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NASA NTRS1989

Infrared backscattering

All particles in the atmosphere are not spherical. Moreover, the scattering properties of randomly oriented nonspherical particles are not equivalent to those of spherical particles no matter how the term equivalent is defined. This is especially true for scattering in the backward direction and at the infrared wavelengths at which some atmospheric particles have strong absorption bands. Thus calculations based on Mie theory of infrared backscattering by dry or insoluble atmospheric particles are suspect. To support this assertion, it was noted that peaks in laboratory-measured infrared backscattering spectra show appreciable shifts compared with those calculated using Mie theory. One example is ammonium sulfate. Some success was had in modeling backscattering spectra of ammonium sulfate particles using a simple statistical theory called the continuous distribution of ellipsoids (CDE) theory. In this theory, the scattering properties of an ensemble are calculated. Recently a modified version of this theory was applied to measured spectra of scattering by kaolin particles. The particles were platelike, so the probability distribution of ellipsoidal shapes was chosen to reflect this. As with ammonium sulfate, the wavelength of measured peak backscattering is shifted longward of that predicted by Mie theory.

Bohren, Craig F.↗

DOE OSTI2021

Calculation of self-diffusion coefficients in supercritical carbon dioxide using mean force kinetic theory

This paper presents an application of mean force kinetic theory (MFT) to the calculation of the self-diffusivity of CO 2 in the supercritical fluid regime. Two modifications to the typical application of MFT are employed to allow its application to a system of molecular species. Therefore, the first is the assumption that the inter-particle potential of mean force can be obtained from the molecule center-of-mass pair correlation function, which in the case of CO 2 is the C–C pair correlation function. The second is a new definition of the Enskog factor that describes the effect of correlations at the surface of the collision volume. The new definition retains the physical picture that this quantity represents a local density increase, resulting from particle correlations, relative to that in the zero density homogeneous fluid limit. These calculations are facilitated by the calculation of pair correlation functions from molecular dynamics (MD) simulations using the FEPM2 molecular CO2 model. The self-diffusivity calculated from theory is in good agreement with that from MD simulations up to and slightly beyond the density at the location of the Frenkel line. The calculation is compared with and is found to perform similarly well to other commonly used models but has a greater potential for application to systems of mixed species and to systems of particles with long range interatomic potentials due to electrostatic interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2024

Enhancing Consistency of Microphysical Properties of Precipitation Across the Melting Layer in the Dual-Frequency Precipitation Radar Data

Stratiform rain and the overlying ice play crucial roles in Earth's climate system. From a microphysics standpoint, water mass flux primarily depends on two variables: particles' concentration and their mass. The Dual-frequency Precipitation Radar (DPR) on the Global Precipitation Measurement mission core satellite is a spaceborne instrument capable of estimating these two quantities through dual-wavelength measurements. In this study, we evaluate bulk statistics on the ice particle properties derived from dual-wavelength radar data in relation to the properties of rain underneath. Specifically, we focus on DPR observations over stratiform precipitation, characterized by columns exhibiting a prominent bright band, where the melting layer can be easily detected. Our analysis reveals a large increase in the retrieved mass flux as we transition from the ice to the rain phase in the official DPR product. This observation is in disagreement with our expectation that mass flux should remain relatively stable across the bright band in cold-rain conditions. To address these discrepancies, we propose an alternative retrieval algorithm that ensures a gradual transition of Dm (mean mass-weighted particle melted-equivalent diameter) and the precipitation rate across the melting zone. This approach also helps in estimating bulk ice density above the melting level. These findings demonstrate that DPR observations can not only quantify ice particle content and their size above stratiform rain regions but also estimate bulk density, provided uniform conditions that minimize uncertainties related to partial beam filling.

radar measurements from space↗

DOE OSTI2022

Quantifying the Impact of Charge Rate and Number of Cycles on Structural Degeneration of Li-Ion Battery Electrodes

A quantitative link between crack evolution in lithium-ion positive electrodes and the degrading performance on cells is not yet well established nor is any single technique capable of doing so widely available. Here, we demonstrate a widely accessible high-throughput approach to quantifying crack evolution within electrodes. The approach applies super-resolution scanning electron microscopy (SEM) imaging of cross-sectioned NMC532 electrodes, followed by segmentation and quantification of crack features. Crack properties such as crack intensity, crack width and length are quantified as a function of charge rate (1C, 6C, and 9C) and cycle number (25, 225, and 600 cycles). Hundreds of particles are characterized for statistical confidence in the quantitative crack measurements. The data on crack evolution is compared to electrochemical data from full cells and half cells with the NMC532 positive electrodes. We show that while crack evolution strongly correlates with capacity fade in the first 25 cycles, it does not correlate well for the following hundreds of cycles indicating that cracking may not be the dominant cause of capacity fade throughout the cycle-life of cells.

25 ENERGY STORAGE↗

NASA NTRS2018

Very Narrow Coronal Mass Ejections Producing Solar Energetic Particles

Aims. Our main aim is to study the relationship between low-energy solar particles (energies below 1 MeV) and very narrow coronal mass ejections (“jets” with angular width ≤ 20°). Methods. For this purpose, we considered 125 very narrow coronal mass ejections (CMEs) from 1999 to 2003 that are potentially associated with low-energy solar particles (LESPs). These events were chosen on the basis of their source location. We studied only very narrow CMEs at the western limb, which are expected to have good magnetic connectivity with Earth. Results. We found 24 very narrow CMEs associated with energetic particles such as ions (protons and 3He), electrons, or both. We show that arrival times at Earth of energetic particles are consistent with onset times of the respective CMEs, and that in the same time intervals, there are no other potential sources of energetic particles. We also demonstrate statistical differences for the angular width distributions using the Kolmogorov–Smirnov test for angular widths for these 24 events. We consider a coherent sample of jets (mostly originating from boundaries of coronal holes) to identify properties of events that produce solar energetic particles (velocities, widths, and position angles). Our study presents a new approach and result: very narrow CMEs can generate low-energy particles in the vicinity of Earth without other activity on the Sun. The results could be very useful for space weather forecasting.

Bronarska, K.↗

DOE OSTI2023

Search for heavy long-lived multi-charged particles in the full LHC Run 2 pp collision data at s = 13 TeV using the ATLAS detector

A search for heavy long-lived multi-charged particles is performed using the ATLAS detector at the LHC. Data collected in 2015-2018 at $\sqrt{s}$ = 13 TeV from pp collisions corresponding to an integrated luminosity of 139 fb -1 are examined. Particles producing anomalously high ionization, consistent with long-lived spin-$\frac{1}{2}$ massive particles with electric charges from |q|=2e to |q|=7e are searched for. No statistically significant evidence of such particles is observed, and 95% confidence level cross-section upper limits are calculated and interpreted as the lower mass limits for a Drell-Yan plus photon-fusion production mode. The least stringent limit, 1060 GeV, is obtained for |q|=2e particles, and the most stringent one, 1600 GeV, is for |q|=6e particles.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Compression behavior of microcrystalline cellulose spheres: Single particle compression and confined bulk compression across regimes

Particle characteristics can drastically influence the process-structure-property-performance aspects of granular materials in compression. In this study, we aim to computationally simulate the mechanical processes of stress redistribution in compacts including the kinematics of particle rearrangement during densification and particle deformation leading to fragmentation. Confined compression experiments are conducted with three sets of commercial microcrystalline cellulose particles nearly spherical in shape with different mean particle size. Experimentally measured compression curves from tall powder columns are fitted with the Kenkre et al. (J. of American Chemical Society, Vol. 79, No. 12) model. This model provides a basis to derive several common two-parameter literature models and as a framework to incorporate statistical representations of critical particle behaviors. We focus on the low-stress compression data and the model comparisons typically not discussed in the literature. Furthermore, additional single particle compressions report fracture strength with particle size for comparison to the apparent particle strength extracted from bulk compression data.

42 ENGINEERING↗

DOE OSTI2022

Nanotomographic observation and statistical analysis of overcharging induced cracks in LiCoO 2 single crystalline particles

Particle fracture represents an important mode of battery electrode degradation. Extensive cracking occurs in the layered oxide cathodes of lithium-ion rechargeable batteries when they are charged beyond safe operational voltages. In this paper, we analyze the morphology and distribution of cracks in over 100 overcharged LiCoO 2 (LCO) single-crystalline particles imaged via X-ray nanotomography. Herein, we observe a strong particle size dependence in both nucleation and growth of cracks, with percentage of cracked particles, crack size, and crack surface area per unit volume all increasing significantly with particle volume. Increasing the cutoff voltage above 4.6V is found to trigger much more pronounced crack growth, which we attribute to the large misfit stress caused by the H1-3 to O1 phase transition. This study offers valuable statistical insights into the fracture behavior of layered oxide cathodes and reveals the importance of particle size control on electromechanical degradation of battery electrodes.

25 ENERGY STORAGE↗

NASA NTRS2000

Inertial Effects in Suspension Dynamics

The present work analyses the dynamics of a suspension of heavy particles in shear flow. The magnitude of the particle inertia is given by the Stokes number St = m(gamma/6(pi)a, which is the ratio of the viscous relaxation time of a particle tau(sub p) = m=6pi(eta)a to the flow time gamma(sup -1). Here, m is the mass of the particle, a is its size, eta is the viscosity of the suspending fluid and gamma is the shear rate. The ratio of the Stokes number to the Reynolds number, Re = (rho)f(gamma)a(exp 2)/eta, is the density ratio rho(sub p)/rho(sub f). Of interest is to understand the separate roles of particle (St) and fluid (Re) inertia in the dynamics of suspensions. In this study we focus on heavy particles, rho(sub p)/rho(sub f) much greater than 1, for which the Stokes number is finite, but the Reynolds number is sufficiently small for inertial forces in the fluid to be neglected; thus, the fluid motion is governed by the Stokes equations. On the other hand, the probability density governing the statistics of the suspended particles satisfies a Fokker-Planck equation that accounts for both configuration and momentum coordinates, the latter being essential for finite St. The solution of the Fokker-Planck equation is obtained to O(St) via a Chapman-Enskog type-procedure, and the conditional velocity distribution so obtained is used to derive a configuration-space Smoluchowski equation with inertial corrections. The inertial effects are responsible for asymmetry in the relative trajectories of two spheres in shear flow, in contrast to the well known symmetric structure in the absence of inertia. Finite St open trajectories in the plane of shear suffer a downward lateral displacement resulting from the inability of a particle of finite mass to follow the curvature of the zero-Stokes-number pathlines. In addition to the induced asymmetry, the O(St) inertial perturbation dramatically alters the nature of the near-field trajectories. The stable closed orbits (for St = 0) in the plane of shear now spiral in, approaching particle-particle contact in the limit. All trajectories starting from an initial offset of O(St(sup 1/2) or less (which remain open for St = 0) also spiral in. The asymmetry of the trajectories leads to a non-Newtonian rheology and diffusive behavior. The latter because a given particle (moving along a finite St open trajectory) suffers a net displacement in the transverse direction after a single interaction. A sequence of such uncorrelated displacements leads to the particle executing a random walk. The inertial diffusivity tensor is anisotropic on account of differing strengths of interaction in the gradient and vorticity directions. Since the entire region (constituting an in finite area) of closed orbits in the plane of shear spirals onto contact for #finite St, the latter represents a singular surface for the pair-distribution function. The exact form of the pair-distribution function at contact is still, however, indeterminate in the absence of non-hydrodynamic effects. It should also be noted that finite St non-rectilinear flows do not support a spatially uniform number density owing to the cross-streamline inertial migration of particles.

J. F. Brady↗

NASA NTRS1980

Distribution function representation of energy spectra of H, He, C, O and Fe in corotating particle streams

From an analysis of nine corotating events observed near 1 AU during the 1974-1976 solar minimum, the spectral parameters for H, He, C, O and Fe and relative abundances of these elements and of Ne, Mg, Si, and S-Ca were determined. The distribution functions of H, He, O and Fe are well represented by an exponential in particle speed over the energy range of the measurements from 0.3 to 5 MeV/nucleon. The composition resembles that of the solar corona, particularly in the O/C ratio which is 0.95 + or - 0.19, and the He/H and He/Ne ratios are similar to the respective ratios in the solar wind. The results are consistent with interplanetary statistical acceleration of these particles out of the high-energy tail of the high-speed solar wind.

Gloeckler, G.↗

NASA NTRS1973

Electron precipitation patterns and substorm morphology.

Statistical analysis of data from the auroral particles experiment aboard OGO 4, performed in a statistical framework interpretable in terms of magnetospheric substorm morphology, both spatial and temporal. Patterns of low-energy electron precipitation observed by polar satellites are examined as functions of substorm phase. The implications of the precipitation boundaries identifiable at the low-latitude edge of polar cusp electron precipitation and at the poleward edge of precipitation in the premidnight sector are discussed.

Hoffman, R. A.↗

NASA NTRS2002

A Theoretical Study of the Global Geospace System Simulations

This report describes work undertaken by the principal investigator (PI) and her colleagues in three areas of research: Relativistic Electron Dynamics, Solar Energetic Particle Study, and ULF Wave Statistical Study. The researchers conducted three dimensional modeling of relativistic electron dynamics, simulated Solar Energetic Particles (SEP) trapping using a magnetohydrodynamic (MHD) code, and a study of Pc 5 magnetic pulsations.

Hudson, Mary K.↗

DOE OSTI2021

Phase-field model of precipitation processes with coherency loss

A phase-field model is proposed to simulate coherency loss coupled with microstructure evolution. A special field variable is employed to describe the degree of coherency loss of each particle and its evolution is governed by a Ginzburg-Landau type kinetic equation. For the sake of computational efficiency, a flood-fill algorithm is introduced that can drastically reduce the required number of field variables, which allows the model to efficiently simulate a large number of particles sufficient for characterizing their statistical features during Ostwald ripening. The model can incorporate size dependence of coherency loss, metastability of coherent particles, and effectively incorporate the underlying mechanisms of coherency loss by introducing a so-called differential energy criterion. The model is applied to simulate coarsening of Al 3 Sc precipitates in aluminum alloy and comprehensively compared with experiments. Our results clearly show how the particle size distribution is changed during coherency loss and affects the coarsening rate.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Stochastic 3D reconstruction of cracked polycrystalline NMC particles using 2D SEM data

Li-ion battery performance is strongly influenced by the 3D microstructure of its cathode particles. Cracks within these particles develop during calendaring and cycling, reducing connectivity but increasing reactive surface, making their impact on battery performance complex. Understanding these contradictory effects requires a quantitative link between particle morphology and battery performance. However, informative 3D imaging techniques are time-consuming, costly and rarely available, such that analyses often have to rely on 2D image data. This paper presents a novel stereological approach for generating virtual 3D cathode particles exhibiting crack networks that are statistically equivalent to those observed in 2D sections of experimentally measured particles. Consequently, 2D image data suffices for deriving a full 3D characterization of cracked cathodes particles. Such virtually generated 3D particles could serve as geometry input for spatially resolved electro-chemo-mechanical simulations to enhance our understanding of structure-property relationships of cathodes in Li-ion batteries.

36 MATERIALS SCIENCE↗

NASA NTRS1999

Predicting Slag Generation in Sub-Scale Test Motors Using a Neural Network

Generation of slag (aluminum oxide) is an important issue for the Reusable Solid Rocket Motor (RSRM). Thiokol performed testing to quantify the relationship between raw material variations and slag generation in solid propellants by testing sub-scale motors cast with propellant containing various combinations of aluminum fuel and ammonium perchlorate (AP) oxidizer particle sizes. The test data were analyzed using statistical methods and an artificial neural network. This paper primarily addresses the neural network results with some comparisons to the statistical results. The neural network showed that the particle sizes of both the aluminum and unground AP have a measurable effect on slag generation. The neural network analysis showed that aluminum particle size is the dominant driver in slag generation, about 40% more influential than AP. The network predictions of the amount of slag produced during firing of sub-scale motors were 16% better than the predictions of a statistically derived empirical equation. Another neural network successfully characterized the slag generated during full-scale motor tests. The success is attributable to the ability of neural networks to characterize multiple complex factors including interactions that affect slag generation.

Wiesenberg, Brent↗

DOE OSTI2022

Imaging Phase Segregation in Nanoscale Li x CoO 2 Single Particles

Li x CoO 2 (LCO) is a common battery cathode material that has recently emerged as a promising material for other applications including electrocatalysis and as electrochemical random access memory (ECRAM). During charge– discharge cycling LCO exhibits phase transformations that are significantly complicated by electron correlation. While the bulk phase diagram for an ensemble of battery particles has been studied extensively, it remains unclear how these phases scale to nanometer dimensions and the effects of strain and diffusional anisotropy at the single-particle scale. Understanding these effects is critical to modeling battery performance and for predicting the scalability and performance of electrocatalysts and ECRAM. Here we investigate isolated, epitaxial LiCoO 2 islands grown by pulsed laser deposition. After electrochemical cycling of the islands, conductive atomic force microscopy (c-AFM) is used to image the spatial distribution of conductive and insulating phases. Above 20 nm island thicknesses, we observe a kinetically arrested state in which the phase boundary is perpendicular to the Li-planes; we propose a model and present image analysis results that show smaller LCO islands have a higher conductive fraction than larger area islands, and the overall conductive fraction is consistent with the lithiation state. Thinner islands (14 nm), with a larger surface to volume ratio, are found to exhibit a striping pattern, which suggests surface energy can dominate below a critical dimension. When increasing force is applied through the AFM tip to strain the LCO islands, significant shifts in current flow are observed, and underlying mechanisms for this behavior are discussed. The c-AFM images are compared with photoemission electron microscopy images, which are used to acquire statistics across hundreds of particles. Finally, the results indicate that strain and morphology become more critical to electrochemical performance as particles approach nanometer dimensions.

25 ENERGY STORAGE↗

DOE OSTI2022

Simple and statistically sound recommendations for analysing physical theories

Physical theories that depend on many parameters or are tested against data from many different experiments pose unique challenges to statistical inference. Many models in particle physics, astrophysics and cosmology fall into one or both of these categories. These issues are often sidestepped with statistically unsound ad hoc methods, involving intersection of parameter intervals estimated by multiple experiments, and random or grid sampling of model parameters. Whilst these methods are easy to apply, they exhibit pathologies even in low-dimensional parameter spaces, and quickly become problematic to use and interpret in higher dimensions. In this article we give clear guidance for going beyond these procedures, suggesting where possible simple methods for performing statistically sound inference, and recommendations of readily-available software tools and standards that can assist in doing so. Our aim is to provide any physicists lacking comprehensive statistical training with recommendations for reaching correct scientific conclusions, with only a modest increase in analysis burden. Furthermore, our examples can be reproduced with the code publicly available at Zenodo.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

NASA NTRS1977

Solar particle propagation from 1 to 5 AU

The radial variation of the interplanetary propagation of solar cosmic rays is investigated on a grand scale by performing a statistical analysis of charged-particle data obtained by Pioneers 10 and 11 from launch to Jovian encounter (i.e., at distances of 1 to 5 AU). A numerical propagation model is adopted which includes diffusion, convection, and adiabatic deceleration, as well as a variable power-law diffusion coefficient. The study of solar particle events is carried out by analyzing individually each of five key parameters that are uniquely defined in each solar particle event: the time to maximum flux starting from the initial release at the sun, the anisotropy at the time to maximum flux, the flux at that time, the time width of the event at half the flux at the time to maximum, and the decay time. Combined results for the proton energy ranges from 3.4 to 5.2 MeV and 24 to 30 MeV are presented, the average radial diffusion coefficients between 1 and 5 AU are determined for each energy range, and it is found that the combination of a near-impusive injection with a temporally constant spectral index produces a reasonably good fit to the high-energy data but not as good a fit to the low-energy data. Implications of the results obtained are discussed for cosmic-ray propagation theory, solar modulation studies, and interplanetary acceleration of solar particles.

Zwickl, R. D.↗