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At least 1,171 records · Page 65

Analysis of the Reactive CO 2 Surface Flux in Electrocatalytic Aqueous Flow Reactors

We study how the mass transfer of a chemical species in shear flow is suppressed by the production of a second species that partially reacts away the first species. The second species is produced at the surface with the first species as a reactant. Our work is directly motivated by electrochemical CO 2 reduction in aqueous flow reactors, where OH– molecules generated by the CO evolution reaction react away CO 2 molecules, ultimately inhibiting the mass transfer of CO 2 to the cathode surface. We derive a simple approximation of the Sherwood number, a dimensionless measure of the mass flux into the surface, as a function of the Péclet number, surface Damköhler number, and bulk Damköhler number, and we compare our approximation to numerical solutions of the governing equations. We find that in the diffusion-limited regime, the Sherwood number is well described by the classical Graetz-Lévêque result reduced by a reaction factor due to the competing bulk reaction; with the stoichiometry relevant to electrochemical CO 2 reduction, this reaction factor is 1/2. While the model problem we solve provides insight into how OH– production affects CO 2 mass transfer, experimental systems often involve more complex chemistry. We thus also show how a common buffered electrolyte, KHCO 3 , affects our results.

30 DIRECT ENERGY CONVERSION↗

Quark Sivers Function at Small-$x$: Leading contribution from the Spin-Dependent Odderon

We present the calculation of the leading contribution to the quark Sivers function at small-Bjorken x as in [1]. This calculation uses the high energy scattering approximation and operator formalism developed in [2,3] to obtain a dominant contribution to the quark Sivers function coming from the spin-dependent odderon, in agreement with the results of [4]. We then calculate this dominant contribution in the diquark model of the proton to obtain a small-x estimate for the Sivers function.

Santiago, M. Gabriel↗

First-Principle Study of the Electronic and Magnetic Properties of Nd{sub 1−x}La{sub x}FeSi Alloys (x = 0, 0.25, 0.50, 0.75, and 1)

The structural, electronic, and magnetic properties of Nd{sub 1−x}La{sub x}FeSi (x = 0, 0.25, 0.50, 0.75, and 1) alloys are investigated based on the first-principle density functional theory by using the full-potential linear muffin-tin orbital (FP-LMTO) method. The exchange-correlation potential is treated with local density approximation (LDA). In addition, to treat localization of 4f-electrons properly, the LDA + U approach (where U is the Hubbard correlation term) is also employed. The calculated structural, electronic, and magnetic properties of these alloys within LDA and LDA + U approaches are compared. The calculated lattice constants of these alloys as a function of x within the LDA + U approach are in the best agreement with linear Vegard’s rule. Most importantly, we focus on the magnetic properties of these alloys and find that the magnetic interaction between Nd atoms is the Rudermen-Kittel-Kasuya-Yosida (RKKY) interaction type. Iron does not carry magnetic moment in these alloys and has just an induced small magnetic moment from Nd atoms.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Computation of Auger Electron Spectra in Organic Molecules with Multiconfiguration Pair-Density Functional Theory

Efficient and accurate computation of molecular Auger electron spectra for larger systems is limited by the rapid increase in the number of doubly ionized final states as the system size grows. Here, in this work, we benchmark the application of multiconfiguration pair-density functional theory with a restricted active space (RAS) reference wave function for computing the carbon K-edge decay spectra of 20 organic molecules. Decay rates are computed within the one-center approximation. We evaluate the performance of different basis sets and on-top functionals and find that multiconfiguration pair-density functional theory achieves accuracy comparable to RAS followed by second-order perturbation theory, but at significantly lower computational cost.

Fouda, Adam E. A. [Argonne National Laboratory (AN↗

First-Principle Calculations of Structural, Elastic, and Electronic Properties of Intermetallic Rare Earth R{sub 2}Ni{sub 2}Pb (R = Ho, Lu, and Sm) Compounds

The structural, elastic, and electronic properties of rare earth intermetallic R{sub 2}Ni{sub 2}Pb (where R = Ho, Lu, and Sm) compounds were investigated with the density functional theory (DFT) calculations. The calculations are performed using the full potential-linearized augmented plane wave (FP-LAPW) method within the framework of local density approximation (LDA). The calculated values of the equilibrium lattice constants were in agreement with the available experimental values. The elastic constants (C{sub ij}) were also calculated to understand the mechanical properties and structural stability of the compounds. Furthermore, the density of states and the charge density distributions of the compounds were calculated to understand the nature of the bonding in the material. The calculated results are in accordance with the available data in the literature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

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↗

Estimation of Sea Spray Aerosol Surface Area Over the Southern Ocean Using Scattering Measurements

This study focuses on methods to estimate dry marine aerosol surface area (SA) from bulk optical measurements. Aerosol SA is used in many models' ice nucleating particle (INP) parameterizations, as well as influencing particle light scattering, hygroscopic growth, and reactivity, but direct observations are scarce in the Southern Ocean (SO). Two campaigns jointly conducted in austral summer 2018 provided co-located measurements of aerosol SA from particle size distributions and lidar to evaluate SA estimation methods in this region. Mie theory calculations based on measured size distributions were used to test a proposed approximation for dry aerosol SA, which relies on estimating effective scattering efficiency (Q) as a function of Ångström exponent (å). For distributions with dry å < 1, Q = 2 was found to be a good approximation within ±50%, but for distributions with dry å > 1, an assumption of Q = 3 as in some prior studies underestimates dry aerosol SA by a factor of 2 or more. We propose a new relationship between dry å and Q, which can be used for –0.2 < å < 2, and suggest å = 0.8 as the cutoff between primary and secondary marine aerosol-dominated distributions. Application of a published methodology to retrieve dry marine aerosol SA from lidar extinction profiles overestimated aerosol SA by a factor of 3–5 during these campaigns. Using Microtops aerosol optical thickness measurements, we derive alternative lidar conversion parameters from our observations, applicable to marine aerosol over the SO.

54 ENVIRONMENTAL SCIENCES↗

Fast Emulation of Expensive Simulations using Approximate Gaussian Processes [Slides]

Nuclear Computational Low-Energy Initiative (NUCLEI) collaboration uses Density Functional Theory (DFT) simulations to predict the structure and binding energies of nuclei over a wide range of proton (Z) and neutron (N) numbers. The DFT simulations utilize a particular parameterization of a Skyrme energy density functional called UNEDF1 which depends on 12 free parameters that must be fit to data (M Kortelainen et al 2014). Fitting involves comparing (e.g.) predicted binding energies of nuclei to experimentally measured values. We use only binding energies as observables, but DFT with UNEDF1 will predict structure (shape) observables as well. In this work, assessing the capability of approximate GP emulators to balance emulator accuracy with computational speed to facilitate improved UNEDF1 calibration. Sparse GPs are straightforward to train and accurate. Calibration is not straightforward with MCMC (using MH or HMC/NUTS). We produced reusable software for continuing and building on this work as well as accessing and using Darwin cluster compute resources

97 MATHEMATICS AND COMPUTING↗

Ab Initio Study of Electronic and Magnetic Properties in ZnO-Doped and Co-doped by Vanadium and Silver

Based upon the ab initio of spin density functional calculation, the electronic and magnetic properties of Zn{sub 1−x}M{sub x}O (M = Ag or V) and Zn{sub 1−x−y}A{sub x}B{sub y}O (A = V; B = Ag) are investigated, using the Korringa-Kohn-Rostoker (KKR) method coupled with the coherent potential approximation (CPA). The total and partial densities of state are calculated. The effect of concentration values in Zn{sub 1−x}V{sub x}O and Zn{sub 1−x−y}V{sub x}Ag{sub y}O are deduced. Moreover, the magnetic disorder local moment (DLM) and the total energy are obtained for different concentration values of doped and co-doped zinc oxide (ZnO).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Deep Learning Approaches to Surrogates for Solving the Diffusion Equation for Mechanistic Real-World Simulations

In many mechanistic medical, biological, physical, and engineered spatiotemporal dynamic models the numerical solution of partial differential equations (PDEs), especially for diffusion, fluid flow and mechanical relaxation, can make simulations impractically slow. Biological models of tissues and organs often require the simultaneous calculation of the spatial variation of concentration of dozens of diffusing chemical species. One clinical example where rapid calculation of a diffusing field is of use is the estimation of oxygen gradients in the retina, based on imaging of the retinal vasculature, to guide surgical interventions in diabetic retinopathy. Furthermore, the ability to predict blood perfusion and oxygenation may one day guide clinical interventions in diverse settings, i.e., from stent placement in treating heart disease to BOLD fMRI interpretation in evaluating cognitive function (Xie et al., 2019; Lee et al., 2020). Since the quasi-steady-state solutions required for fast-diffusing chemical species like oxygen are particularly computationally costly, we consider the use of a neural network to provide an approximate solution to the steady-state diffusion equation. Machine learning surrogates, neural networks trained to provide approximate solutions to such complicated numerical problems, can often provide speed-ups of several orders of magnitude compared to direct calculation. Surrogates of PDEs could enable use of larger and more detailed models than are possible with direct calculation and can make including such simulations in real-time or near-real time workflows practical. Creating a surrogate requires running the direct calculation tens of thousands of times to generate training data and then training the neural network, both of which are computationally expensive. Often the practical applications of such models require thousands to millions of replica simulations, for example for parameter identification and uncertainty quantification, each of which gains speed from surrogate use and rapidly recovers the up-front costs of surrogate generation. We use a Convolutional Neural Network to approximate the stationary solution to the diffusion equation in the case of two equal-diameter, circular, constant-value sources located at random positions in a two-dimensional square domain with absorbing boundary conditions. Such a configuration caricatures the chemical concentration field of a fast-diffusing species like oxygen in a tissue with two parallel blood vessels in a cross section perpendicular to the two blood vessels. To improve convergence during training, we apply a training approach that uses roll-back to reject stochastic changes to the network that increase the loss function. The trained neural network approximation is about 1000 times faster than the direct calculation for individual replicas. Because different applications will have different criteria for acceptable approximation accuracy, we discuss a variety of loss functions and accuracy estimators that can help select the best network for a particular application. We briefly discuss some of the issues we encountered with overfitting, mismapping of the field values and the geometrical conditions that lead to large absolute and relative errors in the approximate solution.

60 APPLIED LIFE SCIENCES↗

Quantification of electron correlation for approximate quantum calculations

State-of-the-art many-body wave function techniques rely on heuristics to achieve high accuracy at an attainable computational cost to solve the many-body Schrödinger equation. By far, the most common property used to assess accuracy has been the total energy; however, total energies do not give a complete picture of electron correlation. In this work, we assess the von Neumann entropy of the one-particle reduced density matrix (1-RDM) to compare selected configuration interaction (CI), coupled cluster, variational Monte Carlo, and fixed-node diffusion Monte Carlo for benchmark hydrogen chains. A new algorithm, the circle reject method, is presented, which improves the efficiency of evaluating the von Neumann entropy using quantum Monte Carlo by several orders of magnitude. The von Neumann entropy of the 1-RDM and the eigenvalues of the 1-RDM are shown to distinguish between the dynamic correlation introduced by the Jastrow and the static correlation introduced by determinants with large weights, confirming some of the lore in the field concerning the difference between the selected CI and Slater–Jastrow wave functions.

Chemistry↗

Magnetic ground state and perturbations of the distorted kagome Ising metal TmAgGe

Here, we present the magnetic orders and excitations of the distorted kagome intermetallic magnet TmAgGe. Using neutron single crystal diffraction we identify the propagation vectors k = ($\frac{1}{2}$ 0 0) and k = (0 0 0) and determine the magnetic structures of the zero-field and magnetic field-induced phases for H along the $\mathcal{a}$ and [–110] crystal directions. We determine the experimental magnetic field- temperature (H, T)-phase diagram and reproduce it by Monte Carlo simulations of an effective spin exchange Hamiltonian for one distorted kagome layer. Our model includes a strong axial single-ion anisotropy and significantly smaller exchange couplings, which span up to the third-nearest neighbors within the layer. Single crystal inelastic neutron scattering (INS) measurements reveal an almost flat, only weakly dispersive mode around 7 meV that we use alongside bulk magnetization data to deduce the crystal-electric field (CEF) scheme for the Tm 3+ ions. Random phase approximation (RPA) calculations based on the determined CEF wave functions of the two lowest quasidoublets enable an estimation of the interlayer coupling that is compatible with the experimental INS spectra. No evidence for low-energy spin waves associated to the magnetic order was found, which is consistent with the strongly Ising nature of the ground state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Investigation of local distortion effects on X-ray absorption of ferroelectric perovskites from first principles simulations

Understanding the role of ferroelectric polarization in modulating the electronic and structural properties of crystals is critical for advancing these materials for overcoming various technological and scientific challenges. However, due to difficulties in performing experimental methods with the required resolution, or in interpreting the results of methods therein, the nanoscale morphology and response of these surfaces to external electric fields has not been properly elaborated. Here, in this work, we investigate the effect of ferroelectric polarization and local distortions in a BaTiO 3 perovskite, using two widely used computational approaches which treat the many-body nature of X-ray excitations using different philosophies, namely the many-body, delta-self-consistent-field determinant (mb-ΔSCF) and the Bethe–Salpeter equation (BSE) approaches. We show that in agreement with our experiments, both approaches consistently predict higher excitations of the main peak in the O–K edge for the surface with upward polarization. However, the mb-ΔSCF approach mostly fails to capture the L 2,3 separations at the Ti–L edge, due to the absence of spin–orbit coupling in Kohn–Sham density functional theory (KS-DFT) at the generalized gradient approximation level. On the other hand, and most promising, we show that application of the GW/BSE approach successfully reproduces the experimental XAS, both the relative peak intensities as well as the L 2,3 separations at the Ti–L edges upon ferroelectric switching. Thus simulated XAS is shown to be a powerful method for capturing the nanoscale structure of complex materials, and we underscore the need for many-body perturbation approaches, with explicit consideration of core-hole and multiplet effects, for capturing the essential physics in these systems.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Global description of $β$ – decay with the axially deformed Skyrme finite-amplitude method: Extension to odd-mass and odd-odd nuclei

Here we use the finite-amplitude method (FAM), an efficient implementation of the quasiparticle random phase approximation, to compute $β$-decay rates with Skyrme energy-density functionals for 3983 nuclei, essentially all the medium-mass and heavy isotopes on the neutron-rich side of stability. We employ an extension of the FAM that treats odd-mass and odd-odd nuclear ground states in the equal filling approximation. Our rates are in reasonable agreement both with experimental data where available and with rates from other global calculations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Bayesian and variational Bayesian approaches for flows in heterogeneous random media

In this paper, we study porous media flows in heterogeneous stochastic media. We propose an efficient forward simulation technique that is tailored for variational Bayesian inversion. As a starting point, the proposed forward simulation technique decomposes the solution into the sum of separable functions (with respect to randomness and the space), where each term is calculated based on a variational approach. This is similar to Proper Generalized Decomposition (PGD). Next, we apply a multiscale technique to solve for each term (as in ) and, further, decompose the random function into 1D fields. As a result, our proposed method provides an approximation hierarchy for the solution as we increase the number of terms in the expansion and, also, increase the spatial resolution of each term. We use the hierarchical solution distributions in a variational Bayesian approximation to perform uncertainty quantification in the inverse problem. We conduct a detailed numerical study to explore the performance of the proposed uncertainty quantification technique and show the theoretical posterior concentration.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Energy release rate approximation for edge cracks using higher-order topological derivatives

Topological derivatives provide the variation of a functional when an infinitesimal hole is introduced into the domain. In Silva et al. (J Mech Phys Solids 59(5):925–939, 2011), the authors developed a first-order approximation of the energy release rate associated with a small crack at any boundary location and at any orientation using a first-order topological derivative. This approach offers significant computational advantages over other methods because (i) it requires only a single analysis while other methods require an analysis for each crack size-location-direction combination, and (ii) it is performed on the non-cracked domain, removing the need to create very fine meshes in the vicinity of the crack. In the present study, higher-precision approximations of the energy release rate are developed using higher-order topological derivatives which allow the analyst to accurately treat longer cracks and determine the crack lengths for which the first-order approximation is accurate.

42 ENGINEERING↗

Overset-Grid Method with Smooth Orbital Partitioning for Molecular Scattering Calculations

To solve molecular photoionization and electron scattering problems, we use an overset-grid representation of electronic continuum functions, which has an extended central spherical grid that overlaps small spherical grids (subgrids) centered on each atom of a polyatomic molecule. Here, in this work, we present an improved algorithm that smoothly partitions the total wave function between the central grid and the atomic subgrids. The smooth partitioning allows one to use approximately one-fourth the number of partial waves on the central grid compared to our previous implementation with switching functions. The resulting numerical method for treating electron scattering and photoionization of polyatomic molecules combines the accuracy and flexibility of pure numerical grid representations with the rapid convergence of hybrid combinations of atom-centered basis-set expansions and grid methods. The overset-grid representation is implemented using the complex Kohn variational principle for scattering and photoionization amplitudes. The faster convergence with respect to the number of central grid partial waves is demonstrated and accuracy is verified by comparisons with the previous implementation and with far more computationally demanding single-center numerical expansions in electron-molecule scattering and photoionization calculations on the neon dimer (Ne 2 ) system, carbon tetrafluoride (CF 4 ) molecule, and the pyridine (C 5 H 5 N) molecule in the static-exchange approximation.

Molecules↗

A least-squares finite element method based on the Helmholtz decomposition for hyperbolic balance laws

In this paper, a least-squares finite element method for scalar nonlinear hyperbolic balance laws is proposed and studied. The approach is based on a formulation that utilizes an appropriate Helmholtz decomposition of the flux vector and is related to the standard notion of a weak solution. This relationship, together with a corresponding connection to negative-norm least-squares, is described in detail. As a consequence, an important numerical conservation theorem is obtained, similar to the famous Lax–Wendroff theorem. The numerical conservation properties of the method in this paper do not fall precisely in the framework introduced by Lax and Wendroff, but they are similar in spirit as they guarantee that when L 2 convergence holds, the resulting approximations approach a weak solution to the hyperbolic problem. The least-squares functional is continuous and coercive in an H -1 -type norm, but not L 2 -coercive. Nevertheless, the L 2 convergence properties of the method are discussed. Convergence can be obtained either by an explicit regularization of the functional, that provides control of the L 2 norm, or by properly choosing the finite element spaces, providing implicit control of the L 2 norm. Numerical results for the inviscid Burgers equation with discontinuous source terms are shown, demonstrating the L 2 convergence of the obtained approximations to the physically admissible solution. The numerical method utilizes a least-squares functional, minimized on finite element spaces, and a Gauss–Newton technique with nested iteration. Finally, we believe that the linear systems encountered with this formulation are amenable to multigrid techniques and combining the method with adaptive mesh refinement would make this approach an efficient tool for solving balance laws (this is the focus of a future study).

97 MATHEMATICS AND COMPUTING↗