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At least 667 records · Page 37

Coupling Processes between Atmospheric Chemistry and Climate

This is the fourth semi-annual report for NAS5-97039, covering the time period July through December 1998. The overall objective of this project is to improve the understanding of coupling processes between atmospheric chemistry and climate. Model predictions of the future distributions of trace gases in the atmosphere constitute an important component of the input necessary for quantitative assessments of global change. We will concentrate on the changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The key modeling tools for this work are the Atmospheric and Environmental Research (AER) two-dimensional chemistry-transport model, the AER two-dimensional stratospheric sulfate model, and the AER three-wave interactive model with full chemistry. For this six month period, we report on a modeling study of new rate constant which modify the NOx/NOy ratio in the lower stratosphere; sensitivity to changes in stratospheric water vapor in the future atmosphere; a study of N2O and CH4 observations which has allowed us to adjust diffusion in the 2-D CTM in order to obtain appropriate polar vortex isolation; a study of SF6 and age of air with comparisons of models and measurements; and a report on the Models and Measurements II effort.

Ko, Malcolm K. W.↗

Predicted aircraft effects on stratospheric ozone

The possibility that the current fleet of subsonic aircraft may already have caused detectable changes in both the troposphere and stratosphere has raised concerns about the impact of such operations on stratospheric ozone and climate. Recent interest in the operation of supersonic aircraft in the lower stratosphere has heightened such concerns. Previous assessments of impacts from proposed supersonic aircraft were based mostly on one-dimensional model results although a limited number of multidimensional models were used. In the past 15 years, our understanding of the processes that control the atmospheric concentrations of trace gases has changed dramatically. This better understanding was achieved through accumulation of kinetic data and field observations as well as development of new models. It would be beneficial to start examining the impact of subsonic aircraft to identify opportunities to study and validate the mechanisms that were proposed to explain the ozone responses. The two major concerns are the potential for a decrease in the column abundance of ozone leading to an increase in ultraviolet radiation at the ground, and redistribution of ozone in the lower stratosphere and upper troposphere leading to changes in the Earth's climate. Two-dimensional models were used extensively for ozone assessment studies, with a focus on responses to chlorine perturbations. There are problems specific to the aircraft issues that are not adequately addressed by the current models. This chapter reviews the current status of the research on aircraft impact on ozone with emphasis on immediate model improvements necessary for extending our understanding. The discussion will be limited to current and projected commercial aircraft that are equipped with air-breathing engines using conventional jet fuel. The impacts are discussed in terms of the anticipated fuel use at cruise altitude.

Ko, Malcolm K. W.↗

Nanoscale mapping of point defect concentrations with $\mathrm{4D-STEM}$

Vacancies are missing atoms in a crystalline material, and occur both at equilibrium (varying with temperature) and out of equilibrium such as when crystalline materials are damaged with radiation or corrosion. While we know of their importance, particularly regarding diffusive mechanisms, it is not straightforward to experimentally measure their concentration or to visualize them directly. Traditionally, measurements such as positron annihilation spectroscopy and to some degree X-ray diffraction can measure average concentrations, but generally lack the ability to visualize or quantify a heterogenous concentration of vacancies that can occur at the level of individual defects and microstructural features. Here, we present a method to map vacancy concentrations and their distribution using local lattice parameter measurements with a high-resolution electron microscope. Our method utilizes a Au thin film as a model to demonstrate the method via four-dimensional scanning transmission electron microscopy (4D-STEM) by correlating the differences between changes in lattice parameter and the volumetric thermal expansion during in situ heating experiments. The vacancy mapping methodology is also applied to non-equilibrium defects accumulated in pure Al via knock-on electron beam irradiation. Our method demonstrates the ability to map point defect concentrations in heterogeneous systems in situ with nanometer spatial resolution. The result is a technique that can provide direct measurements of vacancy concentrations at the level of individual defects in studies of materials in and out of equilibrium.

36 MATERIALS SCIENCE↗

Four-dimensional symmetry from a broad viewpoint. II Invariant distribution of quantized field oscillators and questions on infinities

The foundation of the quantum field theory is changed by introducing a new universal probability principle into field operators: one single inherent and invariant probability distribution P(/k/) is postulated for boson and fermion field oscillators. This can be accomplished only when one treats the four-dimensional symmetry from a broad viewpoint. Special relativity is too restrictive to allow such a universal probability principle. A radical length, R, appears in physics through the probability distribution P(/k/). The force between two point particles vanishes when their relative distance tends to zero. This appears to be a general property for all forces and resembles the property of asymptotic freedom. The usual infinities in vacuum fluctuations and in local interactions, however complicated they may be, are all removed from quantum field theories. In appendix A a simple finite and unitary theory of unified electroweak interactions is discussed without assuming Higgs scalar bosons.

Hsu, J. P.↗

Wave generation in a sunspot

In this paper we analyze the generation of waves in a sunspot by extending Stein's hydrodynamic approach to the turbulent medium permeated by a strong uniform magnetic field oriented parallel to the gravity. For wave sources appropriate to the sunspot, we consider magnetic perturbations and entropy changes as well as turbulent convection. To describe the anisotropy imposed by the sunspot, we use a one-dimensional correlation function relating the turbulent eddies separated along the symmetry axis of the spot. This treatment yields several interesting possibilities for wave generation in a sunspot. First, it is demonstrated that the entropy change and magnetic perturbation can lead to a relative enhancement of acoustic wave emission. Second, the energy flux of Alfven waves may be comparable to that of acoustic waves in sunspots. Third, the anisotropy of the sunspot dynamics can lead to wave energy spectrum in a form which may explain the origin of umbral atmospheric oscillations.

Lee, Jeongwoo W.↗

Collaborative Project: Three-Dimensional Structure of the Southern Ocean Overturning Circulation

The large-scale upwelling in the Southern Ocean provides a pathway for the deep and abyssal water masses of the global ocean to return to the surface, creating a mechanism for the exchange of carbon and heat between the deep ocean water masses and the atmosphere. Despite the significance of the overturning circulation in the Southern Ocean for global climate, very little is known about the depth and longitudinal distribution of the overturning pathways and their influence on heat uptake, regional sea level change and ocean carbon transport. The focus of this grant was to assess the three-dimensional structure of the Southern Ocean overturning circulation in models and observations, with the following three objectives: 1. Quantify and contrast modeled (using GFDL and CESM models) and observed (Argo based) upwelling pathways in the Southern Ocean. 2. Evaluate the impact of model resolution on transport pathways and the associated meridional fluxes of heat and salt. 3. Determine the influence of climate-driven changes in upwelling on the regional patterns and magnitude of heat and carbon uptake and sea level change. We have successfully achieved our three objectives through (1) running Southern Ocean particle tracking simulations in global coupled models with varying resolutions, and (2) quantifying the role played by the overturning circulation and its changes to the surface heat and carbon uptake, in climate models as well as observations. The research funded under this grant led to 8 published papers and 2 submitted papers, with 2 additional papers in preparation.

59 BASIC BIOLOGICAL SCIENCES↗

A one-dimensional unsteady model of dual mode scramjet operation

A one-dimensional unsteady model and code have been developed which can handle internal flows involving area change, heat release, transients and coupled inviscid core-boundary layer flows. The model has been shown to work well in diverging channels with a supersonic entrance Mach number and unseparated boundary layers. Transient flows have also been studied. The model needs no prior knowledge of shock (or shocks) location and can be extended to two or three dimensions. The results show that the one-dimensional unsteady model developed here can be used for analysis of internal flows as occur in scramjet combustors.

Bussing, T. R. A.↗

Effect of ice-albedo feedback on global sensitivity in a one-dimensional radiative-convective climate model

The feedback between the ice albedo and temperature is included in a one-dimensional radiative-convective climate model. The effect of this feedback on global sensitivity to changes in solar constant is studied for the current climate conditions. This ice-albedo feedback amplifies global sensitivity by 26 and 39%, respectively, for assumptions of fixed cloud altitude and fixed cloud temperature. The global sensitivity is not affected significantly if the latitudinal variations of mean solar zenith angle and cloud cover are included in the global model. The differences in global sensitivity between one-dimensional radiative-convective models and energy balance models are examined. It is shown that the models are in close agreement when the same feedback mechanisms are included. The one-dimensional radiative-convective model with ice-albedo feedback included is used to compute the equilibrium ice line as a function of solar constant.

Wang, W.-C.↗

Three-dimensional lattice modulations in the charge density wave system Lu 2 Ir 3 Si 5

Using total and resonant x-ray scattering coupled to large-scale computer modeling, we study the lattice modulations in the complex charge density wave (CDW) material Lu 2 ⁢Ir 3 ⁢Si 5 . Here, we find that it is a unique quantum system where periodic lattice modulations related to emergent CDW order occur in three orthogonal atomic planes of the crystal lattice, leading to the emergence of an unusual three-dimensional (3D) pattern of short and long Ir-Ir and Lu-Lu bonds. The 3D character of observed lattice modulations explains the largely isotropic character of the changes in the electronic properties occurring when the CDW order sets in, demonstrating the strong electron-lattice coupling in Lu 2 ⁢Ir 3 ⁢Si 5 . The result is supported by DFT calculations based on the experimental structure data. Altogether, our work provides strong evidence for the presence of a relationship between the dimensionality of emergent lattice distortions and that of concurrent changes in the electronic properties of CDW materials. The relationship may need to be accounted for when these materials are explored for practical applications.

36 MATERIALS SCIENCE↗

An experimental and theoretical evaluation of increased thermal diffusivity phase change devices

This study was to experimentally evaluate and mathematically model the performance of phase change thermal control devices containing high thermal conductivity metal matrices. Three aluminum honeycomb filters were evaluated at five different heat flux levels using n-oct-adecane as the test material. The system was mathematically modeled by approximating the partial differential equations with a three-dimensional implicit alternating direction technique. The mathematical model predicts the system quite well. All of the phase change times are predicted. The heating of solid phase is predicted exactly while there is some variation between theoretical and experimental results in the liquid phase. This variation in the liquid phase could be accounted for by the fact that there are some heat losses in the cell and there could be some convection in the experimental system.

White, S. P.↗

Microfluidic Investigation of Salinity-Induced Oil Recovery in Porous Media during Chemical Flooding

High and low salinity water flooding are common oil recovery processes performed in the oil fields for extracting crude oil from the reservoir. These processes are often performed sequentially, naturally establishing non-uniform salinity in the porous subsurface. In this article, we investigate oil transport in porous media induced by salinity change upon flooding with high and low salinity water. As we observe a large number of impervious dead-ends from three-dimensional imaging of the actual reservoir, we identify that these areas play an important role in oil recovery where the oil transport is governed by the salinity change rather than hydrodynamics. The salinity gradients induced upon high salinity water flooding provide pathways to enhance the transport of oil drops trapped in the dead-end regions via non-equilibrium effects. However, above a critical salinity, we observe a rapid aggregation of drops that lead to the complete blockage of the pore space, thereby inhibiting oil recovery. We also find that, at an intermediate salinity where the drop aggregation is modest, the aggregation rather promotes the oil recovery. Furthermore, our observations suggest that there exist optimal salinity conditions for maximizing oil recovery during chemical flooding.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Shapiro steps and stability of skyrmions interacting with alternating anisotropy under the influence of ac and dc drives

Here we use atomistic simulations to examine the sliding dynamics of a skyrmion in a two-dimensional system containing a periodic one-dimensional stripe pattern of variations between low and high values of the perpendicular magnetic anisotropy. The skyrmion changes in size as it crosses the interface between two anisotropy regions. On applying combined dc and ac driving in either parallel or perpendicular directions, we observe a wide variety of Shapiro steps, Shapiro spikes, and phase-locking phenomena. The phase-locked orbits have two-dimensional dynamics due to the gyrotropic or Magnus dynamics of the skyrmions and are distinct from the phase-locked orbits found for strictly overdamped systems. Along a given Shapiro step when the ac drive is perpendicular to the dc drive, the velocity parallel to the ac drive is locked while the velocity in the perpendicular direction increases with increasing drive to form Shapiro spikes. At the transition between adjacent Shapiro steps, the parallel velocity jumps up to the next step value, and the perpendicular velocity drops. The skyrmion Hall angle shows a series of spikes as a function of increasing dc drive, where the jumps correspond to the transition between different phase-locked steps. At high drives, the Shapiro steps and Shapiro spikes are lost. When both the ac and dc drives are parallel to the stripe periodicity direction, Shapiro steps appear, while if the dc drive is parallel to the stripe periodicity direction and the ac drive is perpendicular to the stripe periodicity, then there are only two locked phases, and the skyrmion motion consists of a combination of sliding along the interfaces between the two anisotropy values and jumping across the interfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Application of Principal Component Analysis for the Monitoring of the Aging Process of Nuclear Electrical Cable Insulation

To ensure the safe operation of nuclear power plants (NPPs), it is critical to understand how NPP electrical cable insulation will degrade under different service environments. In this study, various nondestructive examination methods were selected to evaluate degradation of electrical cable insulation after aging. Elongation at break, indenter modulus, relaxation constant, mass change, total color difference, and carbonyl index were collected stepwise on cross-linked polyethylene (XLPE) cable insulations after predetermined exposure intervals. Three different insulation aging scenarios were investigated: 1) simultaneous irradiation and heating at 150°C, 2) heating at 150°C followed by corresponding times of irradiation at ambient temperature, and 3) irradiation at ambient temperature followed by heating at 150°C for the same duration. A constant dose rate of 300 Gy/hr was selected with a total gamma irradiation absorbed dose up to 320 kGy. To gain insight into the long-term performance of NPP electrical cable insulation, principal component analysis (PCA), a data-driven approach, was utilized to identify key indicators of cable insulation degradation. By reducing the dimensionality of the data while retaining degradation information, PCA was used to highlight the changes in the measured properties under gamma irradiation according to total absorbed dose and the different aging scenarios.

Li, Donghui↗

Simultaneous conjugate observations of dynamic variations in high-latitude dayside convection due to changes in IMF By

Data from two conjugate HF radars currently operating at Goose Bay (Labrador) and the Halley Station (Antarctica), obtained for a single 45-min period about local noon on April 22, 1988, were used to study the near-instantaneous conjugate two-dimensional patterns of plasma convection in the vicinity of the cusp. In particular, the response of these plasma convection patterns to changes in the By component of the IMF was examined. Results indicate that, under quasi-stationary IMF conditions, the conjugate convection patterns are quite similar to the synthesized patterns of Heppner and Maynard (1987) and that the patterns respond rapidly to changes in the IMF By component. Results also show that transitions between convection states begin to occur within minutes of the time that an IMF state change is incident on the magnetospheric boundary, and that the convection reconfigurations expand poleward, completely filling the field of view of an HF radar within 6 min of the time of onset.

Greenwald, R. A.↗

Operando Nanoscale Imaging of Electrochemically Induced Strain in a Locally Polarized Pt Grain

Developing new methods that reveal the structure of electrode materials under polarization is key to constructing robust structure-property relationships. However, many existing methods lack the spatial resolution in structural changes and fidelity to electrochemical operating conditions that are needed to probe catalytically relevant structures. Here, we combine a nanopipette electrochemical cell with three-dimensional X-ray Bragg coherent diffractive imaging to study how strain in a single Pt grain evolves in response to applied potential. During polarization, marked changes in surface strain arise from the Coulombic attraction between the surface charge on the electrode and the electrolyte ions in the electrochemical double layers, while the strain in the bulk of the crystal remains unchanged. The concurrent surface redox reactions have a strong influence on the magnitude and nature of the strain changes under polarization. In conclusion, our studies provide a powerful blueprint to understand how structural evolution influences electrochemical performance at the nanoscale.

36 MATERIALS SCIENCE↗

Understanding Biomass and Polymer Feedstock Variability Through Analytical Pyrolysis and Two Dimensional Gas Chromatography and Mass Spectrometry

Moving toward a circular carbon economy requires enabling reuse of carbon-based macromolecules like those in biomass and polymers. Meeting this goal requires increased upcycling of waste products into higher value products. For biomass waste such as corn stover, pine needles, or bark, one approach is using pyrolysis to convert these feedstocks into bio-oil that can be used for liquid fuel or transformed into other hydrocarbon based products, like bio-polymers. Waste plastics can be upcycled or recycled into new products, or alternatively converted into bio-oil by pyrolysis. Macromolecules from biomass and polymers are challenging to convert into liquid fuel or chemical feedstocks, due to large and sometimes heterogeneous networks of polymeric bonds. We work with the Idaho National Laboratory’s Biomass Feedstock National User Facility and Department of Energy’s Feedstock Conversion Interface Consortium to develop a molecular understanding of biomass variability that occurs naturally and as a result of storage or preprocessing techniques applied to feedstocks, to understand chemical reactions occurring during pyrolysis and other biomass or polymer conversion techniques. Using two dimensional gas chromatography mass spectrometry coupled to analytical pyrolysis provides insight into the molecular changes that occur during the pyrolysis event, and these insights can extend to bench or pilot scale pyrolysis conversions. Understanding pyrolysis of biomass and polymers at a molecular level contributes to development of new tools to predict and manipulate the optimum conditions and identify the best storage, preprocessing, and conversion techniques to maximize output of specific high-value chemical species in the conversion to fuels, or to characterize feedstocks for blending before pyrolysis. Identification and understanding of the molecular level changes resulting from novel preprocessing techniques that can be used to control and manipulate the chemical output of bench or pilot scale pyrolysis is another focus of investigation, including the use of gamma irradiation, acid, or enzyme pre-treatments. We also focus on the impacts of storage conditions and techniques, which can affect moisture levels, degradation, and impacts from naturally occurring microbes in the environment.

09 BIOMASS FUELS↗

From 2D to 4D: a containerized workflow and browser to explore dynamic chromatin architecture

Background Characterizing the physical organization of the genome is essential for understanding long-range gene regulation, chromatin compartmentalization, and epigenetic accessibility. Hi-C experiments generate two-dimensional (2D) genome-wide contact maps of chromatin interactions by capturing the spatial proximity between genomic loci, which reveal interaction frequencies but lack the spatial resolution needed to interpret the three-dimensional (3D) genome structure(s). Emerging evidence suggests that epigenetic regulation is closely linked to 3D genome architecture, and that structural changes over time (4D) drive key biological processes in development, disease, and environmental response. Thus, integrating 3D structure with functional data is critical for a more complete understanding of genome regulation. Previous work, most notably the 4DHiC chromosome modeling framework, has shown that physical multi-dimensional modeling approaches rooted in polymer physics and molecular dynamics can resolve these structures at biologically meaningful resolutions by integrating temporal Hi-C data with physical constraints to uncover dynamic chromosome reorganization. Thus, molecular dynamics simulations, constrained by Hi-C contact matrices, can resolve fine-scale structural changes and reveal functionally significant transitions in chromatin conformation. Results Herein, we present the 4D Genome Browser Workflow (4DGBWorkflow) and the 4D Genome Browser (4DGB). The algorithm is based on the 4DHiC method, and the containerized tool is an end-to-end workflow that can transform, filter, and view 4D epigenomics and chromatin datasets, allowing non-specialists to apply three-dimensional modeling principles to diverse datasets and experimental conditions. The software executes on a laptop running macOS, Linux or Windows. From input Hi-C files (.hic), the 4DGBWorkflow produces 3D reconstructions of chromosomes, integrates the reconstruction with track data (e.g., epigenetic marks, transcriptome profiles), and provides comparative visualization of the results in a single workflow. Conclusions The 4DGBWorkflow and 4D Genome Browser are open-source tools for comparative analysis and visualization of 4D chromosome datasets, including chromatin architecture and epigenomic signals. Automatic integration of Hi-C data with molecular dynamics democratizes the construction of time resolved 3D genome structures, simplifying complex simulations and data integration schemes.

3D Genome Browser↗

Ozone perturbations by enhanced levels of CFCs, N2O, and CH4 A two-dimensional diabatic circulation study including uncertainty estimates

Observations made over the last few years suggest that the tropospheric concentrations of N2O, CH4, and O3 are increasing. Increases in the concentration of chlorofluorocarbons (CFCs) have been observed for some time. The present study is concerned with combined scenarios of future releases of N2O, CH4, and CFCs, which can affect the height profiles of ozone, while changes in latitudinal gradients of ozone may also be expected. Ozone perturbation calculations performed in the two-dimensional transport-chemistry model described by Stordal et al. (1985) are also presented, and the effects of increased levels of CFCs, N2O, and CH4 are examined. It is found that CH4 may be the most important ozone-perturbing trace species in connection with future tropospheric climatic impacts. A substantial increase in the tropospheric abundancy of CH4 could lead to large future ozone enhancements throughout the troposphere and lower stratosphere at middle and low latitudes.

Isaksen, I. S. A.↗