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DOE OSTI2023

One-dimensional Holstein model revisited

Here, we analyze the global ground-state (quantum) phase diagram of the one-dimensional spinful Holstein model at half filling as a function of the strength of the electron-phonon coupling (represented by the strength of the phonon-induced attraction, U) and the phonon frequency ω 0 . In addition to reanalyzing the various asymptotic regimes, we carry out density-matrix renormalization group simulations to correct previous inferences concerning the antiadiabatic (large ω 0 ) and strong-coupling (large U) regimes. There are two distinct phases—a fully gapped commensurate charge-density-wave phase and a spin-gapped Luther-Emery phase with a gapless charge mode—separated by a phase boundary, with a shape that reflects different microscopic physics in the weak- and strong-coupling limits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS2004

Aluminum-Alloy-Matrix/Alumina-Reinforcement Composites

Isotropic composites of aluminum-alloy matrices reinforced with particulate alumina have been developed as lightweight, high-specific-strength, less-expensive alternatives to nickel-base and ferrous superalloys. These composites feature a specific gravity of about 3.45 grams per cubic centimeter and specific strengths of about 200 MPa/(grams per cubic centimeter). The room-temperature tensile strength is 100 ksi (689 MPa) and stiffness is 30 Msi (206 GPa). At 500 F (260 C), these composites have shown 80 percent retention in strength and 95 percent retention in stiffness. These materials also have excellent fatigue tolerance and tribological properties. They can be fabricated in net (or nearly net) sizes and shapes to make housings, pistons, valves, and ducts in turbomachinery, and to make structural components of such diverse systems as diesel engines, automotive brake systems, and power-generation, mining, and oil-drilling equipment. Separately, incorporation of these metal matrix composites within aluminum gravity castings for localized reinforcement has been demonstrated. A composite part of this type can be fabricated in a pressure infiltration casting process. The process begins with the placement of a mold with alumina particulate preform of net or nearly net size and shape in a crucible in a vacuum furnace. A charge of the alloy is placed in the crucible with the preform. The interior of the furnace is evacuated, then the furnace heaters are turned on to heat the alloy above its liquidus temperature. Next, the interior of the furnace is filled with argon gas at a pressure about 900 psi (approximately equal to 6.2 MPa) to force the molten alloy to infiltrate the preform. Once infiltrated, the entire contents of the crucible can be allowed to cool in place, and the composite part recovered from the mold.

Kashalikar, Uday↗

DOE OSTI2020

An Eulerian multimaterial framework for simulating high-explosive aquarium tests

Aquarium tests of cylindrical high-explosive charges provide optical data of the detonation front velocity and shape, propagation of the shock wave in the surrounding water, and expansion rates of the detonation products behind the front. Data from aquarium experiments is often used for calibration of reactive burn models based on phenomenological equations of state (EOS) and reaction rate laws. This paper presents a multimaterial numerical modeling framework to solve the 2D axisymmetric reactive Euler equations for high-explosive aquarium tests, in particular for ammonium nitrate - fuel oil (ANFO) explosives. An extension of the Ghost Fluid Method (GFM) is used to handle the dynamic material interfaces for the ANFO explosion products, the charge-confining material (polymethyl methacrylate PMMA), and the surrounding water. This study analyzes the sensitivity of calculations (both computational efficiency and numerical accuracy) to different algorithms for the material interface models including the original GFM versus Riemann solver-based strategies. A novel method for defining the left and right states in the interfacial Riemann problem eliminates the need for sorting or nodal interpolation during the projection along the material interface. Numerical tests indicate that populating the interface node values using the Riemann solution mitigate the overheating error observed in steady-state calculations. Solution convergence and computational efficiency are explored as a function of the spatial and temporal order of the schemes. Results from the computational model with analytical equations of state and fitted reaction rate parameters show very good quantitative agreement with experimentally observed detonation front velocity, reaction products expansion, and shock wave propagation in the surrounding water for a cylindrical ANFO charge encased in PMMA. Finally, the proposed modeling framework, in conjunction with experimental tests, provides a reliable tool to assess equations of state and reaction rate expressions for reactive burn models of confined high explosives.

42 ENGINEERING↗

DOE OSTI2024

Explicit simulation of the Brownian rotation of arbitrary shaped aerosol particles using quaternions

The shape of an aerosol particle strongly influences its mass and momentum transfer cross-sections, charging properties, and other physical properties. Here, we present an explicit time-stepping procedure to simulate the rotational Brownian motion of arbitrary shaped aerosol particles by solving Euler’s equation of rotation. A Langevin formulation of the rotation equations is used, wherein Brownian motion due to thermal collisions between a particle and background gas molecules is represented using a stochastic fluctuating torque and fluid resistance is included as a drag torque. To avoid singularities associated with describing the orientation of a shape with Euler angles, we employ a quaternion formulation that leads to first-order stochastic differential equations to describe the evolution of the angular position and angular velocity of a rigid body. We perform all the rotational dynamics calculations in the body-fixed frame of reference attached to the rotating shape whose basis vectors are the normalized eigenvectors of the inertia tensor of the particle. Numerical solutions to rotation under torque-free conditions, damped rotation without Brownian motion, and stochastic rotation for arbitrary shapes are presented and discussed. The presented method enables time-resolved simulation of Brownian rotation for direct comparison with experimentally measured trajectories or statistical measures. The second order accuracy of the used time-stepping procedure places a severe restriction on the timestep that can be used for obtaining accurate results. Animations of presented simulations are included for visualizing rotational motion at various gas pressures. To aid implementation, MATLAB ® codes are also provided. Extension to include translation Brownian motion is straightforward.

Roy, Mrittika↗

DOE OSTI2020

Effects of surface charge and cluster size on the electrochemical dissolution of platinum nanoparticles using COMB3 and continuum electrolyte models

We study the site-dependent dissolution of platinum nanoparticles under electrochemical conditions to assess their thermodynamic stability as a function of shape and size using empirical molecular dynamics and electronic-structure models. The third-generation charge optimized many-body potential is employed to determine the validity of uniform spherical representations of the nanoparticles in predicting dissolution potentials (the Kelvin model). To understand the early stages of catalyst dissolution, implicit solvation techniques based on the self-consistent continuum solvation method are applied. It is demonstrated that interfacial charge and polarization can shift the dissolution energies by amounts on the order of 0.74 eV depending on the surface site and nanoparticle shape, leading to the unexpected preferential removal of platinum cations from highly coordinated sites in some cases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Projecting Electric Vehicle Electricity Demands and Charging Loads

After over a century of petroleum dominance, electric vehicles are rapidly disrupting the transportation energy landscape. At the same time, the electric power systems are undergoing profound changes as variable renewables replace dispatchable fossil generators. It is critically important to understand how transportation electrification will impact electricity demand, including changes in the load shapes that characterize the system, and the value of flexible electric vehicle charging to better balance electricity demand and supply. This talk focuses on methods to project electricity demand for EV charging with high spatiotemporal fidelity to enable electricity system modeling and analysis and summarizes results from recent NREL studies in this area.

ADVANCED PROPULSION SYSTEMS,ENERGY PLANNING, POLIC↗

DOE OSTI2021

Electric field reversals resulting from voltage waveform tailoring in Ar/O 2 capacitively coupled plasmas sustained in asymmetric systems

The etching of nanometer scale high-aspect-ratio (HAR) features into dielectric materials in low pressure radio frequency excited plasmas is often accompanied by charge accumulation inside the features which can slow etching rates and produce distortions such as twisting. The intra feature charging is at least partially produced by differences in electron and ion energy and angular distributions (EADs). Positive ions, accelerated to high energies having narrow angular spreads by the sheath electric field, can penetrate deeply into HAR features. Electrons typically arrive at the wafer with nearly thermal and isotropic distributions and do not penetrate deeply into HAR features. These disparities lead to differential charging of the inside of the feature, which can lead to reductions in etch rate and feature distortion due to ion deflection. With in-creasing aspect ratio of features, charging challenges are expected to continue for the foreseeable future. In this work, the use of tailored voltage waveforms in geometrically asymmetric capacitively coupled plasmas sustained in Ar/O 2 at 40 mTorr was computationally investigated with the goal of shaping the EAD of electrons incident onto the substrate to address differential charging. The tailored waveform consisted of a sinusoidal wave and its higher harmonics with a fundamental frequency of 1 MHz. Further, we found that electric field reversals in the sheath and presheath can occur during the anodic portion of the cycle. The electric field reversal increases the energy and decreases the angular spread of electrons incident onto the substrate. The magnitude of the electric field reversal can be controlled by the phase angle of the even harmonics and the gas composition. Due to its electronegative nature, increasing mole fractions of O 2 impedes electron transport to the surface which further increases the electric field reversal.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Integrated Transportation-Energy Systems Modeling

Transportation is currently the least-diversified energy demand sector, with over 90% of global transportation energy use coming from petroleum product. After over a century of petroleum dominance, however, many leading experts anticipate major electrification trends that could disrupt the transportation energy demand landscape. These changes in electricity demand complement profound changes happening within electric power supply systems, including integration of variable renewables, distributed generation and storage, and greater participation in power system planning and operations from traditionally passive consumers. This broader context underscores the importance of understanding how transportation electrification will impact electricity demand, including changes in the load shapes that characterize the system and the opportunity to leverage flexible EV charging to more cost-effectively balance demand and supply. This talk provides an overview of recent findings on infrastructure requirements to support EV adoption, integration challenges and the impact of EV on power systems, and opportunities to leverage flexible (or smart) EV charging to support power system planning and operations.

ADVANCED PROPULSION SYSTEMS,ENERGY PLANNING, POLIC↗

DOE OSTI2025

REIMAGINING HEAT EXCHANGERS FOR NEXT GENERATION ENVIRONMENTAL SYSTEMS

Air-to-refrigerant heat exchangers (HXs) are essential components in space conditioning, refrigeration, and power systems, and recent efforts have focused on making these devices more compact, reducing refrigerant charge and lowering manufacturing costs. Historically, HX innovation has been limited by available computational resources, design tools, and manufacturing constraints. The best available technologies utilize tube-fin and micro- or macro-channel tubes with fins, which are not necessarily the optimal designs achievable with current technology. In this paper, we highlight the latest advancements in air-to-refrigerant HXs, specifically emphasizing innovations achieved through shape and topology optimization. A multi-scale design optimization approach is introduced, alongside similar methods in literature, which enable highly sophisticated shape-optimized tube designs with more than 50% reduction in size and 25% reduction in refrigerant charge, essential for A3 refrigerant charge limit compliance. The frameworks integrate traditional heat and mass transfer science with state-of-the-art machine learning, genetic algorithms, and adjoint algorithms to create novel designs. While many of these innovative designs may not be manufacturable using conventional methods, they allow us explore the boundaries of what is possible. These novel air-to-refrigerant HXs are key enablers for ultra-low-refrigerant charge heat pump and refrigeration systems.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2020

Role of Electric Vehicles in the U.S. Power Sector Transition: A System-Level Perspective

After over a century of petroleum dominance many anticipate that electrification could disrupt the transportation energy landscape. At the same time, the electric power systems are undergoing profound changes: variable renewables are displacing conventional generation sources; distributed generation is disrupting utility business models; energy storage and other new technologies are emerging; and the traditional system based on the premise that generation is dispatched to match an inelastic demand is evolving to create a system with greater participation in power system planning and operations from traditionally passive consumers. In this context, it is important to understand how transportation electrification will impact electricity demand and in turn electricity supply, including changes in the load shapes that characterize the system and the opportunity to leverage flexible electric vehicle (EV) charging to better integrate demand and supply. Assessing the impacts of electrification on the energy system requires an understanding of how it might impact the amount and shape of electricity consumption, and how this electricity can be supplied. In particular, increased adoption of electric vehicles introduces a new source of demand altogether, potentially very flexible. Moreover, electrification could shift the consumption of natural gas between sectors, thereby affecting the economics for natural gas-fired generation relative to other electricity generation options. Several factors will impact the evolution of the power system under a widespread electrified future, which, in turn, could have far-reaching effects on future energy costs and emissions.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Arrested-motility states in populations of shape-anisotropic active Janus particles

The emergence of large-scale collective phenomena from simple interactions between individual units is a hallmark of active matter systems. Active colloids with alignment-dominated interparticle interactions tend to develop orientational order and form motile coherent states, such as flocks and swarms. Alternatively, a combination of self-propulsion and excluded-volume interactions results in self-trapping and active phase separation into dense clusters. Here, we reveal unconventional arrested-motility states in ensembles of active discoidal particles powered by induced-charge electrophoresis. Combining experiments and computational modeling, we demonstrate that the shape asymmetry of the particles promotes the hydrodynamically assisted formation of active particles’ bound states in a certain range of excitation parameters, ultimately leading to a spontaneous collective state with arrested motility. Unlike the jammed clusters obtained through self-trapping, the arrested-motility phase remains sparse, dynamic, and reconfigurable. The demonstrated mechanism of phase separation seeded by bound state formation in ensembles of oblate active particles is generic and should be applicable to other active colloidal systems.

42 ENGINEERING↗

DOE OSTI2021

Comparison of Single-Event Transients in an Epitaxial Silicon Diode Resulting from Heavy Ion-, Focused X-Ray-, and Pulsed Laser-Induced Charge Generation

Heavy ion, focused x-ray, and pulsed laser single event transient experiments are performed on a silicon epitaxial diode. Collected charge, transient rise times, and transient fall times are calculated and compared between the different sources. It is observed that these transient shape characteristics depend on the source (ion, x-ray, or laser), even when similar amounts of charge are generated. Finally, the observed differences are examined and explained in terms of basic charge collection mechanisms.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Mutations of Omicron Variant at the Interface of the Receptor Domain Motif and Human Angiotensin-Converting Enzyme-2

The most recent Omicron variant of SARS-CoV-2 has caused global concern and anxiety. The only thing certain about this strain, with a large number of mutations in the spike protein, is that it spreads quickly, seems to evade immune defense, and mitigates the benefits of existing vaccines. Based on the ultra-large-scale ab initio computational modeling of the receptor binding motif (RBM) and the human angiotensin-converting enzyme-2 (ACE2) interface, we provide the details of the effect of Omicron mutations at the fundamental atomic scale level. In-depth analysis anchored in the novel concept of amino acid-amino acid bond pair units (AABPU) indicates that mutations in the Omicron variant are connected with (i) significant changes in the shape and structure of AABPU components, together with (ii) significant increase in the positive partial charge, which facilitates the interaction with ACE2. We have identified changes in bonding due to mutations in the RBM. The calculated bond order, based on AABPU, reveals that the Omicron mutations increase the binding strength of RBM to ACE2. Our findings correlate with and are instrumental to explain the current observations and can contribute to the prediction of next potential new variant of concern.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1985

The electrostatics of a dusty plasma

Voyager 1 and 2 observations of the Saturnian ring system have led to the discovery of several interesting phenomena associated with its fine dust component. The dust grains are immersed in a plasma. The present paper is concerned with the electrostatics of a dusty plasma, giving particular attention to the capacitance and charge of an individual grain in the presence of neighboring grains and the surrounding plasma. The Poisson equation and gauge considerations are discussed along with a solution of the Poisson equation for several models, taking into account impermeable grains, permeable grains, and a spherical capacitor model. A comparison of potential shapes for three models is conducted, and the effect of neighbors on charging currents is explored.

Whipple, E. C.↗

NASA NTRS2016

Meeting the Grand Challenge of Protecting Astronauts Health: Electrostatic Active Space Radiation Shielding for Deep Space Missions

This report describes the research completed during 2011 for the NASA Innovative Advanced Concepts (NIAC) project. The research is motivated by the desire to safely send humans in deep space missions and to keep radiation exposures within permitted limits. To this end current material shielding, developed for low earth orbit missions, is not a viable option due to payload and cost penalties. The active radiation shielding is the path forward for such missions. To achieve active space radiation shielding innovative large lightweight gossamer space structures are used. The goal is to deflect enough positive ions without attracting negatively charged plasma and to investigate if a charged Gossamer structure can perform charge deflections without significant structural instabilities occurring. In this study different innovative configurations are explored to design an optimum active shielding. In addition, to establish technological feasibility experiments are performed with up to 10kV of membrane charging, and an electron flux source with up to 5keV of energy and 5mA of current. While these charge flux energy levels are much less than those encountered in space, the fundamental coupled interaction of charged Gossamer structures with the ambient charge flux can be experimentally investigated. Of interest are, will the EIMS remain inflated during the charge deflections, and are there visible charge flux interactions. Aluminum coated Mylar membrane prototype structures are created to test their inflation capability using electrostatic charging. To simulate the charge flux, a 5keV electron emitter is utilized. The remaining charge flux at the end of the test chamber is measured with a Faraday cup mounted on a movable boom. A range of experiments with this electron emitter and detector were performed within a 30x60cm vacuum chamber with vacuum environment capability of 10-7 Torr. Experiments are performed with the charge flux aimed at the electrostatically inflated membrane structure (EIMS) in both charged and uncharged configurations. The amount of charge shielding behind and around the EIMS was studied for different combinations of membrane structure voltages and electron energies. Both passive and active shielding were observed, with active shielding capable of deflecting nearly all incoming electrons. The pattern of charge distribution around the structure was studied as well as the stability of the structures in the charge flow. The charge deflection experiments illustrate that the EIMS remain inflated during charge deflection, but will experience small amplitude oscillations. Investigations were performed to determine a potential cause of the vibrations. It is postulated these vibrations are due to the charge flux causing local membrane charge distribution changes. As the membrane structure inflation pressure is changed, the shape responds, and causes the observed sustained vibration. Having identified this phenomenon is important when considering electrostatically inflated membrane structures (EIMS) in a space environment. Additionally, this project included a study of membrane material impacts, specifically the impact of membrane thickness. Extremely thin materials presented new challenges with vacuum preparation techniques and rapid charging. The thinner and lighter membrane materials were successfully inflated using electrostatic forces in a vacuum chamber. However, care must be taken when varying the potentials of such lighter structures as the currents can cause local heating and melting of the very thin membranes. Lastly, a preliminary analysis is performed to study rough order of magnitude power requirements for using EIMS for radiation shielding. The EIMS power requirement becomes increasingly more challenging as the spacecraft voltage is increased. As a result, the emphasis is on the deflection of charges away from the spacecraft rather than totally stopping them. This significantly alleviates the initial power requirements. With modest technological development(s) active shielding is emerging to be a viable option.

Radiation↗

NASA NTRS2023

Metrics for Anomalous Charging currents in Polymer Tantalum Capacitors

Anomalous charging currents (ACC) in polymer tantalum capacitors may appear as a temporary short circuit that can last for dozens of milliseconds, cause failures to the parts, or cause malfunctions to fast operating electronic systems. Currently, there is no standard technique or set of metrics to evaluate the level of ACC which compares results obtained by different users and manufacturers. In this work, ACC in different types of capacitors were characterized by analysis of current transients during the constant voltage ramp or power surge testing (PST) techniques. It is shown that although the shape of transients may vary at different test conditions, the transfer charge and energy remain practically the same. The level of ACC is characterized by the energy dissipated in the part during PST. Variations of the dissipated energy with moisture content, test temperature, and voltage are evaluated. Effects of different reflow soldering conditions and long-term (up to 3000 hours) storage at 125 °C are discussed.

polymer tantalum capacitor↗

DOE OSTI2023

Photon-to-Digital Converters for Neutron Imaging Instruments (Final Report)

Oak Ridge National Laboratory (ORNL) collaborated with the Université de Sherbrooke (UdeS) to design a modular and scalable tile of innovative digital photodetectors called Photon-to-Digital Converters (PDC) and the required subsystems to demonstrate the feasibility of large area single-photon detectors to support high-resolution, depth-of-interaction, fast neutron radiography based on scintillation detectors. The goal is to demonstrate the advantages of using PDC over conventional Silicon Photomultiplier (SiPM) for neutron imaging systems. The basic building blocks of analog SiPM and PDC are Single-Photon Avalanche Photodiodes (SPAD). The main difference between conventional SiPMs and PDCs, is in the fact that analog SiPMs sum the charge produced by individual SPAD passively, while in PDCs each SPAD is read out individually by an active electronic circuit. Hence, PDCs provide a direct photon-to-bit conversion where a logic “1” means that there was a detection in a given SPAD. Conversely, an analog SiPM requires a sophisticated preamplifier (current amplifiers or transimpedance amplifier) followed by a shaping amplifier and an analog-to-digital converter. Moreover, since the charge from each SPAD varies slightly, the passive sum of the analog SiPM will have signal fluctuations for the same amount of photon detected. This is one of many issues that is completely eliminated by individual one-to-one SPAD read out in PDCs. The large area required for scintillator readouts for neutron imaging is such that the output capacitance of a large area of SiPM arrays is very high. This creates a burden on the signal-to-noise optimization with respect to the power budget. For PDC, the power consumption is dictated by rate of the incident photon flux, or in photon-starved environments, the dark noise rate of the SPAD array. In other words, the power consumption in the absence of events is extremely low. Hence, the power consumption of a PDC read out system is much lower than its analog counterpart. Further, the large SiPM capacitance may introduce signal distortions on the scintillator fast rise or decay time with undesired effects on timing and pulse shape discrimination. The problem is absent in PDCs, as their readout is independent on device capacitance. UdeS is the world leader in 3D vertical integration of frontside illuminated SPAD arrays over CMOS readouts. These capabilities allow future production of “3D PDC” with maximum photosensitive fill factor and electronic functionalities tailored to the application. UdeS' vast knowledge of SPADs and CMOS design made the team an ideal collaborator in the development of large area high-resolution fast neutron radiography.

42 ENGINEERING↗

DOE OSTI2020

Theoretical insights into the surface physics and chemistry of redox-active oxides

Redox active oxides are ubiquitous in materials applications, including catalysis, photovoltaics, self-cleaning glasses, chemical sensors, and electronic components. Their utility derives from their unique ability to access multiple metal charge states within a finite energy window. However, this property also confounds our ability to study reducible oxides, because it leads to structural, compositional, and electronic complexities that elude simplistic models of materials structure and function. Oxygen vacancies play a critical role in shaping the functional properties of such oxides; most notably, they lead to mobile charge imbalances that impact surface processes at significant distances from the originating defect. Atomistic simulations are inherently equipped to illuminate these phenomena at a fundamental level; however, reducible oxides pose great challenges due to the high level of electron correlation needed to correctly describe them. Knowing how defects form, couple, propagate, agglomerate, or repel each other and influence the surface properties of reducible oxides is only now coming into the grasp of modern theory and simulation capabilities. This knowledge is also key to discovering and controlling emergent materials processes at nanometer scale and beyond. The manuscript was written with support of all three authors from U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. Work by RR and VG was performed at Pacific Northwest National Laboratory (PNNL), which is a multi-program laboratory operated by Battelle for DOE under Contract DE AC05 76RL01830. AS was supported under Award DE-SC0007347.

Rousseau, Roger J.↗