Interpretation of Magnetospheric Cold Particle Distribution Functions Measured with Active Spacecraft Control
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Nuclear particulate fallout is the radioactive byproduct of a nuclear event formed by the mixture of proximate environmental materials with vaporized bomb debris. The debris can be transported into the atmosphere during cloud rise, raining out locally and globally constituting a radiation hazard. Questions remain on how entrainment of environmental material in the fireball affects fallout formation processes and radionuclide incorporation during cooling.
Particle phase state is a property of atmospheric aerosols that has important implications for the formation, evolution, and gas/particle partitioning of secondary organic aerosol (SOA). In this work, we use a size-resolved chemistry and microphysics model (SOM-TOMAS), updated to include an explicit treatment of particle phase state, to constrain the bulk diffusion coefficient (Db) of SOA produced from ??- pinene ozonolysis. By leveraging data from laboratory experiments performed in the absence of a seed and under dry conditions, we find that the Db for SOA can be constrained (1-7 ×10-15 cm2 s-1 in these experiments) by simultaneously reproducing the time-varying SOA mass concentrations and the evolution of the particle size distribution. Another version of our model that used the predicted SOA composition to calculate the glass transition temperature, viscosity, and, ultimately, Db (~10-15 cm2 s-1) of the SOA was able to reproduce the mass and size distribution measurements when we included oligomer formation (oligomers accounted for about a fifth of the SOA mass). Our work highlights the potential of a size resolved SOA model to constrain the particle phase state of SOA by utilizing historical measurements of the evolution of the particle size distribution.
Ambient aerosol particle size distributions measured by the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) at various sites around the world exhibit modes at optical diameters near 600 nm and 850 nm. These modes are not present in concurrent measurements with the Grimm 11-D Optical Particle Counter (OPC). Here, in this study, we argue that these modes result from the optical measurement technique itself, and we explain why they appear in measurements by the UHSAS but not in those by the Grimm OPC. We construct computer models of the UHSAS and Grimm (“digital UHSAS” and “digital Grimm”) and use these to investigate the size distribution that would result from measurements of artificial aerosol particle size distributions that do not contain modes. The appearance of modes for the structureless incoming size distributions sampled by the digital UHSAS is explained by the nonlinear behavior of partial scattering cross sections of uniform spherical particles as a function of their diameter. The absence of modes in the digital Grimm is explained by the coarser size resolution of that instrument. Detailed analysis of the relationship between optical and geometric diameters for uniform spherical particles reveals two important results. First, these diameters generally have different numerical values for the same particle, and second, the relationship is nonlinear; thus, widths of size bins in terms of optical diameter differ from those in geometric diameter. These results explain the modes observed in the ambient size distributions and highlight concerns with attempts to create a merged size distribution by combining measurements from different instruments.
Atmospheric pressure low-temperature plasmas are often utilized to perform particle synthesis, treatment, and removal. It is well-known that dust particles are highly negatively charged in these plasmas; however, little is known about dust particle charging behavior as particles leave the plasma volume and pass through the spatial afterglow region. In this work, monodisperse particles of various sizes and work functions were introduced into an atmospheric pressure radiofrequency capacitively coupled flow-through plasma. Dust particle electrical mobility distributions downstream of the flow-through plasma were measured utilizing a differential mobility analyzer in conjunction with a condensation particle counter at various gas flow velocities. Charge distributions were determined from the measured electrical mobility distributions. Experiments confirm that particles become less negatively charged, and even net-positively charged after leaving the plasma volume, with a distribution that follows a shifted Boltzmann charge distribution. Additionally, particle charge in the effluent of the flow-through plasma is negligibly dependent on work function but highly size and flow velocity dependent. Larger particles were shown to have a higher magnitude of charge under all studied conditions; however, particle polarity was switchable by varying gas flow velocity. The charging dynamics were simulated utilizing a constant number Monte Carlo model that accounts for electron temperature decay and the transition from ambipolar to free diffusion of electrons and ions in the spatial afterglow. Simulation results also suggest that, at the same flow velocity, larger particles obtain a greater magnitude of charge, negative or positive. Furthermore, the decrease in electron mobility and the difference between ion and electron convective loss rates create an ion-rich region in the plasma effluent that promotes ion–particle collisions and drives particle charge removal and even reversal of polarity. Larger particles more favorably collide with energetic species in these environments, which results in higher charge states.
Atmospheric new particle formation (NPF) is a crucial process driving aerosol number concentrations in the atmosphere; it can significantly impact the evolution of atmospheric aerosol and cloud processes. This study analyses at least 1 year of asynchronous particle number size distributions from six different locations in India. We also analyze the frequency of NPF and its contribution to cloud condensation nuclei (CCN) concentrations. We found that the NPF frequency has a considerable seasonal variability. At the measurement sites analyzed in this study, NPF frequently occurs in March–May (pre-monsoon, about 21% of the days) and is the least common in October–November (post-monsoon, about 7% of the days). Considering the NPF events in all locations, the particle formation rate (J SDS ) varied by more than 2 orders of magnitude (0.001–0.6 cm –3 s –1 ) and the growth rate between the smallest detectable size and 25nm (GR SDS-25nm ) by about 3 orders of magnitude (0.2–17.2nm h –1 ). We found that J SDS was higher by nearly 1 order of magnitude during NPF events in urban areas than mountain sites. GR SDS did not show a systematic difference. Our results showed that NPF events could significantly modulate the shape of particle number size distributions and CCN concentrations in India. The contribution of a given NPF event to CCN concentrations was the highest in urban locations (4.3 × 10 3 cm –3 per event and 1.2 × 10 3 cm –3 per event for 50 and 100nm, respectively) as compared to mountain background sites (2.7 × 10 3 cm –3 per event and 1.0 × 10 3 cm –3 per event, respectively). We emphasize that the physical and chemical pathways responsible for NPF and factors that control its contribution to CCN production require in situ field observations using recent advances in aerosol and its precursor gaseous measurement techniques.
A fluidized-particles two-tube solar receiver was tested at ambient temperature at PROMES Laboratory to investigate the influence of an inhomogeneous solar flux density on the particle mass flow rate between the tubes. The principle of this 3rd generation solar receiver is to fluidize the particles in a container, called dispenser, in which the tubes’ bottom are immersed. The fluidized particles are flowing upward the tubes by applying an overpressure in the dispenser. Air velocities are changed inside the tubes, thanks to air mass flow controllers, to represent temperature heterogeneity between the tubes. Air velocities from 0.05 up to 0.52 m/s were tested, both in homogeneous and heterogeneous conditions. In the heterogeneous ones, the differences in air velocity between the tubes aim to mimic a difference in temperature from 20 to 100 % with homogeneous air flow rates injected. The following conclusions were drawn. First, the particle mass flux in the tubes are the same with homogeneous air velocities, each one following a calibration map previously obtained. Second, different air velocities lead to different particle mass flux. Third, the rise of the total particle mass flux diminishes the pressure in the dispenser. Four, this diminution of pressure leads to a decrease of the particle mass flow rate of the tube with the lower air velocity. This influence can lead in some cases to the stop of the fluidized bed circulation in the affected tube.
Particle size distributions measured using a custom scanning mobility analyzer (SMPS) and a TSI, Inc. aerodynamic particle sizer (APS). The size distributions measured with the two instruments were merged during data inversion to produce a single distribution spanning a diameter range from approximately 19 nanometers to 15 micrometers. Size-dependent cloud condensation nuclei (CCN) activity measured with a CCN counter operated in parallel to the condensation particle counter in the SMPS are reported separately. The measurements were made from the Baylor University/University of Houston Mobile Air Quality Laboratory (MAQL) between July 5 and August 30, 2022 during the TRACER-MAP project. The trailer moved between five sites in the Houston regions as follows: Aldine: 7/5-7/8, 7/21-7/26, 8/15-8/24 University of Houston: 7/8-7/16, 8/8-8/15 San Jacinto monument: 7/16-7/21 Jones State Forest: 7/26-8/1; 8/24-8/30 AMF site in La Porte: 8/1-8/8
Particle size distributions measured using a custom scanning mobility analyzer (SMPS) and a TSI, Inc. aerodynamic particle sizer (APS). The size distributions measured with the two instruments were merged during data inversion to produce a single distribution spanning a diameter range from approximately 19 nanometers to 15 micrometers. Size-dependent cloud condensation nuclei (CCN) activity measured with a CCN counter operated in parallel to the condensation particle counter in the SMPS are reported separately. The measurements were made from the Baylor University/University of Houston Mobile Air Quality Laboratory (MAQL) between July 5 and August 30, 2022 during the TRACER-MAP project. The trailer moved between five sites in the Houston regions as follows: Aldine: 7/5-7/8, 7/21-7/26, 8/15-8/24 University of Houston: 7/8-7/16, 8/8-8/15 San Jacinto monument: 7/16-7/21 Jones State Forest: 7/26-8/1; 8/24-8/30 AMF site in La Porte: 8/1-8/8
Particle size distributions using a custom-built SMPS. The measurements were made at the AMF-1 site in La Porte, TX between July 15, 2022 and August 30, 2022. The SMPS alternated between sampling ambient air and that in the portable Captive Aerosol Growth and Evolution (CAGE) chamber. The distributions from those two sources are separated.
An empirical model is presented that describes anode-side losses related to porous transport layer (PTL) morphology in proton exchange membrane water electrolysis (PEMWE). The model is based on an advanced voltage breakdown analysis that links various overpotentials to PTL morphology. Custom Ti PTLs, spanning uncommonly low porosities (22 - 31%), were fabricated and analyzed with X-ray CT to obtain pore and particle size distributions. Particle size distributions were consistent across samples with an average particle diameter of 12.0?..mu..m, whereas average pore diameters ranged from 6.0 to 7.0?..mu..m. The PTLs were tested in standard PEMWE cell assemblies with anode catalyst loadings of 0.1 mgIr cm-2 to obtain polarization curves, electrochemical impedance spectra, and augmented Tafel analysis. The PTL-dependent anode side losses were deconvoluted and assigned to excess utilization, concentration, ion transport resistance, and electrical contact resistance overpotentials. The data and model reveal an optimal 20 - 28% PTL porosity region where utilization and contact resistance overpotentials are minimized without triggering concentration and ion transport losses related to water deprivation. The optimal PTL porosity depends on the operating current density and is demonstrated at realistic PEMWE water flow rates to establish PTL design guidance for operation at scale.
Due to significant computational expense, discrete element method simulations of jammed packings of size-dispersed spheres with size ratios greater than 1:10 have remained elusive, limiting the correspondence between simulations and real-world granular materials with large size dispersity. Here, invoking a recently developed neighbor binning algorithm, we generate mechanically stable jammed packings of frictionless spheres with power-law size distributions containing up to nearly 4 000 000 particles with size ratios up to 1:100. By systematically varying the width and exponent of the underlying power laws, we analyze the role of particle size distributions on the structure of jammed packings. The densest packings are obtained for size distributions that balance the relative abundance of large-large and small-small particle contacts. Although the proportion of rattler particles and mean coordination number strongly depend on the size distribution, the mean coordination of nonrattler particles attains the frictionless isostatic value of six in all cases. The size distribution of nonrattler particles that participate in the load-bearing network exhibits no dependence on the width of the total particle size distribution beyond a critical particle size for low-magnitude exponent power laws. This signifies that only particles with sizes greater than the critical particle size contribute to the mechanical stability. However, for high-magnitude exponent power laws, all particle sizes participate in the mechanical stability of the packing.
Here, we investigate properties of the particle distribution near the tip of one-dimensional branching random walks at large times t , focusing on unusual realizations in which the rightmost lead particle is very far ahead of its expected position, but still within a distance smaller than the diffusion radius ~$\sqrt{t}$. Our approach consists in a study of the generating function $G_{Δx}(λ) = Σ_n$ ${λ^n}p_n(Δx)$ for the probabilities $p_n(Δx)$ of observing $\textit{n}$ particles in an interval of given size $Δ\textit{x}$ from the lead particle to its left, fixing the position of the latter. This generating function can be expressed with the help of functions solving the Fisher-Kolmogorov-Petrovsky-Piscounov (FKPP) equation with suitable initial conditions. In the infinite-time and large-$Δ\textit{x}$ limits, we find that the mean number of particles in the interval grows exponentially with $Δ\textit{x}$, and that the generating function obeys a nontrivial scaling law, depending on $Δ\textit{x}$ and λ through the combined variable $[Δx — f(λ)]^3 / Δx^2$, where $\textit{f}$(λ) ≡ – ln(1 – λ) – ln [– ln(1 – λ)]. From this property, one may conjecture that the growth of the typical particle number with the size of the interval is slower than exponential, but, surprisingly enough, only by a subleading factor at large Δ$\textit{x}$. The scaling we argue is consistent with results from a numerical integration of the FKPP equation.
We introduce a positive-definite single-particle distribution that is suitable for describing the transition from a macroscopic hydrodynamic to a microscopic kinetic description during the late stages of heavy-ion collisions in the presence of moderately large viscous corrections. The modified equilibrium distribution function can be constructed with hydrodynamic input from either relativistic viscous fluid dynamics or anisotropic fluid dynamics. We test the modified equilibrium distribution's hydrodynamic output for a stationary hadron resonance gas subject to either shear stress, bulk pressure, or baryon diffusion current at a given freeze-out temperature and baryon chemical potential. While it does not reproduce all components of the net baryon current and energy-momentum tensor exactly, it significantly improves upon the customary linearized approximations for the nonequilibrium correction δf n which typically lead to unphysical negative distribution functions at large particle momenta. A comparison of particle spectra and p T –differential elliptic flow coefficients from the Cooper–Frye formula computed with the modified equilibrium distribution and with linearized δf n corrections is presented, for two different (2 + 1)–dimensional hypersurfaces corresponding to central and noncentral Pb + Pb collisions at the Large Hadron Collider (LHC).
Abstract Clays are known for their small particle sizes and complex layer stacking. We show here that the limited dimension of clay particles arises from the lack of long-range order in low-dimensional systems. Because of its weak interlayer interaction, a clay mineral can be treated as two separate low-dimensional systems: a 2D system for individual phyllosilicate layers and a quasi-1D system for layer stacking. The layer stacking or ordering in an interstratified clay can be described by a 1D Ising model while the limited extension of individual phyllosilicate layers can be related to a 2D Berezinskii–Kosterlitz–Thouless transition. This treatment allows for a systematic prediction of clay particle size distributions and layer stacking as controlled by the physical and chemical conditions for mineral growth and transformation. Clay minerals provide a useful model system for studying a transition from a 1D to 3D system in crystal growth and for a nanoscale structural manipulation of a general type of layered materials.
New computational tools for solid-state synthesis recipe design are needed in order to accelerate the experimental realization of novel functional materials proposed by high-throughput materials discovery workflows. This work contributes a cellular automaton simulation framework for predicting the time-dependent evolution of intermediate and product phases during solid-state reactions as a function of precursor choice and amount, reaction atmosphere, and heating profile. The simulation captures the effects of reactant particle spatial distribution, particle melting, and reaction atmosphere. Reaction rates based on rudimentary kinetics are estimated using density functional theory data from the Materials Project and machine learning estimators for the melting point and the vibrational entropy component of the Gibbs free energy. The resulting simulation framework allows for the prediction of the likely outcome of a reaction recipe before any experiments are performed. We analyze five experimental solid-state recipes for BaTiO 3 , CaZrN 2 , and YMnO 3 found in the literature to illustrate the performance of the model in capturing reaction selectivity and reaction pathways as a function of temperature and precursor choice. This simulation framework offers an easier way to optimize existing recipes, aid in the identification of intermediates, and design effective recipes for yet unrealized inorganic solids in silico .
The influence of initial carbide particle distribution features on particle fracture and the evolution of stringer distribution within an alloy of uranium with 10 weight percent molybdenum during cold rolling was investigated in this study. This work will provide guidance to casting optimization work and identify actionable process changes to eliminate the surface features directly attributed to carbides. In a previous study, various synthetic microstructure-based finite-element (FE) models were generated with consideration of different parameters (i.e., particle shape, particle volume fraction, and particle distribution), and used to examine the effects of hot rolling on the microstructure evolution. In this study, microstructures after ~80% hot rolling were used as the initial microstructures for the subsequent cold rolling simulation. Plane-strain compression loading was employed in the FE models to simulate cold rolling with reductions from ~80% to ~94%. Stringer analyses with the consideration of particle fracture were then performed with the simulated cold rolling results. The results of void evolution analyses show that microstructures with elliptical particles incorporate a much larger (almost double) void volume fraction than those with circular particles, indicating that the elliptical particles are fractured more easily than the circular ones. The results from the fracture mode analyses show that, under the adopted simple compression loading assumption, almost all the particles (i.e., >99%) were fractured by tensile separation. The results of stringer analyses show that, during cold rolling, the stringer volume fractions increase substantially due to the particle fracture, especially for the microstructures with the elliptical particles, and that the stringer volume fractions from stringers comprising many particles tend to increase faster. The maximum stringer lengths for the microstructures with circular particles tend to remain constant or decrease during cold rolling, whereas those for elliptical particles tend to slightly increase after a slight decrease. The number of particles at the surface increases very rapidly due to particle fracture during cold rolling.