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At least 289 records · Page 16

Prandtl number effects on extreme mixing events in forced stratified turbulence

Relatively strongly stratified turbulent flows tend to self-organise into a ‘layered anisotropic stratified turbulence’ (LAST) regime, characterised by relatively deep and well-mixed density ‘layers’ separated by relatively thin ‘interfaces’ of enhanced density gradient. Understanding the associated mixing dynamics is a central problem in geophysical fluid dynamics. It is challenging to study LAST mixing, as it is associated with Reynolds numbers $Re := UL/\nu \gg 1$ and Froude numbers $Fr :=(2{\rm \pi} U)/(L N) \ll 1$ ( $U$ and $L$ being characteristic velocity and length scales, $\nu$ the kinematic viscosity and $N$ the buoyancy frequency). Since a sufficiently large dynamic range (largely) unaffected by stratification and viscosity is required, it is also necessary for the buoyancy Reynolds number $Re_{b} := \epsilon /(\nu N^{2}) \gg 1$ , where $\epsilon$ is the (appropriately volume-averaged) turbulent kinetic energy dissipation rate. This requirement is exacerbated for oceanically relevant flows, as the Prandtl number $Pr := \nu /\kappa = {O}(10)$ in thermally stratified water (where $\kappa$ is the thermal diffusivity), thus leading (potentially) to even finer density field structures. We report here on four forced fully resolved direct numerical simulations of stratified turbulence at various Froude ( $Fr=0.5, 2$ ) and Prandtl ( $Pr=1, 7$ ) numbers forced so that $Re_{b}=50$ , with resolutions up to $30\,240 \times 30\,240 \times 3780$ . We find that, as $Pr$ increases, emergent ‘interfaces’ become finer and their contribution to bulk mixing characteristics decreases at the expense of the small-scale density structures populating the well-mixed ‘layers’. However, extreme mixing events (as quantified by significantly elevated local destruction rates of buoyancy variance $\chi _0$ ) are always preferentially found in the (statically stable) interfaces, irrespective of the value of $Pr$ .

Mechanics↗

Using solid debris radiochemistry to measure tungsten mixing in ignition experiments [Slides]

Study to understand how high-Z mix impacts burn and to help inform scaling of mix to EYC.Ride-along on ignition-scale experiments (e.g., HyE). Main goal is to constrain ICF mix simulations against simultaneous radiochemical and x-ray emission measurements of mix. Future experiments may alter design of W-layer to change mix characteristics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Dynamics of plasma atomic layer etching: Molecular dynamics simulations and optical emission spectroscopy

Atomic layer etching is intrinsically dynamic as it involves sequential and repeated exposures of a surface to be etched with different species at different energies. The composition and structure of the near surface region change in both time and depth. Full understanding of this process requires resolving both temporal and spatial variations. In this work, we consider silicon (Si) atomic layer etching (ALE) by alternating exposure to chlorine gas (Cl 2 ) and argon ions (Ar + ). Molecular dynamics (MD) simulations are compared to experimental measurements with the aim of better understanding the dynamics of ALE and to test the simulation procedure. The simulations help to more fully interpret the experimental measurements. Further, optical emission measured just above the surface being etched can be related to etch products and can, therefore, be directly compared to simulation predictions. The simulations capture the measured initial product distribution leaving the surface and match the measured etch per cycle reasonably well. While simulations demonstrate the importance of ion-induced surface damage and mixing into a layer below the surface, the depth of which depends mainly on ion energy, the experiments suggest there is more Cl mixed into the layer than the MD procedure predicts.

74 ATOMIC AND MOLECULAR PHYSICS↗

Rain-Induced Stratification of the Equatorial Indian Ocean and Its Potential Feedback to the Atmosphere

Surface freshening through precipitation can act to stably stratify the upper ocean, forming a rain layer (RL). RLs inhibit subsurface vertical mixing, isolating deeper ocean layers from the atmosphere. This process has been studied using observations and idealized simulations. The present ocean modeling study builds upon this body of work by incorporating spatially resolved and realistic atmospheric forcing. Fine-scale observations of the upper ocean collected during the Dynamics of the Madden-Julian Oscillation field campaign are used to verify the General Ocean Turbulence Model (GOTM). Spatiotemporal characteristics of equatorial Indian Ocean RLs are then investigated by forcing a 2D array of GOTM columns with realistic and well-resolved output from an existing regional atmospheric simulation. RL influence on the ocean-atmosphere system is evaluated through analysis of RL-induced modification to surface fluxes and sea surface temperature (SST). This analysis demonstrates that RLs cool the ocean surface on time scales longer than the associated precipitation event. A second simulation with identical atmospheric forcing to that in the first, but with rainfall set to zero, is performed to investigate the role of rain temperature and salinity stratification in maintaining cold SST anomalies within RLs. Approximately one third, or 0.1°C, of the SST reduction within RLs can be attributed to rain effects, while the remainder is attributed to changes in atmospheric temperature and humidity. The prolonged RL-induced SST anomalies enhance SST gradients that have been shown to favor the initiation of atmospheric convection. These findings encourage continued research of RL feedbacks to the atmosphere.

54 ENVIRONMENTAL SCIENCES↗

Preparation and characterization of isotopically pure Mo targets for nuclear science measurements

Isotopically pure molybdenum targets are essential in various nuclear science measurements. For studies of cross sections of capture reactions on molybdenum, uniform targets with areal densities of hundreds of g/cm 2 are desired. Mechanical rolling of enriched metal pieces or vacuum sputtering methods used in previous studies to prepare molybdenum targets are challenging and involve labor- and time-intensive processes. Therefore, reliable and straightforward methods to produce molybdenum targets are crucial. We have developed a new double-step method to produce targets meeting these needs. The first step consists of evaporating isotopically enriched MoO 3 onto gold backings. The second step involves the reduction of the oxide layer in a 5% H 2 -Ar environment to obtain molybdenum targets. X-ray fluorescence (XRF) spectroscopy, X-ray Diffraction (XRD), a scanning electron microscope/focused ion beam milling, and energy-dispersive X-ray spectroscopy (EDS) were used to characterize the targets. These methods show that the targets exhibit a uniform coverage of Mo over the gold backings. Furthermore, significant volume shrinkage occurring during the reduction of MoO 3 creates a porous Mo layer where the gold diffuses due to the high processing temperatures, resulting in mixed Mo–Au layers.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Idealized Large-Eddy Simulations of Stratocumulus Advecting over Cold Water. Part I: Boundary Layer Decoupling

Abstract We explore the decoupling physics of a stratocumulus-topped boundary layer (STBL) moving over cooler water, a situation mimicking warm-air advection (WADV). We simulate an initially well-mixed STBL over a doubly periodic domain with the sea surface temperature decreasing linearly over time using the System for Atmospheric Modeling large-eddy model. Due to the surface cooling, the STBL becomes increasingly stably stratified, manifested as a near-surface temperature inversion topped by a well-mixed cloud-containing layer. Unlike the stably stratified STBL in cold-air advection (CADV) that is characterized by cumulus coupling, the stratocumulus deck in the WADV is unambiguously decoupled from the sea surface, manifested as weakly negative buoyancy flux throughout the subcloud layer. Without the influxes of buoyancy from the surface, the convective circulation in the well-mixed cloud-containing layer is driven by cloud-top radiative cooling. In such a regime, the downdrafts propel the circulation, in contrast to that in CADV regime for which the cumulus updrafts play a more determinant role. Such a contrast in convection regime explains the difference in many aspects of the STBLs including the entrainment rate, cloud homogeneity, vertical exchanges of heat and moisture, and lifetime of the stratocumulus deck, with the last being subject to a more thorough investigation in Part II. Finally, we investigate under what conditions a secondary stratus near the surface (or fog) can form in the WADV. We found that weaker subsidence favors the formation of fog whereas a more rapid surface cooling rate does not. Significant Statement The low-lying blanketlike clouds, called stratocumulus (Sc), reflect much incoming sunlight, substantially modulating Earth’s temperature. While much is known about how the Sc evolves when it moves over warmer water, few studies examine the opposite situation of Sc moving over colder water. We used a high-resolution numerical model to simulate such a case. When moving over cold water, the Sc becomes unambiguously decoupled from the water surface, distinctive from its warm counterpart in which the Sc interacts with the water surface via intermittent cauliflower-like clouds called cumulus clouds. Such decoupling influences many aspects of the Sc–sea surface system, which combine to alter the ability of the Sc to reflect sunlight, thereby influencing the climate. This work laid the foundation for future work that quantifies the contribution of such a decoupled Sc regime to Earth’s radiative budget and climate change.

54 ENVIRONMENTAL SCIENCES↗

Freestream turbulence effects on unsteady wind turbine loads and wakes: An IDDES study

We investigate numerically the effects of freestream turbulence on the unsteady aerodynamics and wakes of the National Renewable Energy Laboratory Phase VI wind turbine rotor for increasing wind speed. Turbulence is modeled using the Improved Delayed Detached-Eddy Simulation (IDDES) method. As a first step, a detailed mesh resolution study is conducted with the decaying freestream turbulence model at turbulence intensity of 0.5%. Our blade-resolved IDDES simulations show that grid-independent average torque and thrust results can be achieved with relatively coarse meshes, whereas dramatically higher mesh resolution is required for grid-independent results for power spectral densities of thrust force, especially in the deep-stall regime. Comparing the loads with the Shear-Stress Transport model demonstrates the superiority of IDDES in predicting massively separated flows. The aerodynamic performance and wake predictions with the decaying freestream turbulence model are compared with the synthetic freestream turbulence model. Both models predict nearly the same loads, spectral energy content, and wake characteristics. The properties of both the near- and far-wake regions are then examined. Furthermore, we show that separated boundary layers accelerate turbulent mixing and entrainment of the external flow, which results in faster wake recovery. The effect of increasing turbulence intensity to 6% is investigated using the synthetic freestream turbulence model. In contrast with the fully attached boundary layer, higher freestream turbulence in deep stall does not significantly affect the loads and vortex-shedding characteristics. However, the turbulent mixing in the wake is enhanced, which further hastens the recovery of the self-similar velocity profile. In general, increasing the wind speed at high turbulence intensity shifts the recovery farther upstream and increases the wake width.

17 WIND ENERGY↗

Convective shells in the interior of Cepheid variable stars: Overshooting models based on hydrodynamic simulations

Context. Because Cepheid variable stars have long been used as a cosmic benchmark for scaling distances in our Galaxy and beyond, the accuracy of stellar evolution models for Cepheids have wide-reaching effects. However, our understanding of the dynamics in the interiors of these physically complex stars is limited. Aims. Our goal is to provide a detailed multi-dimensional picture of hydrodynamic convection and convective boundary mixing in the interior of Cepheids. Methods. Using the Modules for Experiments in Stellar Astrophysics (MESA), we studied the structure of intermediate-mass stars that cross the instability strip. Then, we performed two-dimensional hydrodynamic simulations of six stars with the fully compressible Multidimensional Stellar Implicit Code (MUSIC). Our simulations did not model the radial pulsations but focused on the interior structure of this family of stars. We developed and applied a new statistical analysis to examine convection and convective boundary mixing in the interior of these stellar simulations. Results. Based on a grid of MESA models, we demonstrated that a common structure for intermediate mass Cepheids includes an interior convective shell as well as a thin outer convective envelope. Using the extreme value theory approach to analyze our MUSIC simulation data, we found that overshooting above the convective shell fills the space between these convectively unstable layers. We developed a new statistical analysis that provides a clearer picture of how overshooting fills this layer; it also allowed us to formulate a detailed comparison between overshooting above and below the convective shell. Our analysis effectively decomposes the overshooting layer into two layers: a weak overshooting layer and a strong overshooting layer. Statistically, this is accomplished by decomposing the strongly non-Gaussian probability density function into a mixture of gamma distributions. Using our mixture model, we showed that the ratio of overshooting lengths above and below the convective shell depends directly on the radial extent of the convective shell as well as its depth in the star. We proposed a new form for the diffusion coefficient that addresses the need for overlapping overshooting layers between convective shells. We introduced the idea of a “super-mixing layer” where overshooting from both the convective shell and the convective envelope results in efficient mixing and could be viewed as merging the two adjacent convective zones.

79 ASTRONOMY AND ASTROPHYSICS↗

Mixed Tin-Titanium Oxides by Atomic Layer Deposition on Planar Substrates: Physical and Electronic Structure

Ternary atomic layer deposition of Sn-doped TiO x (Sn:TiO x ) and Ti-doped SnO x (Ti:SnO x ) was performed using tetrakisdimethylamidotitanium (IV) and tin(IV) with water at 150 °C on (1 0 0) Si and quartz substrates. The physical structure of the films was investigated using scanning electron, atomic force, and Kelvin probe force microscopies as well as spectroscopic ellipsometry, Raman spectroscopy, and X-ray diffraction. All as-deposited films are amorphous and possessed flat and conformal topographies with low surface roughness (<1 nm). Annealed Sn:TiO x and Ti:SnO x crystallize into the tetragonal anatase TiO 2 and cassiterite SnO 2 structures, respectively, without large variations to the film topography. The chemical composition of the as-deposited and annealed films was investigated through X-ray photoelectron spectroscopy. While dopants are homogenously mixed, the ternary ALD to form Sn:TiO x and Ti:SnO x surprisingly does not follow the rule of mixtures, despite similarities in both the growth rates of binary SnO x and TiO x and the precursors used. This finding is also supported by spectroscopic ellipsometry. Here, we postulate the deviation from the rule of mixtures is due to non-ideal surface chemistry of the binary ALD of SnO x . The optical bandgap of all films was quantified by the Tauc analysis and the valence band position was investigated by valence band X-ray photoelectron spectroscopy. Intra-bandgap states above the valence band maximum were observed for as-deposited Ti:SnO x and Sn:TiO x and ascribed to 5 s states from Sn 2+ ions. The presence of these intra-bandgap states induces enhanced visible absorption and bathochromic shifts to the apparent bandgap for all as-deposited films. Annealing the films removes the intra-bandgap states and increases the optical bandgap. Simplified band diagrams created using the data available demonstrated that the conduction and valence band positions did not vary between the positions of pure TiO 2 or SnO 2 with monotonic increases to the dopant incorporation.

36 MATERIALS SCIENCE↗

Structure–Property Relationships of Recycled Lithium-Ion Battery Cathodes: Microstructure Optimization Using Virtual Materials Testing

The increasing demand for sustainable battery technologies requires effective recycling strategies for end-of-life lithium-ion battery cathodes. In this study, virtual materials testing, a well-established framework for modeling conventionally manufactured NMC-based cathodes, is applied to partially recycled cathodes. To this end, virtual cathodes consisting of mixtures of pristine and recycled NMC particles are utilized to systematically analyze structure–property relationships depending on mixing ratios and different spatial arrangement strategies. For this purpose, a stochastic 3D model is developed that is capable of generating virtual cathodes with arbitrary volume fractions of active materials and mixing ratios of pristine and recycled NMC particles. Particularly, the stochastic 3D model can mimic the different size distributions of pristine and recycled particles that are observed in image data. Additionally, the model allows the structuring of pristine and recycled NMC either uniformly mixed or layer-wise arranged, mimicking single- and dual-layer cathodes. Subsequently, a systematic computational analysis is conducted to assess the influence of increasing active material ratios of recycled particles, ranging from 0 % to 100 %, while maintaining a constant overall active material volume fraction. The impact of particle mixing on cathode performance is evaluated by examining transport-relevant geometrical descriptors and effective properties, such as geodesic tortuosity, specific surface area, and tortuosity factor.

25 ENERGY STORAGE↗

First large capsule implosions in a frustum-shaped hohlraum

Here, we report on the first indirect-drive implosions driven by a dual conical frustum-shaped hohlraum denoted “frustraum” and the experimental tuning campaigns leading up to two layered implosions. The campaign used 1.2 and 1.4 mm inner radius high density carbon (HDC) capsules and represented the largest HDC capsules to be imploded on the National Ignition Facility via indirect drive. Several techniques were successfully implemented to control the Legendre mode 2 capsule symmetry of the implosions, including changing the wall angle of the frustraum, which is not possible with cylindrical hohlraums. A mode 4 feature was observed and its implications for hotspot mix discussed. Two layered implosions were conducted with 1.2 mm inner radius capsules, the latter of which achieved the highest layered capsule absorbed energy on the National Ignition Facility using only 1.74 MJ of laser energy. The layered implosion results, along with generalized Lawson parameters, suggest that increasing the energy absorbed by the capsule at the expense of long coast times makes it more challenging to achieve ignition and that further reducing coast time (time between end of laser pulse and bang time) closer to the 1 ns level is warranted to improve the areal density and make it easier to achieve the hotspot temperature, alpha heating, and yield amplification required for ignition.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Near-surface damage and mixing in Si-Cl 2 -Ar atomic layer etching processes: Insights from molecular dynamics simulations

Silicon-chlorine-argon (Si-Cl 2 -Ar) atomic layer etching (ALE) is simulated using classical molecular dynamics (MD). The simulations provide a detailed view into the near-surface region during ALE processing. Bombardment of Ar + ions creates a mixed amorphous region that significantly differs from the picture of ideal ALE. There is also a significant change in the Si etch yield and the etch product distribution as a function of Ar + ion fluence. The Si etch yield is the highest at the beginning of the bombardment step but eventually decays to the physical sputtering yield. Atomic Cl and silicon chlorides are major etch products at the start of an ion bombardment step, but quickly decay. Atomic Si yields remain relatively constant as a function of Ar + ion fluence. As a result, a new schematic of Si-Cl 2 -Ar ALE is presented in order to emphasize the complex behavior observed in MD simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fluid inertia controls mineral precipitation and clogging in pore to network-scale flows

Mineral precipitation caused by fluid mixing presents complex control and predictability challenges in a variety of natural and engineering processes, including carbon mineralization, geothermal energy, and microfluidics. Precipitation dynamics, particularly under the influence of fluid flow, remain poorly understood. Combining microfluidic experiments and three-dimensional reactive transport simulations, we demonstrate that fluid inertia controls mineral precipitation and clogging at flow intersections, even in laminar flows. We observe distinct precipitation regimes as a function of Reynolds number (Re). At low Reynolds numbers (Re < 10), precipitates form a thin, dense layer along the mixing interface, which shuts precipitation off, while at high Reynolds numbers (Re > 50), strong three-dimensional flows significantly enhance precipitation over the entire intersection, resulting in rapid clogging. When injection rates from two inlets are uneven, flow symmetry-breaking leads to unexpected flow bifurcation phenomena, which result in enhanced concurrent precipitation in both downstream channels. Finally, we extend our findings to rough channel networks and demonstrate that the identified inertial effects on precipitation at the intersection scale are also present and even more dramatic at the network scale. This study sheds light on the fundamental mechanisms underlying mixing-induced mineral precipitation and provides a framework for designing and optimizing processes involving mineral precipitation.

Science & Technology - Other Topics↗

Unravelling the Nature of the Intrinsic Complex Structure of Binary‐Phase Na‐Layered Oxides

Abstract The layered sodium transition metal oxide, NaTMO 2 (TM = transition metal), with a binary or ternary phases has displayed outstanding electrochemical performance as a new class of strategy cathode materials for sodium‐ion batteries (SIBs). Herein, an in‐depth phase analysis of developed Na 1− x TMO 2 cathode materials, Na 0.76 Ni 0.20 Fe 0.40 Mn 0.40 O 2 with P2‐ and O3‐type phases (NFMO‐P2/O3) is offered. Structural visualization on an atomic scale is also provided and the following findings are unveiled: i) the existence of a mixed‐phase intergrowth layer distribution and unequal distribution of P2 and O3 phases along two different crystal plane indices and ii) a complete reversible charge/discharge process for the initial two cycles that displays a simple phase transformation, which is unprecedented. Moreover, first‐principles calculations support the evidence of the formation of a binary NFMO‐P2/O3 compound, over the proposed hypothetical monophasic structures (O3, P3, O′3, and P2 phases). As a result, the synergetic effect of the simultaneous existence of P‐ and O‐type phases with their unique structures allows an extraordinary level of capacity retention in a wide range of voltage (1.5–4.5 V). It is believed that the insightful understanding of the proposed materials can introduce new perspectives for the development of high‐voltage cathode materials for SIBs.

Paidi, Anil K.↗

Role of mixed conducting Pr 0.1 Gd 0.1 Ce 0.8 O 1.9-δ barrier layer on the promotion of SOFC performance

The cathode activity in a solid oxide fuel cell can be promoted by introducing various catalysts to reduce its polarization resistance towards oxygen reduction, and thus improve cell performance. Here, in this work, the La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3 (LSCF) cathode surface is modified by the infiltration of Pr 6 O 11 and the power density at 0.8 V and 750 °C is improved by 21%. Moreover, by replacing the traditional barrier layer Gd 0.2 Ce 0.8 O 1.9 with mixed conducting Pr 0.1 Gd 0.1 Ce 0.8 O 1.9 (PGCO), the power density increases by 38%. The ohmic resistance is dramatically reduced by applying the PGCO interlayer. The distribution of relaxation time was used to analyze the mechanism for which the polarization resistance was decreased, attributing to the mixed conduction nature in PrO x . An increase of power density, ~0.358 W/cm 2 (71%) at 0.8 V, is achieved with the implementation of both surface modification and buffer layer engineering.

08 HYDROGEN↗

Intrinsic Li Distribution in Layered Transition-Metal Oxides Using Low-Dose Scanning Transmission Electron Microscopy and Spectroscopy

Understanding Li distribution in layered lithium transition-metal oxide (LiTMO) cathodes in Li-ion batteries has been a major challenge at the atomic scale and nanoscale. Li is extremely difficult to study by transmission electron microscopy (TEM) because the high-energy electrons impart significant energy and cause massive migration. Here, we directly map the intrinsic spatial distribution and bonding of Li in LiNiO 2 -layered cathode materials using low-dose and low-loss electron energy loss spectroscopy (EELS). EELS spectra of the Li–K edge are measured simultaneously with O–K and Ni–L, M 3,2 edges from layered, cation-mixed, and rock-salt phases and directly matched with atomic-resolution scanning TEM images to correlate the changes in peak intensities and positions to the stoichiometry changes with continual loss of Li and O. Changes in the Li content in the LiNiO 2 particles as a function of electron beam dose are studied by sequential Li spectroscopic mapping. We show that the “intrinsic” Li distribution can be observed using a total dose of less than ~1.5 × 10 8 e – nm –2 at an accelerating voltage of 80 kV. The method of nanoscale mapping of Li distribution introduced in this study is applicable to high-Ni LiTMO cathode materials (>89% of Ni) as well as LiNiO 2 . Further study on the extra peaks of the Li–K edge reveals that the peak at ~59 eV is from the Li ions intercalated in between NiO 2 layers barely interacting with each other with less Li K shell electrons pulled to the L shell electrons in NiO 2 . Furthermore, the results shown here provide improved low-loss TEM characterization approaches that can be used to understand the intrinsic fundamental behaviors in Li-ion batteries.

25 ENERGY STORAGE↗