We improved the scientific capability of the UT pressure core center by adding the ability to X-ray pressure cores, and the ability to cut and store multiple core samples for experimental analysis. We transferred pressure cores to peer institutions, including the National Energy Technology Lab (NETL) the United States Geological Survey (USGS Woods Hole). We made advances in understanding the composition and source of gasses locked in the methane hydrate from Green Canyon 955 (GC-955). We developed approaches to determine the in-situ salinity of hydrate-bearing samples, revealing that the in situ salinity of the GC 955 reservoir is just above that of seawater. We determined that the GC-955 hydrate reservoir is composed of sandy silt with a high concentration of hydrate interbedded with clayey silt with no hydrate present. We determined that some or all of the intervals bounding the hydrate reservoir are composed of material similar to the reservoir (sandy silt with hydrate and clayey silt with no hydrate), but with a lower net to gross. We determined that the reservoir effective permeability at a hydrate saturation of ~80-90 % is ~0.1 mD (or 1.0×10-16 m2) to ~0.5 mD (or 5.0×10-16 m2) and the intrinsic permeability is ~12 mD (or 1.2×10-14 m2). The GC-955 reservoir in-situ porosity of sandy silt is 0.38 to 0.40 and is largely independent of effective stress, and that the porosity of clayey silt is 0.33 at an in situ effective stress of 3.8 MPa to ~0.37 at zero effective stress. We developed a systematic, repeatable approach to studying hydrate reservoir properties by reconstituting individual lithofacies from dissociated pressure cores. We determined index properties of GC-955 reservoir, including liquid limit and plasticity, porosity, capillary behavior, and particle size distribution. We developed a more robust pressure coring technology. We finalized and published the UT-GOM2-1 Expedition Volume and we finalized a dedicated volume on the UT-GOM2-1 expedition that will be published in the American Association of Petroleum Geologists Bulletin (AAPG) in spring 2020.

03 NATURAL GAS↗

Markets and Economic Requirements for Fission Batteries and Other Nuclear Systems

Fission Batteries (FBs) are nuclear reactors defined by five characteristics which enable large-scale deployment: cost competitive, standardized sizes for economic mass production, easy installation and removal, secure and safe unattended operation with high reliability. FBs are not defined by technology or power level. Technical and market considerations suggest that most FBs will produce 20 to 30 MWt. This proceedings reports on the outcomes of two workshops that were held in January 2021 to better define markets and economic challenges for FBs. Three major markets were identified. The largest market is the industrial and commercial heat market. There are about 4000 industrial users (excluding utilities) that require more than one megawatt of heat. The number of customers versus size of heat demand was determined. In a low-carbon world there is the potential for many additional customers—including expanded biofuels production and district heat. The second market is for non-grid electricity. This includes co-generation plants that produce heat and electricity for a single customer. The third market is the maritime market with ~100,000 ships worldwide. In the United States, natural gas is the low-cost energy option today and will remain so unless constraints or taxes impact its use. If restrictions on greenhouse gas emissions, the FB competition includes natural gas with carbon capture, biofuels, hydrogen and grid electricity. Natural gas with carbon capture is not economically viable on a small scale. Biofuels may be expensive but may be the economically preferred option for locations with small energy demands of a few megawatts. Hydrogen is a potential competitor with many of the characteristics of natural gas. Grid electricity is not a competitive source of heat. For FBs to be economically competitive, the price of delivered heat must be $20-50/MWh ($6-15/million BTU). The economically competitive range for non-grid electricity is estimated at $70-100/MWh. These electricity prices are competitive with the retail prices of electricity in many parts of the United States for the customer. FBs are not expected to be competitive selling wholesale electricity to the grid. To achieve the aforementioned cost targets for heat and electricity markets, FB designers must (1) maximize the power output within the constraints of a FB (e.g., truck transportability, passive decay heat removal), (2) drastically reduce the size of onsite staff, (3) adopt core designs with low fuel costs (enrichment and fabrication), and (4) develop a system design that is efficiently manufactured in factories. The business case depends upon more than being just a replacement for natural gas. The largest incentives for adoption of FBs is where they create new markets and new sources of revenue. An example is the paper and pulp industry that burns biomass wastes to provide heat and electricity to make paper. An external heat source could meet the demand for heat and electricity by the paper process and enable converting waste biomass into liquid biofuels rather than burning to provide heat. Other markets, such as data centers, are driven by special energy requirements such as extreme reliability. Most customers are not in the energy business but need heat and electricity to produce a product—a manufactured good, education, retail sales (shopping malls), marine transport or some other product. As a consequence, there will be large incentives to lease rather than own FBs. Leasing avoids the regulatory challenges that remain with the owner of the FB. Leasing creates large incentives for FP standardization of sizes and transportability to maintain the value of the FB at the end of the lease—similar to the leasing of jet engines and aircraft. The economic constraints combined with technical constraints suggest competitive FBs will likely have outputs exceeding 10 MWt. There appear to be little incentives for very long-lived reactor cores because such machines require much larger inventories of fuel. Maintenance requirements and the options to provide technology updates may favor shorter lifetimes (~5 years). The assessment is that there is the potential for FBs to be economically viable and play a major role in global decarbonization in three markets: heat, non-grid electricity and maritime applications.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Apex hydrogen bonds in dendron assemblies modulate close-packed mesocrystal structures

The close-packed mesocrystal structures from soft-matter assemblies have recently received attention due to their structural similarity to atomic crystals, displaying various sphere-packing Frank–Kasper (FK) and quasicrystal structures. Herein, diverse mesocrystal structures are explored in second-generation dendrons (G2-X) designed with identical wedges, in which the terminal functionalities X = CONH 2 and CH 2 NH 2 represent two levels of the strong and weak hydrogen-bonding apexes, respectively. The cohesive interactions at the core apex, referred to as the core interactions, are effectively modulated by forming heterogeneous hydrogen bonds between these two functional units. For the dendron assemblies compositionally close to each pure component of G2-CONH 2 and G2-CH 2 NH 2 , their own FK A15 and C14 phases dominate other phases, respectively. We show the existence of the wide-range FK σ including the dodecagonal quasicrystal (DDQC) phases from the dendron mixtures between G2-CONH 2 and G2-CH 2 NH 2 , providing an experimental phase sequence of A15–σ–DDQC–C14 as the core interactions are alleviated. Intriguingly, the temperature dependence of particle sizes shows that the high plateau values of particle sizes are maintained equivalently until each threshold temperature (T th ), followed by a prompt decrease above the T th . A decrease in T th by alleviating the core interactions and its composition dependence suggest that the more size-dispersed particles, the more susceptibility to chain exchange with increasing temperature. Here our results on the formation of supramolecular dendron assemblies provide a guide to understand the core-interaction-dependent mesocrystal structures toward the fundamental principle underlying the temperature dependence of their particle sizes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Data for Spatial Analysis of Cell Patterning to Aid Genetic and Phenotypic Understanding of Grass Stomatal Density: A Case Study in Maize

Biological processes involve complex hierarchies where composite traits result from multiple component traits. However, holistically understanding of how sets of component traits interact to underpin genotype-to-phenotype relationships is generally lacking. Stomatal density (SD) is a tractable model system for exploring how high-throughput phenotyping (HTP) data could be exploited by a new spatial analysis approach to better understand a developmentally and functionally important trait. SD is a composite trait, resulting from various components related to cell identity and size, which are themselves governed by a series of spatio-developmental processes. Data from 192 recombinant inbred lines of maize [Zea mays (L.)] were analyzed by a new stomatal patterning phenotype (SPP) to (1) describe the average spatial probability distribution of the nearest neighboring stomata; (2) derive a core set of component traits related to cell size, cell packing, and positional probabilities; (3) build a structural equation model of component traits underlying SD; and (4) identify stomatal patterning quantitative trait loci (QTL). The core set of SPP-derived traits explained 74% of the variation in SD. Analyzing SPP component traits allowed some loci previously identified as generic SD QTL to be recognized as specific to lateral versus longitudinal elements of stomatal patterning. Therefore, this study highlights how novel insights can be gained by decomposing a composite trait (e.g., SD) into a set of component traits that were present in HTP data but not previously exploited.

AI/ML↗

Petrophysical and geomechanical properties of gas hydrate-bearing sediments recovered from Alaska North Slope 2018 Hydrate-01 Stratigraphic Test Well

Knowledge of petrophysical and geomechanical properties of gas hydrate-bearing sediments are essential for predicting reservoir response due to gas production from gas hydrate reservoirs. That information will be critical parameters for designing production well completion such as specification of depressurization pump, water storage tank, and mesh size of sand screen. In December 2018, Stratigraphic Test Well Hydrate-01 was drilled in the western part of the Prudhoe Bay Unit, Alaska North Slope as part of the technical planning effort for a future long-term production test by collaborative team of DOE/NETL, USGS, and MH21-S (Boswell et al., 2020, Collett et al., 2020, Okinaka et al., 2020). Data set of logging-while-drilling (LWD) were acquired (Haines et al., 2020, Suzuki et al., 2019) and core sampling depth was determined on-site.Side-wall pressure coring was conducted to recover gas hydrate-bearing sediments from two reservoir sections named Unit-B and Unit-D. A total of 34 cores were successfully recovered by 5 runs of a wire-line deployed pressure corer (CoreVault® System - Halliburton). Core analysis scheme of this project are shown in Figure 1. All cores were quenched in liquid nitrogen while at high pressure in the laboratory of Stratum Reservoir, LLC. at Anchorage (Figure 1, a)). And the cores were removed from the pressure corer autoclave with temperature support of dry ice and stored under liquid nitrogen at atmospheric pressure. 19 damaged cores were processed to index property measurements directly such as grain size, grain density. 4 of another 17 cores were depressurized and trimmed for making a plug to analyze petrophysical properties of host sediments. Unsteady-state permeability test was conducted to obtain relative water permeability to gas and core scale NMR T2 distribution measurement was performed for evaluating pore size distribution at Houston (Figure 1, b)). Remained high quality 13 cores were preserved with gas hydrate for advanced laboratory analysis. National Institute of Advanced Industrial Science and Technology, as a part of the Japanese National Hydrate Research Program (MH21-S, funded by Ministry of Economy, Trade and Industry), received the samples at Sapporo, Japan for advanced core analysis. High-resolution X-ray CT was used to analyze the quality of the samples, which showed undisturbed lithological layers. Cores were lathed into cylindrical shape and distributed for multi property measurements (Figure 1, c)).<p>As a result, sediment from Unit-D is categorized as silty sand at ~37% porosity with ~80% gas hydrate saturation. An average hydration number n = 6.16 was measured by Raman spectroscopy. An average intrinsic permeability of ~400 mD and in situ effective permeability (with hydrate) on the order of ~10 mD. The Unit B recovered cores consisted of well sorted sand at ~40% porosity with ~95% gas hydrate saturation. An average intrinsic permeability of ~1 Darcy and in situ effective permeability on the order of ~30 mD was measured for the Unit B cores. There was a small permeability reduction due to porosity loss with increasing effective stress that simulated consolidation behavior along with depressurization in the highly permeable sandy sediment. The apparent minimum change in porosity and permeability may be caused by the low compressibility of quartz sand grains in the recovered cores. XRD and thermal conductivity analysis also suggested high quartz content. Triaxial compression tests established internal friction angles based on the Mohr-Coulomb's failure criterion, which are 40° for hydrate-bearing sediment and 29.8° for hydrate free sediment.</p>

Yoneda, Jun↗

Photoelectrochemically Self Improving Si/GaN Photocathode: Figure 3c Raw Data

XPS after 0hr of chronoampometry. Surface chemical composition and valence band structure of GaN were obtained by X-ray photoemission spectroscopy (XPS) on a Kratos Axis Ultra DLD system at a takeoff angle of 0° relative to the surface normal. An Al Kα source (hν = 1486.6 eV) was used to excite the core level electrons. Pass energy of 20 eV was used for the narrow scan of core levels and valence band spectra, and step size of 0.05 eV and 0.025 eV, respectively. The Spectral fitting was conducted using CasaXPS analysis software. The binding energy scales of all core levels were corrected to the N 1s of Ga – N bond at 397.8 eV. XPS O1s core level spectra from as-received Si/GaN sample, and deconvolution shows O - Ga bond and OH - H2O bond.

photocathode↗

Photoelectrochemically Self Improving Si/GaN Photocathode: Figure 3d Raw Data

XPS of Si/GaN photocathode after 1 hour chronoamperometry (CA) testing. Surface chemical composition and valence band structure of GaN were obtained by X-ray photoemission spectroscopy (XPS) on a Kratos Axis Ultra DLD system at a takeoff angle of 0° relative to the surface normal. An Al Kα source (hν = 1486.6 eV) was used to excite the core level electrons. Pass energy of 20 eV was used for the narrow scan of core levels and valence band spectra, and step size of 0.05 eV and 0.025 eV, respectively. The Spectral fitting was conducted using CasaXPS analysis software. The binding energy scales of all core levels were corrected to the N 1s of Ga – N bond at 397.8 eV. X-ray photoemission spectroscopy (XPS) O1s core level spectra from 1 hour chronoamperometry (CA) tested Si/GaN sample, and deconvolution shows O - Ga bond, O - N - Ga bond, and OH - H2O bond.

photocathode↗

Photoelectrochemically Self Improving Si/GaN Photocathode: Figure 3f Raw Data

XPS of Si/GaN photocathode after 10 hour chronoamperometry (CA) testing. Surface chemical composition and valence band structure of GaN were obtained by X-ray photoemission spectroscopy (XPS) on a Kratos Axis Ultra DLD system at a takeoff angle of 0° relative to the surface normal. An Al Kα source (hν = 1486.6 eV) was used to excite the core level electrons. Pass energy of 20 eV was used for the narrow scan of core levels and valence band spectra, and step size of 0.05 eV and 0.025 eV, respectively. The Spectral fitting was conducted using CasaXPS analysis software. The binding energy scales of all core levels were corrected to the N 1s of Ga – N bond at 397.8 eV. XPS O1s core level spectra from 10 hours CA tested Si/GaN sample, and deconvolution shows O - Ga bond, O - N - Ga bond and OH - H2O bond.

photocathode↗

Photoelectrochemically Self Improving Si/GaN Photocathode: Figure 3e Raw Data

XPS of Si/GaN photocathode after 4 hour chronoamperometry (CA) testing. Surface chemical composition and valence band structure of GaN were obtained by X-ray photoemission spectroscopy (XPS) on a Kratos Axis Ultra DLD system at a takeoff angle of 0° relative to the surface normal. An Al Kα source (hν = 1486.6 eV) was used to excite the core level electrons. Pass energy of 20 eV was used for the narrow scan of core levels and valence band spectra, and step size of 0.05 eV and 0.025 eV, respectively. The Spectral fitting was conducted using CasaXPS analysis software. The binding energy scales of all core levels were corrected to the N 1s of Ga – N bond at 397.8 eV. XPS O1s core level spectra from 4 hour CA tested Si/GaN sample, and deconvolution shows O - Ga bond, O - N - Ga bond and OH - H2O bond.

photocathode↗

Size-dependent second-order-like phase transitions in Fe nanocluster melting from low-temperature structural isomerization

Here, in this work, the melting phase transitions of Fe n nanoclusters with 10 ≤ n ≤ 100 atoms are investigated using classical many-body molecular dynamics simulations. For many cluster sizes, surface melting occurs at much lower temperatures than core melting. Surface and core melting points and energetic melting points (temperatures of maximum heat capacity, C v ) are calculated for all cluster sizes. Melting properties are found to be strong functions of cluster structure. Cluster sizes with closed-shell structures always have first-order-like phase transitions. Almost one-third of cluster sizes in the analyzed range exhibit second-order-like phase transitions due to the presence of multiple structural configurations close in energy. 1-shell clusters with one to a few more atoms than a neighboring closed-shell structure have very low surface melting points and very high energetic melting points compared to their closed-shell counterparts. In clusters above 50 atoms with certain core structures, melting of the surface before the core was observed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices

By combining colloidal nanocrystal synthesis, self-assembly, and solution phase epitaxial growth techniques, we developed a general method for preparing single dot thick atomically attached quantum dot (QD) superlattices with high-quality translational and crystallographic orientational order along with state-of-the-art uniformity in the attachment thickness. The procedure begins with colloidal synthesis of hexagonal prism shaped core/shell QDs (e.g., CdSe/CdS), followed by liquid subphase self-assembly and immobilization of superlattices on a substrate. Solution phase epitaxial growth of additional semiconductor material fills in the voids between the particles, resulting in a QD-in-matrix structure. The photoluminescence emission spectra of the QD-in-matrix structure retains characteristic 0D electronic confinement. Importantly, annealing of the resulting structures removes inhomogeneities in the QD–QD inorganic bridges, which our atomistic electronic structure calculations demonstrate would otherwise lead to Anderson-type localization. The piecewise nature of this procedure allows one to independently tune the size and material of the QD core, shell, QD–QD distance, and the matrix material. These four choices can be tuned to control many properties (degree of quantum confinement, quantum coupling, band alignments, etc.) depending on the specific applications. Lastly, cation exchange reactions can be performed on the final QD-in-matrix, as demonstrated herein with a CdSe/CdS to HgSe/HgS conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Changes in Four Decades of Near‐CONUS Tropical Cyclones in an Ensemble of 12 km Thermodynamic Global Warming Simulations

We evaluate tropical cyclones (TCs) in a set of thermodynamic global warming (TGW) simulations over the continental United States (CONUS). A 12 km simulation forced by ERA5 provides a 40‐year historical (1980–2019) control. Four complimentary future scenarios are generated using thermodynamic deltas applied to lateral boundary, interior, and surface forcing. We curate a data set of 4,498 6‐hourly TC snapshots in the control and find a corresponding “twin” in each counterfactual, permitting a paired comparison. Warming results in an increase in mean dynamical TC intensity and moisture‐related quantities, with the latter being more pronounced. TC inner cores contract slightly but outer storm size remains unchanged. The frequency with which TCs become more intense is only moderately consistent, with snapshots having increased hazards ranging from 50% to 80% depending on warming level. The fractions of TCs undergoing rapid intensification and weakening both increase across all warming simulations, suggesting elevated short‐term intensity variability.

54 ENVIRONMENTAL SCIENCES↗

Ab initio calculations in atoms, molecules, and solids, treating spin–orbit coupling and electron interaction on an equal footing

We incorporate explicit, non-perturbative treatment of spin–orbit coupling into ab initio auxiliary-field quantum Monte Carlo (AFQMC) calculations. The approach allows a general computational framework for molecular and bulk systems in which material specificity, electron correlation, and spin–orbit coupling effects can be captured accurately and on an equal footing, with favorable computational scaling vs system size. We adopt relativistic effective-core potentials that have been obtained by fitting to fully relativistic data and that have demonstrated a high degree of reliability and transferability in molecular systems. This results in a two-component spin-coupled Hamiltonian, which is then treated by generalizing the ab initio AFQMC approach. We demonstrate the method by computing the electron affinity in Pb, the bond dissociation energy in Br 2 and I 2 , and solid Bi.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗