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DOE OSTI2024

Liquid Structure of Iron and Iron–Nitrogen–Carbon Alloys Within the Cores of Small Terrestrial Bodies

Abstract Nitrogen has been proposed to be stored within planetary cores, but its effects on the structure and density of molten Fe–alloys have not been explored experimentally. Using energy‐dispersive X‐ray diffraction, we determined the structure of Fe–N(–C) liquids at core conditions (1–7 GPa and 1700–1900°C) within a Paris‐Edinburgh press. Variation of N up to 7 wt.% and C up to 1.5 wt.% results in near‐linear changes in Fe–Fe atom distances and structure factor with increasing light element content. We did not observe a significant pressure‐driven structural transition in Fe–N(–C) liquids. We model the expansion of the Fe–Fe bonds using a modified Birch‐Murnaghan equation of state. With this model, we demonstrate that N or C contamination could lead to an overestimation of the Fe–Fe distances of pure Fe. We observe that the incorporation of 1 wt.% N or C into Fe results in a change in Fe–Fe distances that is twice as significant as the effect of 1 GPa. By approximating the change in volume, we infer that N and C incorporated in liquid iron could contribute to the density deficit observed in the cores of terrestrial bodies.

Pease, Allison [Department of Earth and Environmen↗

DOE OSTI2023

Unraveling H2 chemisorption and physisorption on metal decorated graphene using quantum Monte Carlo

Molecular hydrogen has the potential to significantly reduce the use of carbon dioxide emitting energy processes. However, hydrogen gas storage is a major bottleneck for its large-scale use as current storage methods are energy intensive. Among different storage methods, physisorbing molecular hydrogen at ambient pressure and temperatures is a promising alternative—particularly in light of the advancements in tunable lightweight nanomaterials and high throughput screening methods. Nonetheless, understanding hydrogen adsorption in well-defined nanomaterials remains experimentally challenging and reference information is scarce despite the proliferation of works predicting hydrogen adsorption. We focus on Li, Na, Ca, and K, decorated graphene sheets as substrates for molecular hydrogen adsorption, and compute the most accurate adsorption energies available to date using quantum diffusion Monte Carlo (DMC). Building on our previous insights at the density functional theory (DFT) level, we find that a weak covalent chemisorption of molecular hydrogen, known as Kubas interaction, is feasible on Ca decorated graphene according to DMC, in agreement with DFT. This finding is in contrast to previous DMC predictions of the 4H2/Ca+ gas cluster (without graphene) where chemisorption is not favored. However, we find that the adsorption energy of hydrogen on metal decorated graphene according to a widely used DFT method is not fully consistent with DMC. The reference adsorption energies reported herein can be used to find better work-horse methods for application in large-scale modeling of hydrogen adsorption. Furthermore, the implications of this work affect strategies for finding suitable hydrogen storage materials and high-throughput methods.

Chemistry↗

DOE OSTI2024

X-ray spectroscopic investigation of crystal fields in Ce 2 Rh 1 − x Ir x In 8 heavy fermions

The higher dimensionality in the crystal fields of the Ce 2 M In 8 ( M = Rh , Ir ) compounds and its interplay with hybridization and disorder are key ingredients to understand the complex phase diagrams by this family, which have been explored extensively by macroscopic techniques. Here, we present an investigation of the crystal-electric field schemes of Ce 2 Rh 1 − x Ir x In 8 using x-ray absorption spectroscopy. Our full multiplet calculations for the 4 f 1 configuration of Ce 3 + to describe the temperature-dependent linear dichroism in Ce 2 M In 8 are consistent with a Γ 7 1 = 1 − α 2 · | ∓ 3 2 〉 − | α | · | ± 5 2 〉 ground state containing a predominant | ± 3 / 2 〉 contribution that increases further with x . This enhancement is believed to favor superconductivity in Ce-based heavy fermion materials, observed in previous results in the Ce M In 5 family. Our recent observations shed light on the unexpected emergence of the ambient-pressure superconducting dome in the center of the composition phase diagram and its subsequent suppression on the Ir-rich side due to the early onset of fluctuations associated with the structurally more disordered state, inferred from previous neutron magnetic diffraction experiments. Published by the American Physical Society 2024

Christovam, D. S. (ORCID:0000000250698107)↗

DOE OSTI2022

Modularity-at-scale for advanced reactors presentation

Modularity options have been limited for traditional nuclear energy deployment due to the conventional light water reactor (LWR) safety requirements, such as high pressure retaining heavy and robust containment structures. However, a relatively new regulatory approach called ‘Functional Containment’ has potential to allow less expensive and more flexible designs for non-LWRs. Functional containment provides flexibility in design and deployment based on risk-informed and performance-based criteria, so that reactors are not over-designed. Non-nuclear industry has successfully used modular design approaches in automotive, aerospace, chemical processing, building construction, and ship building. These industries have shown that modular construction reduces construction time by around 30% - 50% compared to the conventional stick-built approach. The nuclear industry can use similar approaches to reduce construction time and costs, balanced with safety requirements, using the functional containment approach. This paper discussing the background of modularity in nuclear energy, examples of less learned, modularity approaches in non-nuclear industries and the potential of cost and schedule savings through the emerging regulatory design flexibilities potentially enabling combination of modular deployment at different scales.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

MODULARITY-AT-SCALE FOR COST COMPETITIVE DEPLOYMENT OF NUCLEAR ENERGY

Modularity options have been limited for traditional nuclear energy deployment due to the conventional light water reactor (LWR) safety requirements, such as high pressure retaining heavy and robust containment structures. However, a relatively new regulatory approach called ‘Functional Containment’ has potential to allow less expensive and more flexible designs for non LWRs. Functional containment provides flexibility in design and deployment based on risk informed and performance-based criteria, so that reactors are not over-designed. Non-nuclear industry has successfully used modular design approaches in automotive, aerospace, chemical processing, building construction, and ship building. These industries have shown that modular construction reduces construction time by around 30% - 50% compared to the conventional stick built approach. The nuclear industry can use similar approaches to reduce construction time and costs, balanced with safety requirements, using the functional containment approach. This paper discussing the background of modularity in nuclear energy, examples of less learned, modularity approaches in non-nuclear industries and the potential of cost and schedule savings through the emerging regulatory design flexibilities potentially enabling combination of modular deployment at different scales.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2021

Assessing Forest Level Response to the Death of a Dominant Tree within a Premontane Tropical Rainforest

Small-scale treefall gaps are among the most important forms of forest disturbance in tropical forests. These gaps expose surrounding trees to more light, promoting rapid growth of understory plants. However, the effects of such small-scale disturbances on the distribution of plant water use across tree canopy levels are less known. To address this, we explored plant transpiration response to the death of a large emergent tree, Mortoniodendron anisophyllum Standl. & Steyerm (DBH > 220 cm; height ~40 m). Three suppressed, four mid-story, and two subdominant trees were selected within a 50 × 44 m premontane tropical forest plot at the Texas A&M Soltis Center for Research and Education located in Costa Rica. We compared water use rates of the selected trees before (2015) and after (2019) the tree gap using thermal dissipation sap flow sensors. Hemispherical photography indicated a 40% increase in gap fraction as a result of changes in canopy structure after the treefall gap. Micrometeorological differences (e.g., air temperature, relative humidity, and vapor pressure deficit (VPD)) could not explain the observed trends. Rather, light penetration, as measured by sensors within the canopy, increased significantly in 2019. One year after the tree fell, the water usage of trees across all canopy levels increased modestly (15%). Moreover, average water usage by understory trees increased by 36%, possibly as a result of the treefall gap, exceeding even that of overstory trees. These observations suggest the possible reallocation of water use between overstory and understory trees in response to the emergent tree death. With increasing global temperatures and shifting rainfall patterns increasing the likelihood of tree mortality in tropical forests, there is a greater need to enhance our understanding of treefall disturbances that have the potential to redistribute resources within forests.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Data Science and Computation for Rapid and Dynamic Compression Experiment Workflows at Experimental Facilities, September 8-11, 2020. Workshop Report

The application of high pressure to materials has enabled discoveries in scientific fields such as planetary science, materials science, and materials synthesis. Recent advances in X-ray user light sources and other facilities, co-location and integration of user facilities with high-pressure drivers, availability of high-performance computing (HPC) platforms, and the development of new data science techniques have created opportunities for, and challenges in, advancing data analytics for rapid and dynamic compression experiments. To address these challenges, harness the emerging technology now available, and expedite scientific discovery, Los Alamos National Laboratory (LANL) hosted a virtual workshop entitled “Data Science and Computation for Rapid and Dynamic Compression Workflows at Experimental Facilities” from September 8 to 11, 2020. The workshop included 95 registered scientists and analytics experts from 15 universities, 9 United States (US) national laboratories, 5 US and European X-ray light sources, neutron sources such as the Los Alamos Neutron Science Center (LANSCE), other big science facilities such as the National Ignition Facility (NIF), and an industry representative. The workshop included 31 invited talks and 4 lightning talks by students and postdocs.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Hanover LED Streetlight Conversion

On May 8, 2017, Hanover residents voted overwhelmingly to transition to 100% renewable electricity by 2030 and heating, cooling and transportation by 2050. In so doing, we became the first municipality in the country to make this commitment by popular vote. To accomplish these goal town leaders developed a plan to address first transitioning municipal energy uses to renewable forms of energy, through on-site generation of the municipal electrical load, load reduction through energy efficiency improvements to town facilities and infrastructure. Significant progress has been accomplished in the generation of energy with 90%+ of the 2024 municipal load being offset by generation and through various energy efficiency projects. The utility owned street lighting was identified as a large energy consumer of 165 MWh annually (7% of the annual municipal load) due to old inefficient high-pressure sodium and mercury vapor streetlights with no ability to reduce wattage during periods with low lighting needs. The Hanover LED Streetlight Replacement Project replaced utility owned streetlights with town owned controllable (dimmable and trimmable) LED lights that can be adjusted by location and time of night. Coupled with ownership of the streetlights transfer to the town, the town’s share of the project pay back is 11 months and for the complete project including federal share the payback is approximately 3 years. With the completion of lighting upgrade, the annual streetlighting energy load has dropped by 60% to 67 MWh in the first year of operation (7/1/24 - 6/30/25). This amounts to an approximate $90,000 annual savings or a local 1% tax rate impact. Additionally, over 200,000 pounds of CO2 will be saved annually.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2023

Near-MHz temperature and H 2 O measurements in post-detonation fireballs of 25 g hemispherical explosives using scanned-wavelength-modulation spectroscopy

A laser absorption spectroscopy diagnostic integrated within a hardened optical probe was used to measure temperature and water mole fraction at 500 kHz in post-detonation fireballs of explosives. In the experiments, an exploding-bridgewire detonator initiated a 25 g hemisphere of explosive (N5 or PETN). This produced a hemispherical fireball that traveled radially towards a hardened measurement probe. The probe contained a pressure transducer and optical equipment to pitch fiber-coupled laser light across a 12.6 cm gap onto a detector. Tunable diode lasers emitting near 7185.6 and 6806 c m − <#comment/> 1 were used to measure the absorbance spectrum of H 2 O utilizing peak-picking scanned-wavelength-modulation spectroscopy with a scan frequency of 500 kHz and modulation frequencies of 35 and 45.5 MHz, respectively. This enabled measurements of temperature and X H 2 O in the shock-heated air and trailing fireball at 500 kHz. Time histories of pressure, temperature, and H 2 O mole fraction were acquired at different standoff distances to quantify how the fireball evolved in space and time as well as to compare measured quantities between PETN and N5 fireballs. The standard deviation of temperature and X H 2 O during one representative test were found to be 17 K (1.3%) and 0.011 (5%), respectively. These measurements demonstrate this diagnostic’s ability to provide rapid and reliable measurements in harsh, highly transient post-detonation environments produced by solid explosives.

Schwartz, Charles J.↗

DOE OSTI2021

Density of Fe-Ni-C Liquids at High Pressures and Implications for Liquid Cores of Earth and the Moon

The presence of light elements in the metallic cores of the Earth, the Moon, and other rocky planetary bodies has been widely proposed. Carbon is among the top candidates in light of its high cosmic abundance, siderophile nature, and ubiquity in iron meteorites. It is, however, still controversial whether carbon-rich core compositional models can account for the seismic velocity observations within the Earth and lunar cores. In this paper we report the density and elasticity of Fe 90 Ni 10 -3 wt.% C and Fe 90 Ni 10 -5 wt.% C liquid alloys using synchrotron-based X-ray absorption experiments and first-principles molecular dynamics simulations. Our results show that alloying of 3 wt.% and 5 wt.% C lowers the density of Fe 90 Ni 10 liquid by ~2.9-3.1% at 2 GPa, and ~3.4-3.6% at 9 GPa. More intriguingly, our experiments and simulations both demonstrate that the bulk moduli of the Fe-Ni-C liquids are similar to or slightly higher than those of Fe-Ni liquids. Thus, the calculated compressional velocity ($v_p$) of Fe-Ni-C liquids are higher than that of pure Fe-Ni alloy, promoting carbon as a possible candidate to explain the elevated v p in the Earth's outer core. However, the values and slopes of both density and v p of the studied two Fe-Ni-C liquids do not match the outer core seismic models, suggesting that carbon may not be the sole principal light element in Earth's outer core. The high $v_p$ of Fe-Ni-C liquids does not match the presumptive $v_p$ of the lunar outer core well, indicating that carbon is less likely to be its dominant light element.

58 GEOSCIENCES↗

DOE OSTI2021

Effects of Hydrogen on the Phase Relations in Fe-FeS at Pressures of Mars-Sized Bodies

The large radius, and therefore low density, of the Martian core found in the InSight mission data analysis highlights the importance of considering other light elements besides sulfur (S), which has been considered as the main light element for Mars for decades. Hydrogen (H) is abundant in the solar system and becomes siderophile at high pressures. Although Fe-S and Fe-H systems have been studied individually, the Fe-S-H ternary system has only been investigated up to 16 GPa and 1723 K. We have investigated the Fe-S-H system at pressures and temperatures (P-T) relevant to the cores of Mars-sized planets (up to 45 GPa and well above the melting temperature of FeS) in the laser-heated diamond anvil cell combined with in situ synchrotron X-ray diffraction. Here we found that sufficient hydrogen leads to the disappearance of Fe 3 S at high P-T. Instead, separate Fe-H and Fe-S phases appear at 23–35 GPa. At pressures above 35 GPa, we found a new phase appearing while Fe-S phases disappear and Fe-H phases remain. Our analysis indicates that the new phase likely contains both S and H in the crystal structure (tentatively FeS x H y where x ≈ 1 and y ≈ 1). The observed pressure-dependent changes in the phase relation may be important for understanding the structure and dynamics of the Martian core and the cores of Mars-sized exoplanets.

58 GEOSCIENCES↗

DOE OSTI2022

A mortar thermomechanical contact computational framework for nuclear fuel performance simulation

Nuclear fuel performance simulations involve the modeling of complex physical phenomena, ranging from fission gas release to fuel swelling and other temperature-induced effects. For light-water reactors (LWRs), swelling of the fuel and the pressure it imposes on the clad when they come into contact causes permanent clad deformation. Accurately characterizing the fuel-cladding interaction, which involves multiple physics, is essential to accurately simulate the fuel/cladding system. Thermomechanical modeling of this problem using a variationally consistent enforcement (e.g., a mortar approach) has been shown to improve the quality of results and facilitate convergence. Here, we present a general multiphysics computational framework for solving nuclear fuel problems using a mortar approach in BISON, a nuclear fuel performance code. In this study analyses show that using the mortar approach, which enables variationally consistent constraint enforcement, improves the quality of results as compared to the more commonly used node-on-face enforcement for representative LWR nuclear fuel simulations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Progress Toward Simulating Departure from Nucleate Boiling at High-Pressure Applications with Selected Wall Boiling Closures

Recently, a Eulerian-based two-fluid computational fluid dynamics (CFD) framework with a wall heat flux partitioning approach has been intensively investigated for departure from nucleate boiling (DNB) simulation under the U.S. Department of Energy–funded Consortium for Advanced Simulation of Light Water Reactors (CASL) program. Understanding of the DNB characteristics over a range of pressurized water reactor–like operating conditions and accurate prediction of boiling crisis in the nuclear power system have been grand challenges because of the large impact of DNB on reactor safety and operational economics. The ultimate goal of this task in the CASL program is to introduce a robust multiphase CFD–based DNB modeling framework that is capable of characterizing an entire boiling history in which the wall boiling mode experiences the following through multiple stages of heat transfer mode: (1) single-phase convective heat transfer, (2) nucleate boiling heat transfer, and (3) identification of the departure of nucleate boiling. To validate the CASL boiling model, we have benchmarked simulated DNB over three different flow channel configurations (pipe flow, 5 × 5 fuel bundle with mixing vane tests, and 5 × 5 fuel bundle without mixing vane tests) against experimental measurements, and the validation result with open literature is reported. The DNB detection criteria in the simulation are checked by monitoring the peak wall temperature, wall dryout factor, and net energy balance. In addition to the DNB performance test, some preliminary sensitivity results on closure model selection are reported to address the prediction capability of local void profile against measurements. The boiling simulation tested in this study exhibits a maximum deviation of 24% from the measured DNB value in a high-pressure (i.e., 138 bars) subcooled pipe flow test. The ranges of operating conditions are as follows: 1650 to 2650 kg/m 2 ·s for mass flux and 8.5 to 96 K for subcooled inlet temperature. The deviation is even reduced to 7% when the subcooled temperature is less than 40 K. Besides accuracy, base practice guidelines for DNB detection criteria are tested by monitoring three simulation variables: (1) maximum wall temperature, (2) wall dryout factor (i.e., K-value), and (3) energy balance. Numerical robustness of DNB simulation is largely achieved in most of the validation test except for a few high subcooled test cases.

42 ENGINEERING↗

DOE OSTI2023

A Miniaturized Ignition Screening Rapid Compression Machine for probing low-to-intermediate temperature chemistry

With an objective to achieve net-zero emissions by no later than 2050, biofuels hold enormous potential as sustainable, renewable fuels that can be produced on a large scale. However, fuels of a similar type, derived from limited feedstock batch can dramatically vary in terms of their chemical structures and compositions, causing significant differences in physicochemical properties mainly influencing ignition-relevant properties. Rigorous prescreening and testing efforts are involved to evaluate fuels to comply with engines equipped with advanced combustion modes. The testing of some of these fuels implies low quantity fuel samples, access to relevant temperature and pressure conditions, high reproducibility, and a high throughput rate. In light of these considerations, a Miniaturized Ignition Screening Rapid Compression Machine (MISR) has been developed and built at the University of Illinois Chicago (UIC). Some design features include a smaller bellows-actuated driver section compared to other RCM designs, an adjustable brake section, and full optical access. The setup is designed to achieve reaction conditions (T > 600K and P < 100 bar with repetition rates of about 8 seconds per experiment). These conditions are relevant to low-to-intermediate temperature auto-ignition and can generate data for developing relevant chemical kinetics models or ignition maps. A brief insight into MISR design and its operating mechanism is shown. Also, to demonstrate the performance characteristics of the MISR, Ignition Delay (I.D) experiments for ethanol fuel at different equivalence ratios (Φ) are discussed in the context of plans with additional optical diagnostics, high-speed imaging, and gas sampling experiments.

Tomar, Mukul↗

DOE OSTI2021

Development of dispensing hardware for safe fueling of heavy duty vehicles

The development of safe dispensing equipment for the fueling of heavy duty (HD) vehicles is critical to the expansion of this newly and quickly expanding market. This paper discusses the development of a HD dispenser and nozzles assembly (nozzle, hose, breakaway) for these new, larger vehicles where flow rates are more than double compared to light duty (LD) vehicles. This equipment must operate at nominal pressures of 700 bar, -40o C gas temperature, and average flow rate of 5-10 kg/min at a high throughput commercial hydrogen fueling station without leaking hydrogen. The project surveyed HD vehicle manufacturers, station developers, and component suppliers to determine the basic specifications of the dispensing equipment and nozzle assembly. The team also examined existing codes and standards to determine necessary changes to accommodate HD components. From this information, the team developed a set of specifications which will be used to design the dispensing equipment. In order to meet these goals, the team performed computational fluid dynamic, pressure modelling, and temperature analysis in order to determine the necessary parameters to meet existing safety standards modified for HD fueling. The team also considered user, operational, and maintenance requirements, such as freeze lock which has been an issue which prevents the removal of the nozzle from LD vehicles. The team also performed a failure mode and effects analysis (FMEA) to identify the possible failures in the design. The dispenser and nozzle assembly will be tested separately, and then installed on an innovative, HD fueling station which will use a HD vehicle simulator to test the entire system.

08 HYDROGEN↗

DOE OSTI2021

Ultra-high energy density relativistic plasmas from nanostructures: scaling to ultra-high intensities (Final Report)

This project investigated the ultra-high energy density (UHED) regime of matter found in the center of stars, using a compact PW-class laser. These extreme conditions are typically only obtained in the laboratory in the central hot-spot of spherically imploded capsules in inertial confinement fusion experiments driven by the world’s largest lasers. We have shown that near-solid density arrays of aligned nanostructures can be volumetrically heated to multi-keV temperatures by irradiation at relativistic intensity with ultrafast laser pulses of modest energy, opening a path for the generation of UHED plasmas with compact lasers. This new UHED plasma generation approach promises to create an environment with extreme energy densities and degrees of ionization, record conversion of optical laser light into ultrafast x-ray pulses, gigantic magnetic fields and pressures, and directed beams of high energy particles . In this project we achieved record degree of ionization in volumetric heating solid density and near-solid density plasmas. Gold plasmas which spectra is characterized by L shell transition emission from ions with charge up to the Ne-like state, Au+ 72 were generated using ultrafast laser pulses of less than 10 J of energy from a compact laser focused to an intensity of ~ 3x10 21 Wcm -2 . We also conducted measurements to determine the heat penetration depth in Ni nanowire arrays as compared to Ni foil targets by monitoring the line emission of a Co buried tracer underneath a variable amount of Ni. The measurements revealed that the nanowire plasmas are roughly six times larger in depth than the solid density target plasmas. A result of this increased plasma in nanowire arrays is a greatly increased conversion of optical laser light into > 1 KeV x-rays, a record conversion efficiency of 20 %. Critical to the realization of the proposed experiments was the generation of ultrafast laser pulses with ultra-high contrast that can deposit the energy deep into the nanowire arrays before the nanowires explode to create a continuous plasma. Supporting the proposed experiments was the recent demonstration at Colorado State University of a Petawatt-class laser that emits 30 fs pulses at high repetition rates. The experiments combined this unique laser tool with a variety of tailored nanowire arrays fabricated in house and with an extensive suite of diagnostics. The experiments were accompanied by 3-dimensional particle-in-cell simulations and detailed atomic physics simulations with transient kinetics and radiation transport. The proposed research allowed us to continue training Ph.D students and post-docs with broad experience in HEDP Science.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Observational Study Reveals Inverse Relationship: Rising PM2.5 Concentrations Linked to Decreasing Muon Flux

Muon flux, the rate of muons reaching Earth from the atmosphere, is impacted by various factors such as air pressure, temperature, and humidity. However, the influence of concentrations of PM2.5 (particulate matter with diameters 2.5 mm or smaller) on muon detection rates remains unexplored. During the summer of 2023, smoke from Canadian wildfires (containing significant amounts of particulate matter) blew over regions in the Northern US, introducing huge fluctuations in PM2.5 concentrations, thus inspiring this experiment to investigate the correlation of PM2.5 concentrations and muon rates. To investigate the correlation, muon collision rates were measured and analyzed alongside PM2.5 concentration data over the periods of both light and heavy smoke. Other confounding variables, including temperature, humidity, and atmospheric pressure, were also considered. The results reveal a statistically significant inverse correlation between muon flux and PM2.5 concentrations, indicating that particulate matter has an impact on the rate of muons reaching the earth’s surface.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

Observational Study Reveals Inverse Relationship: Rising PM2.5 Concentrations Linked to Decreasing Muon Flux

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗