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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Prediction of the Thermal Runaway Limit and Optimal Operation of Heat Transfer-Limited, Fixed-Bed Reactor Systems

Here, we derive a new prediction for thermal runaway starting from the alpha model for fixed-bed reactor systems. This method accounts for thermal resistance internal to the reactor tube and the radial temperature gradients that result. To showcase our method, we compare its predictions to other common criteria for thermal runaway using o-xylene oxidation as the example chemistry. Even in systems where internal heat transfer is negligible, the empirical practical design criterion for thermal runaway is inaccurate. For cases where internal heat transfer is relevant, our runaway limit is more stringent than limits derived from simpler 1-D models. To augment our work, we optimize the product yield with the thermal runaway constraint using orthogonal collocation. Using the alpha model, the results illustrate that the thermal runaway limit can be accurately determined using either numerical or analytical methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Pressure Barrier Applicability to Polymer Flood Design

Effective oil displacement from a reservoir requires adequate and properly directed pressure gradients in areas of high oil saturation. If the polymer bank is too large or too viscous during a polymer flood, the pressure drop from the injection well to the polymer front may act as a pressure barrier by usurping most of the downstream driving force for oil displacement. Polymer injection pressures must be limited. The maximum allowable injection pressure is commonly constrained by caprock integrity, injection equipment, and/or regulations, even though fractures can be beneficial to polymer injectivity (and even sweep efficiency in some cases). This paper examines when the pressure-barrier concept limits the size and viscosity of the polymer bank during a polymer flood. Both analytical and numerical methods are used to address this issue. We examine the relevance of the pressure barrier concept for a wide variety of circumstances, including oil viscosities ranging from 10-cp (like at Daqing, China) to 1650-cp (like at Pelican Lake, Alberta), vertical wells (like at Tambaredjo, Suriname) versus horizontal wells (like at Milne Point, Alaska), single versus multiple layered reservoirs, permeability contrast, and with versus with crossflow between layers. We also examine the relation between the pressure-barrier concept and fractures and fracture extension during polymer injection. We demonstrate that in reservoirs with single layers, the pressure-barrier concept only limits the optimum viscosity of the injected polymer if the mobility of the polymer bank is less than the mobility of the displaced oil bank. The same is true for multi-zoned reservoirs with no crossflow between layers. Thus, for these cases, the optimum polymer viscosity is likely to be dictated by the mobility of the oil bank, unless other factors (like fracture extension) intervene. For multi-zoned reservoirs with free crossflow between layers, the situation is different. A compromise must be reached between injected polymer viscosity and the efficiency of oil recovery. The relevance of our findings is applied to operations for several existing polymer floods. This work is particularly relevant to viscous-oil reservoirs (like Pelican Lake and others) where the injected polymer viscosities are substantially lower than the oil viscosity

Wang, Dongmei↗
DOE OSTI2025

Hybrid HEFA-HDCJ Process for the Production of Jet Fuel Blendstocks

The hydrotreatment of bio-oil derived from the pyrolysis and biocrude from hydrothermal liquefaction of lignocellulosic materials to produce hydrocarbons faces significant technological challenges, mainly due to the high reactivity and poor thermal stability of bio-oil, resulting in the formation of large quantities of coke. This problem has been addressed by existing PNNL patents with a two-step hydrotreatment technology in which the bio-oil is first stabilized with a noble hydrogenation metal (often Pt or Ru). Then, in the second step, the bio-oil is deoxygenated with a Ni-Mo or Co-Mo sulfide catalyst. The main problem with this approach is that the Pt/Ru catalysts deactivate easily in the presence of S or other impurities, which are commonly present in pyrolysis oils. In this project, we explored technological solutions to mitigate coke formation, avoiding the use of Pt/Ru catalysts. Our strategy is based on three actions: (1) Bio-oil stabilization in the presence of alcohols. In this project, we studied the stabilization with butanol. (2) the use of a cosolvent to solubilize the bio-oil. Because coke formation reactions are second-order reactions a reduction in the concentration of reactive bio-oil molecules. In this case, we used yellow greases as a co-solvent. (3) Separation of bio-oil reactive fractions. In this project, we studied the removal of water-soluble fractions. Our batch co-hydrotreatment studies confirmed that the addition of butanol and methanol and the blend with lipids effectively contributed to mitigating coke formation (reducing coke yield to about 1 wt.% %). The removal of sugars did not have a noticeable effect on the overall coke yield, suggesting that coke precursors are present in all bio-oil fractions. Our analytical work suggests that they may be concentrated in the water-insoluble/CH 2 Cl 2 insoluble fractions of pyrolysis oils. Although the technological strategies tested resulted in significant coke reductions, the levels achieved were not sufficiently low to ensure a reliable operation in continuous, fixed-bed trickle-bed reactors. Long runs of more than 100 hours (maximum: 255 h) of co-processing time on stream were achieved in a continuous 40 mL reactor. When the same test was conducted in a larger 400 mL reactor, pressure drop increases associated with coke formation were observed. This increase in coke formation could be due to larger temperature gradients in the bed. Hydrodeoxygenation tests in moving bed reactors and using more active hydrogenation catalysts (for example Ni) could lead to more reliable operations. Unfortunately, our team did not have access to such experimental setups. The technoeconomic analysis suggests that although alcohol use is an effective means to reduce coke formation, the use of alcohol increases production cost. Thus, its use needs to be minimized. A delicate balance needs to be found between the use of technological solutions that allow the reliable operation of the system (stabilization with Ni catalysts, use of small quantities of solvents, processing in moving bed reactors) with a tolerable level of coke formation for the hydrodeoxygenation reactor used and that result in minimum production costs.

09 BIOMASS FUELS↗
DOE OSTI2025

EVALUATION OF OPERATION TEMPERATURES UNDER NATURAL CONVECTION HELIUM FLOW IN A CONFINED CAVITY

The Spallation Neutron Source (SNS) is a high-power accelerator-based pulsed neutron source led by Oak Ridge National Laboratory (ORNL) to achieve high fluxes of neutrons for scientific experiments. Active and passive cooling of the systems and parts forming the SNS have been considered to warrant the safe operation of the facility. The diverse cooling systems make use of conjugated heat transfer mechanisms to provide a stable operation temperature for all components in the machine. Thermal power deposited into stainless-steel piping lines due to particle radiation may reach values of up to 1.2 W/cc in the regions located closer to the center of the lower IRP. These energy deposition levels, in not actively cooled components, such as the transfer-line-outer-vacuum-layer may increase the temperature of the component beyond design requirement limitations. The evaluation of the operation temperatures for the former components relies in the assumption that a low-pressure helium atmosphere provides enough heat removal capacity based on natural convection phenomena. In this work, the evaluation of steady state temperatures in components such as the CMS transfer lines has been evaluated using computational fluid dynamics (CFD), analytical correlations and experimental measurements. The companion experiments were conducted in a closed helium system at pressures varying from 1.1 to 1.5 bar. A copper rod was affixed horizontally between viewing windows and heated at constant power, and measurements were made of both the rod temperature and ambient temperature via a system fiberoptic distributed temperature sensors and RTDs. It was found that the measured heat transfer coefficients agree well with the predictions of Churchill and Chu correlations across the range of cases considered. Additionally, the ambient helium volume above the rod was imaged via background oriented schlieren (BOS), and these data was used to determine the line-averaged density gradients in this region. These gradients were compared to simulation data to validate the predictions of natural convection simulations.

Dominguez-Ontiveros, Elvis [ORNL] (ORCID:000000018↗
DOE OSTI2021

PDG: A Composite Method Based on the Resolution of the Identity

The Gaussian-3 (G3) composite approach for thermochemical properties is revisited in light of the enhanced computational efficiency and reduced memory costs by applying the resolution-of-the-identity (RI) approximation for two-electron repulsion integrals (ERIs) to the computationally demanding component methods in the G3 model: the energy and gradient computations via the second-order Møller–Plesset perturbation theory (MP2) and the energy computations using the coupled-cluster singles–doubles method augmented with noniterative triples corrections [CCSD(T)]. Efficient implementation of the RI-based methods is achieved by employing a hybrid distributed/shared memory model based on MPI and OpenMP. The new variant of the G3 composite approach based on the RI approximation is termed the RI-G3 scheme, or alternatively the PDG method. The accuracy of the new RI-G3/PDG scheme is compared to the “standard” G3 composite approach that employs the memory-expensive four-center ERIs in the MP2 and CCSD(T) calculations. Taking the computation of the heats of formation of the closed-shell molecules in the G3/99 test set as a test case, it is demonstrated that the RI approximation introduces negligible changes to the mean absolute errors relative to the standard G3 model (less than 0.1 kcal/mol), while the standard deviations remain unaltered. Furthermore, the efficiency and memory requirements for the RI-MP2 and RI-CCSD(T) methods are compared to the standard MP2 and CCSD(T) approaches, respectively. The hybrid MPI/OpenMP-based RI-MP2 energy plus gradient computation is found to attain a 7.5× speedup over the standard MP2 calculations. For the most demanding CCSD(T) calculations, the application of the RI approximation is found to nearly halve the memory demand, confer about a 4–5× speedup for the CCSD iterations, and reduce the computational time for the compute-intensive triples correction step by several hours.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Thermal Gradient Effects on Local Hotspot Ignition in 1,3,5,7‐Tetranitro‐1,3,5,7‐tetrazocane (HMX)

Understanding hotspot ignition, growth, and criticality, as well as the timescales of each, is crucial for parameterizing mesoscale and continuum‐level models that rely on a statistical understanding of hotspots. However, these models often consider hotspots to have uniform temperatures or for hotspots of a given temperature and size to always behave the same. Therefore, using molecular dynamics simulations, we assess the influence of thermal distribution effects on hotspot local ignition and time to ignition in 1,3,5,7‐tetranitro‐1,3,5,7‐tetrazocane (HMX) nanoscale hotspots. Finally, by assessing hotspots with a gradient driven from an initial two‐temperature core–shell setup, we show that small increases in the core temperature under a constant average temperature can lead to order‐of‐magnitude effects on reaction and local ignition timescales.

36 MATERIALS SCIENCE↗
DOE OSTI2020

A molecular dynamics simulation study of thermal conductivity anisotropy in β-octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (β-HMX)

Molecular dynamics (MD) simulations were used to predict the thermal conductivity of β-octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (β-HMX) along directions normal to the (011), (110), and (010) crystal planes. These directions were selected based on the measured morphological importance of the corresponding crystal surfaces. A reverse non-equilibrium MD approach was used wherein a constant heat flux is imposed along a prescribed direction and the resulting steady-state temperature gradient determined. The coefficient of thermal conductivity λ is the quotient of heat flux and temperature gradient (i.e. Fourier's law). Finite-size effects and sensitivity to imposed heat flux were investigated. The results reveal a modest dependence of the conductivity on crystal orientation, significant finite-size effects, and low sensitivity to imposed flux so long as the Fourier's law analysis is limited to the spatial interval in the simulation cell for which the temperature gradient is constant. Infinite-length thermal conductivities were estimated by linear regression of λ -1 (L) versus reciprocal cell length L -1 for each direction. The predicted values are systematically larger, but within a factor of two, than most published experimental determinations, the latter of which were obtained for pressed-powder or composite samples rather than oriented single crystals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Persistent compositions of non-stoichiometric compounds with low bulk diffusivity: A theory and application to Nb3Sn superconductors

Non-stoichiometric compounds may develop a composition gradient when they are formed by reactive diffusional processes. This paper reports an interesting phenomenon that in compounds with low bulk diffusivities, which rely mainly on grain boundary diffusion for their growth, the final bulk compositions may be far from equilibrium, with a very low bulk diffusivity leading to fixed (persistent) compositions – one such example is Nb 3 Sn, a superconductor. We investigated the microchemistry at the reactive interface using atom probe tomography to clarify the diffusion reaction mechanism for this low-bulk-diffusivity case and thus propose a theory for what determines the compound composition, using Nb 3 Sn as an example for concreteness. Using certain approximations, we derive an explicit analytical equation that illustrates what factors determine its composition profile. We compare our model with the known facts of Nb 3 Sn and see good agreement. In particular, this model predicts that internal oxidation may lead to higher Sn contents than conventional, non-oxidized Nb 3 Sn. Our measurements show that this is indeed true, and that the internally-oxidized Nb 3 Sn also has higher upper critical fields, achieving up to 28.2 T at 4.2 K. We discuss the general applicability of this model to non-stoichiometric compounds with low bulk diffusivity, and propose it as a tool to help in the design and processing of such materials for compositional control.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Atomically Local Electric Field Induced Interface Water Reorientation for Alkaline Hydrogen Evolution Reaction

The slow water dissociation process in alkaline electrolyte severely limits the kinetics of HER. The orientation of H 2 O is well known to affect the dissociation process, but H 2 O orientation is hard to control because of its random distribution. Herein, an atomically asymmetric local electric field was designed by IrRu dizygotic single-atom sites (IrRu DSACs) to tune the H 2 O adsorption configuration and orientation, thus optimizing its dissociation process. The electric field intensity of IrRu DSACs is over 4.00×10 10 N/C. The ab initio molecular dynamics simulations combined with in situ Raman spectroscopy analysis on the adsorption behavior of H 2 O show that the M–H bond length (M=active site) is shortened at the interface due to the strong local electric field gradient and the optimized water orientation promotes the dissociation process of interfacial water. This work provides a new way to explore the role of single atomic sites in alkaline hydrogen evolution reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Heterogeneity and Hysteresis in the Polymer Collapse of Single Core–Shell Stimuli-Responsive Plasmonic Nanohybrids

Broad application of polymeric stimuli-responsive smart nanohybrids requires understanding the mechanisms governing active control. Ensemble techniques have identified inhomogeneous polymer collapse in microgels that potentially arise from heterogeneous interchain interactions and differences in core size. A single-particle examination would establish the influence of core size and internal polymer network heterogeneity on local interactions that contribute to the observed inhomogeneous polymer collapse dynamics of nanohybrids. Using single-particle dark-field spectroscopy, we investigated the complex polymer collapse profiles of core–shell plasmonic nanohybrids comprising thermoresponsive poly(N-isopropylacrylamide) (pNIPAM)-encapsulated gold nanorods (AuNRs). We report that the polymer collapse behavior was independent of the core size. For thinner polymer shells, we observed hysteresis in the collapse of AuNR@pNIPAMs, likely related to local pNIPAM aggregation due to interchain hydrogen bonding. For thicker polymer shells, we observed a broad polymer collapse distribution that we attributed to a two-step phase transition that arises from a polymer network density gradient. Furthermore, our single-particle approach relates the internal heterogeneity of the polymer network of nanohybrids to the mechanisms underlying heterogeneous phase transitions that traditional, ensemble-averaged approaches are unable to discern.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Solid-state polymer-particle hybrid electrolytes: Structure and electrochemical properties

Solid-state electrolytes (SSEs) are challenged by complex interfacial chemistry and poor ion transport through the interfaces they form with battery electrodes. Here, we investigate a class of SSE composed of micrometer-sized lithium oxide (Li 2 O) particles dispersed in a polymerizable 1,3-dioxolane (DOL) liquid. Ring-opening polymerization (ROP) of the DOL by Lewis acid salts inside a battery cell produces polymer-inorganic hybrid electrolytes with gradient properties on both the particle and battery cell length scales. These electrolytes sustain stable charge-discharge behavior in Li||NCM811 and anode-free Cu||NCM811 electrochemical cells. On the particle length scale, Li 2 O retards ROP, facilitating efficient ion transport in a fluid-like region near the particle surface. On battery cell length scales, gravity-assisted settling creates physical and electrochemical gradients in the hybrid electrolytes. By means of electrochemical and spectroscopic analyses, we find that Li 2 O particles participate in a reversible redox reaction that increases the effective CE in anode-free cells to values approaching 100%, enhancing battery cycle life.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Positron Beam Loading and Acceleration in the Blowout Regime of a Plasma Wakefield Accelerator

Plasma wakefield acceleration in the nonlinear blowout regime has achieved marked milestones in electron beam acceleration, demonstrating high acceleration gradients and energy efficiency while preserving excellent beam quality. However, this regime is deemed unsuitable for achieving positron acceleration of comparable results, which is vital for future compact electron–positron colliders. In this article, we find that an intense positron beam loaded at the back of beam-driven blowout cavity can self-consistently induce the focusing field and flatten the longitudinal wakefield, leading to stable, high-efficiency, and high-quality positron acceleration. This is achieved through the formation of an on-axis electron filament induced by positron beam load, which shapes the plasma wakefield in a distinct way compared to electron beam load in the blowout regime. Via a nonlinear analytic model and numerical simulations, we explain the novel beam loading effects of the interaction between the on-axis filament and the blowout cavity. High-fidelity simulations show that a high-charge positron beam can be accelerated with >20% energy transfer efficiency, ~1% energy spread, and ~1 mm·mrad normalized emittance, while considerably depleting the energy of the drive beam. The concept can also be extended to simultaneous acceleration of electron and positron beams and high transformer ratio positron acceleration as well. This development offers a new route for the application of plasma wakefield acceleration into particle physics.

Science & Technology - Other Topics↗
DOE OSTI2021

Modeling Liquid Water by Climbing up Jacob’s Ladder in Density Functional Theory Facilitated by Using Deep Neural Network Potentials

Within the framework of Kohn–Sham density functional theory (DFT), the ability to provide good predictions of water properties by employing a strongly constrained and appropriately normed (SCAN) functional has been extensively demonstrated in recent years. Here, we further advance the modeling of water by building a more accurate model on the fourth rung of Jacob’s ladder with the hybrid functional, SCAN0. In particular, we carry out both classical and Feynman path-integral molecular dynamics calculations of water with the SCAN0 functional and the isobaric–isothermal ensemble. To generate the equilibrated structure of water, a deep neural network potential is trained from the atomic potential energy surface based on ab initio data obtained from SCAN0 DFT calculations. For the electronic properties of water, a separate deep neural network potential is trained by using the Deep Wannier method based on the maximally localized Wannier functions of the equilibrated trajectory at the SCAN0 level. The structural, dynamic, and electric properties of water were analyzed. The hydrogen-bond structures, density, infrared spectra, diffusion coefficients, and dielectric constants of water, in the electronic ground state, are computed by using a large simulation box and long simulation time. For the properties involving electronic excitations, we apply the GW approximation within many-body perturbation theory to calculate the quasiparticle density of states and bandgap of water. Compared to the SCAN functional, mixing exact exchange mitigates the self-interaction error in the meta-generalized-gradient approximation and further softens liquid water toward the experimental direction. For most of the water properties, the SCAN0 functional shows a systematic improvement over the SCAN functional. However, some important discrepancies remain. The H-bond network predicted by the SCAN0 functional is still slightly overstructured compared to the experimental results.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Robust scalable initialization for Bayesian variational inference with multi-modal Laplace approximations

Predictive modeling typically relies on Bayesian model calibration to provide uncertainty quantification. Variational inference utilizing fully independent (“mean-field”) Gaussian distributions are often used as approximate probability density functions. This simplification is attractive since the number of variational parameters grows only linearly with the number of unknown model parameters. However, the resulting diagonal covariance structure and unimodal behavior can be too restrictive to provide useful approximations of intractable Bayesian posteriors that exhibit highly non-Gaussian behavior, including multimodality. High-fidelity surrogate posteriors for these problems can be obtained by considering the family of Gaussian mixtures. Gaussian mixtures are capable of capturing multiple modes and approximating any distribution to an arbitrary degree of accuracy, while maintaining some analytical tractability. Unfortunately, variational inference using Gaussian mixtures with full-covariance structures suffers from a quadratic growth in variational parameters with the number of model parameters. The existence of multiple local minima due to strong nonconvex trends in the loss functions often associated with variational inference present additional complications, These challenges motivate the need for robust initialization procedures to improve the performance and computational scalability of variational inference with mixture models. In this work, we propose a method for constructing an initial Gaussian mixture model approximation that can be used to warm-start the iterative solvers for variational inference. The procedure begins with a global optimization stage in model parameter space. In this step, local gradient-based optimization, globalized through multistart, is used to determine a set of local maxima, which we take to approximate the mixture component centers. Around each mode, a local Gaussian approximation is constructed via the Laplace approximation. Finally, the mixture weights are determined through constrained least squares regression. The robustness and scalability of the proposed methodology is demonstrated through application to an ensemble of synthetic tests using high-dimensional, multimodal probability density functions. Here, the practical aspects of the approach are demonstrated with inversion problems in structural dynamics.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Selective and Scalable Control of Spin Quantum Memories in a Photonic Circuit

A central goal in many quantum information processing applications is a network of quantum memories that can be entangled with each other while being individually controlled and measured with high fidelity. This goal has motivated the development of programmable photonic integrated circuits (PICs) with integrated spin quantum memories using diamond color center spin-photon interfaces. However, this approach introduces a challenge into the microwave control of individual spins within closely packed registers. Here, we present a quantum memory-integrated photonics platform capable of (i) the integration of multiple diamond color center spins into a cryogenically compatible, high-speed programmable PIC platform, (ii) selective manipulation of individual spin qubits addressed via tunable magnetic field gradients, and (iii) simultaneous control of qubits using numerically optimized microwave pulse shaping. The combination of localized optical control, enabled by the PIC platform, together with selective spin manipulation opens the path to scalable quantum networks on intrachip and interchip platforms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Structural Changes during the Conversion Reaction of Tungsten Oxide Electrodes with Tailored, Mesoscale Porosity

In-plane tungsten oxide nanostructures, including hexagonally patterned cylinders and holes in a matrix, were fabricated via sequential infiltration synthesis (SIS) on self-assembled block copolymer templates. Using the tailored morphology and porosity of these model electrodes with in situ grazing incidence small angle X-ray scattering, the intrinsic structural change of nanoscale active materials during the conversion reaction of WO 3 + 6Li ↔ W + 3 Li 2 O was investigated at controlled electrochemical conditions. Reversible electrode volume expansion and contraction was observed during lithiation and delithiation cycles, respectively. The potential where electrode’s thickness expansion started was ~1.6 V, which is close to thermodynamically expected one for conversion reaction of WO 3 with lithium (1.65 V). The temporal evolution of the electrode volume at constant electrode potentials revealed high overpotential for bulk lithiation and slow conversion reaction kinetics, despite the tailored porosity of the SIS electrodes. Oxide cylinders showed smaller overall electrode thickness change, likely due to unconstrained lateral volume change, as compared to a matrix with holes. On the other hand, better connectivity and guided volume change of the latter electrode morphology provided improved cycling stability. Additionally, heterogeneity in an electrode, from internal pores and density gradients, was found to aggravate the fragmentation of the electrode during conversion reaction. Insights into oxide conversion reaction kinetics and the relationship between electrode mesostructure and cycling behavior obtained from this study can help guide the more rational design of conversion electrode for high performing batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Localized Evaluation for Constructing Discrete Vector Fields

Topological abstractions offer a method to summarize the behavior of vector fields, but computing them robustly can be challenging due to numerical precision issues. One alternative is to represent the vector field using a discrete approach, which constructs a collection of pairs of simplices in the input mesh that satisfies criteria introduced by Forman's discrete Morse theory. While numerous approaches exist to compute pairs in the restricted case of the gradient of a scalar field, state-of-the-art algorithms for the general case of vector fields require expensive optimization procedures. This paper introduces a fast, novel approach for pairing simplices of two-dimensional, triangulated vector fields that do not vary in time. The key insight of our approach is that we can employ a local evaluation, inspired by the approach used to construct a discrete gradient field, where every simplex in a mesh is considered by no more than one of its vertices. Specifically, we observe that for any edge in the input mesh, we can uniquely assign an outward direction of flow. We can further expand this consistent notion of outward flow at each vertex, which corresponds to the concept of a downhill flow in the case of scalar fields. Working with outward flow enables a linear-time algorithm that processes the (outward) neighborhoods of each vertex one-by-one, similar to the approach used for scalar fields. Here, we couple our approach to constructing discrete vector fields with a method to extract, simplify, and visualize topological features. Empirical results on analytic and simulation data demonstrate drastic improvements in running time, produce features similar to the current state-of-the-art, and show the application of simplification to large, complex flows.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2021

From Molecules to Solids: A vdW-DF-C09 Case Study of the Mercury Dihalides

The mercury dihalides show a remarkable diversity in the structural preferences in their minimum energy structure types, spanning molecular to strongly bound ionic solids. A challenge in the development of density functional methods for extended systems is to arrive at strategies that serve equally well such a broad range of bonding modes or structural preferences. The chemical bonding and the stabilities of mercury dihalides and the general utility and reliability of the van der Waals density functional with C09 exchange (vdW-DF-C09) in predicting or describing the energetics and structural preferences in these metal dihalides is examined. Here, we show that, in contrast with the uncorrected generalized gradient approximation of the Perdew-Burke-Erzenhoff (PBE) exchange-correlation functional, qualitative and quantitative patterns in the bonding of the mercury dihalide solids are well reproduced with vdW-DF-C09 for the full series of HgX 2 systems for X = F, Cl, Br, and I. The possible existence of a low-temperature cotunnite polymorph for HgF 2 and PbF 2 is posited.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗