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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
NASA NTRS1991

Field-aligned dynamics of chemically induced perturbations to the ionosphere

Ionospheric modification using photochemically reactive vapors is studied with a one-dimensional, multiion, fluid model of plasma flow along magnetic field lines. The magnitudes of ion and electron density changes are determined by considering both chemical processes (i.e., photoionization, ion-molecule reactions, dissociative recombination, electron attachment) and transport processes (i.e., multispecies diffusion, electric currents, ambipolar electric fields). The numerical treatment in the model is not specific to any type of release or any interaction chemistry. It has been used to simulate releases of Ba, CO2, and CF3Br in the ionosphere, but generalization to other species may be easily accomplished. The results of the calculations are found to be in good agreement with experimental observations. The feasibility of modifying the parallel current paths in the auroral F region is examined.

Bernhardt, P. A.↗
NASA NTRS1992

State-selected chemical reaction dynamics at the S matrix level - Final-state specificities of near-threshold processes at low and high energies

State-to-state reaction probabilities are found to be highly final-state specific at state-selected threshold energies for the reactions O + H2 yield OH + H and H + H2 yield H2 + H. The study includes initial rotational states with quantum numbers 0-15, and the specificity is especially dramatic for the more highly rotationally excited reactants. The analysis is based on accurate quantum mechanical reactive scattering calculations. Final-state specificity is shown in general to increase with the rotational quantum number of the reactant diatom, and the trends are confirmed for both zero and nonzero values of the total angular momentum.

Chatfield, David C.↗
NASA NTRS1999

Dynamical and Chemical Behavior of the Lower Stratosphere and Interactions with the Troposphere

Equivalent-barotropic calculations, in tandem with Lagrangian analyses, reveal how changes of total ozone follow from vertical and horizontal transport by planetary waves. Those calculations also throw light on how diabatic motions comprising the Brewer-Dobson circulation develop from quasi-horizontal advection by planetary waves. Potential temperature along a material surface indicates organized subsidence inside the polar-night vortex, resembling tracer observations from UARS. Lagrangian histories illustrate that this sinking motion follows in large part from parcels being driven out of thermodynamic equilibrium by planetary waves, especially at high latitudes. Irreversible heat transfer then produces a net drift of air across isentropic surfaces as parcels orbit about the displaced vortex. By driving mean-meridional overturning in the stratosphere, this downward drift is ultimately responsible for transferring ozone from the tropics to the extratropical lower stratosphere. It also introduces horizontal structure into the distribution of total ozone, which surfaces clearly in ozone trends. High-resolution global cloud imagery constructed from 6 satellites simultaneously observing the Earth was used to investigate the spectrum of equatorial waves generated by tropical convection and propagating vertically into the stratosphere. The results indicate that temperature variability is dominated by planetary-scale equatorial waves like the Kelvin mode, which agrees with satellite observations of the tropical stratosphere. However, the Kelvin mode accounts for only about 30 - 50% of the eastward momentum flux radiating into the stratosphere, the remainder coming from gravity waves. An algorithm was developed to determine 3-dimensional atmospheric motion from satellite tracer measurements. Based on Lagrangian constraints, the algorithm circumvents limitations of the traditional scheme for inferring motion from temperature measurements and determines the circulation in the tropics as reliably as elsewhere. A study of deep convection revealed that the highest towers (those penetrating into stratospheric air and controlling tropopause height and composition through convective mixing) occur in close association with the diurnal cycle of convection. Clouds colder than 220 K develop almost entirely in association with the diurnal cycle of convection over tropical landmasses and substantially in association with it even over maritime regions.

Salby, Murry L.↗
NASA NTRS2005

Separating the Chemical and Dynamical Contributions to the Ozone Change

Statistical analysis is used to extract the sensitivity of ozone to changes in stratospheric chlorine due to emissions of chlorofluorcarbons from the observed ozone record. The statistical analysis relies on a model that accounts for natural variations in ozone including the seasonal cycle, the solar cycle, variations in aerosols due to volcanic eruption, and the quasi- biennial oscillation, A noise term includes contributions to ozone variability due to inter-annual variability in the stratospheric circulation not due to the quasi-biennial oscillation, The residual circulation varies due to variability in planetary wave forcing, and studies using meteorological analyses show that the build-up of ozone over the winter is correlated with the planetary wave Eliassen-Palm flux. This variability in the residual circulation is not included in the statistical model, and contributes to the apparent ozone sensitivity to chlorine derived from observations for 1979 - 2000. We have investigated these relationships using multi-decadal simulations of our off-line chemistry and transport model (CTM). Our simulations use meteorological fields output from a 50 year simulation of a general circulation model (GCM). A 50 climatology specifies the sea surface temperatures to produce the GCM simulation. The CTM was used with these winds to produce two simulations, one in which the boundary conditions for chlorofluorcarbons and other source gases vary as specified for 1973-2022 by the Scenario A2 of the World Meteorological Organization ozone assessment, and the second with source gases fixed to their 1979 values. The same statistical analysis used to derive trends from observations is applied to the CTM output. When applied to the difference between the two simulations the statistical analysis provides a more precise measure of the ozone sensitivity to chlorine change. We are testing ways of including the interannual variability in the residual circulation in the statistical model so that we can derive the same result from the Scenario A2 simulation as is obtained when the statistical analysis is applied to the difference between the two simulations. This should provide direction as to how to account for the changes in ozone due to interannual variability in the residual circulation in the statistical model that is applied to the observed data record.

Douglass, Anne R.↗
NASA NTRS2012

The Chemical and Dynamical Responses of Ozone and Nitrogen Dioxide to the Eruption of Mt. Pinatubo

Observations have shown that the concentration of nitrogen dioxide decreased in both hemispheres in the years following the eruption of Mt. Pinatubo. In contrast, the observed ozone response was largely asymmetrical with respect to the equator, with a decrease in the northern hemisphere and little or no change in the southern hemisphere. Simulations including enhanced heterogeneous chemistry due to the presence of the volcanic aerosol reproduce a decrease of ozone in the northern hemisphere, but also produce a comparable ozone decrease in the southern hemisphere contrary to observations. Our simulations show that the heating due to the volcanic aerosol enhanced both the tropical upwelling and the extratropical downwelling. The enhanced extratropical downwelling, combined with the time of the eruption relative to the seasonal phase of the Brewer-Dobson circulation, increased the ozone in the southern hemisphere and counteracted the ozone depletion due to heterogeneous chemistry on volcanic aerosol.

Aquila, V.↗
NASA NTRS1985

Effects of breaking gravity waves on the chemical composition of the mesosphere and lower thermosphere

Eddy diffusion and momentum forcing in the mesosphere and lower thermosphere arise principally from the effects of breaking gravity and waves. The propagation and dissipation of gravity waves depend strongly on season and latitude because of its relationship to the background zonal wind. These processes have significant effects on the transport of chemical species in that region, so that observations of variations in chemical constituents provide useful tracers for dynamical theory. A parameterization of gravity wave propagation and dissipation was incorporated in the coupled dynamical-chemical model to study these effects. Several easily observable airglow features of the mesosphere-thermosphere region are shown to provide sensitive indications of gravity wave influence. In particular, theoretical predictions of large seasonal and latitudinal variations in the atomic oxygen green line, the Meinal bands of excited OH, and the O3 densities inferred from O2 (delta supra 1 sub g) emission at altitudes from 75 to 90 km are shown to be in remarkably good agreement with observations. Implications of these sensitive chemical tracers for the dynamics of the mesosphere-lower thermosphere region and its relationship to gravity waves are discussed.

Solomon, S.↗
DOE OSTI2021

Stiff neural ordinary differential equations

Neural Ordinary Differential Equations (ODEs) are a promising approach to learn dynamical models from time-series data in science and engineering applications. This work aims at learning neural ODEs for stiff systems, which are usually raised from chemical kinetic modeling in chemical and biological systems. We first show the challenges of learning neural ODEs in the classical stiff ODE systems of Robertson’s problem and propose techniques to mitigate the challenges associated with scale separations in stiff systems. We then present successful demonstrations in stiff systems of Robertson’s problem and an air pollution problem. The demonstrations show that the usage of deep networks with rectified activations, proper scaling of the network outputs as well as loss functions, and stabilized gradient calculations are the key techniques enabling the learning of stiff neural ODEs. The success of learning stiff neural ODEs opens up possibilities of using neural ODEs in applications with widely varying time-scales, such as chemical dynamics in energy conversion, environmental engineering, and life sciences.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2021

Revealing the Dynamics and Roles of Iron Incorporation in Nickel Hydroxide Water Oxidation Catalysts

We report the surface of an electrocatalyst undergoes dynamic chemical and structural transformations under electro-chemical operating conditions. There is a dynamic exchange of metal cations between the electrocatalyst and electrolyte. Understanding how iron in the electrolyte gets incorporated in the nickel hydroxide electrocatalyst is critical for pinpointing the roles of Fe during water oxidation. Here, we report that iron incorporation and oxygen evolution reaction (OER) are highly coupled, especially at high working potentials. The iron incorporation rate is much higher at OER potentials than that at the OER dormant state (low potentials). At OER potentials, iron incorporation favors electrochemically more reactive edge sites, as visualized by synchrotron X-ray fluorescence microscopy. Using X-ray absorption spectroscopy and density functional theory calculations, we show that Fe incorporation can suppress the oxidation of Ni and enhance the Ni reducibility, leading to improved OER catalytic activity. Our findings provide a holistic approach to understanding and tailoring Fe incorporation dynamics across the electrocatalyst-electrolyte interface, thus controlling catalytic processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

Discoveries about Tropospheric Ozone Pollution from Satellite and Sounding

We have been producing near-real time tropospheric ozone satellite maps from the TOMS (Total Ozone Mapping Spectrometer) sensor since 1997. This is most readily done for the tropics, where the stratospheric and tropospheric ozone column amounts can be discriminated readily. Maps for 1996-2000 for the operational Earth-Probe instrument reside at: chttp://www.atmos.umd.edu/-trope>. Pollution in the tropics is influenced by biomass burning and by transport patterns that favor recirculation and in other cases reflect climate variability like the El-Nino-Southern Oscillation [Thompson et al., 2001]. Time permitting, examples of mid-latitude, intercontinental transport of ozone pollution sensed by TOMS will be shown. The satellite view of chemical-dynamical interactions in tropospheric ozone is not adequate to capture vertical variability. Thus, in 1998, NASA's Goddard Space Flight Center and a team of international sponsors established the SHADOZ (Southern Hemisphere ADditional OZonesondes) project to address the gap in tropical ozone soundings. SHADOZ augments launches and provides a public archive of ozonesonde data from twelve tropical stations at http://croc.gsfc.nasa.gov/shadoz. Further insights into the role of chemical and dynamical influences have emerged from the first 4-5 years of SHADOZ data (less than 2000 ozone profiles): (a) highly variable tropospheric ozone; (b) a zonal wave-one pattern in tropospheric column ozone; (c) convective variability affects tropospheric ozone over the Indian and Pacific Ocean; (d) a "tropical Atlantic Paradox" appears in December-January-February.

Thompson, Anne M.↗
NASA NTRS2004

Discoveries about Tropospheric Ozone Pollution from Satellite and Soundings

We have been producing near-red time tropospheric ozone satellite maps from the TOMS (Total Ozone Mapping Spectrometer) sensor since 1997. Maps for 1996-2000 for the operational Earth-Probe instrument are at: . Pollution in the tropics is influenced by biomass burning and by transport patterns that favor recirculation and in other cases reflect climate variability like the El-Nino-Southern Oscillation [Thompson et al., 2001]. The satellite view of chemical-dynamical interactions in tropospheric ozone is not adequate to capture vertical gradients in pollution. Thus, in 1998, NASA's Goddard Space Flight Center and a team of international sponsors established the SHADOZ (Southern Hemisphere ADditional OZonesondes) project to address the gap in tropical ozone soundings. SHADOZ augments launches and provides a public archive of ozonesonde data from twelve tropical stations at http://croc.gsfc.nasa.gov/shadoz. Further insights into the role of chemical and dynamical influences have emerged from the first 4-5 years of SHADOZ data (more than 2000 ozone profiles). Highly variable tropospheric ozone and a zonal wave-one pattern in tropospheric ozone suggest that dynamics is as important as pollution in determining tropical ozone distributions.

Thompson, Anne M.↗
DOE OSTI2023

Remembering the Work of Phillip L. Geissler: A Coda to His Scientific Trajectory

Phillip L. Geissler made important contributions to the statistical mechanics of biological polymers, heterogeneous materials, and chemical dynamics in aqueous environments. He devised analytical and computational methods that revealed the underlying organization of complex systems at the frontiers of biology, chemistry, and materials science. In this retrospective we celebrate his work at these frontiers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1988

Effects of eddy viscosity and thermal conduction and Coriolis force in the dynamics of gravity wave driven fluctuations in the OH nightglow

The chemical-dynamical model of Walterscheid et al. (1987), which describes wave-driven fluctuations in OH nightglow, was modified to include the effects of both eddy thermal conduction and viscosity, as well as the Coriolis force (with the shallow atmosphere approximation). Using the new model, calculations were performed for the same nominal case as used by Walterscheid et al. but with only wave periods considered. For this case, the Coriolis force was found to be unimportant at any wave period. For wave periods greater than 2 or 3 hours, the inclusion of thermal conduction alone greatly modified the results (in terms of a complex ratio 'eta' which expresses the relationship between the intensity oscillation about the time-averaged intensity and the temperature oscillation about the time-averaged temperature); this effect was reduced with the further inclusion of the eddy viscosity.

Hickey, M. P.↗
DOE OSTI2025

Learning to Simulate Aerosol Dynamics with Graph Neural Networks

Aerosol effects on climate, weather, and air quality depend on characteristics of individual particles, which are tremendously diverse and change in time. Particle-resolved models are the only models able to capture this diversity in particle physiochemical properties, and these models are computationally expensive. As a strategy for accelerating particle-resolved microphysics models, we introduce Graph-based Learning of Aerosol Dynamics (GLAD) and use this model to train a surrogate of the particle-resolved model PartMC-MOSAIC. GLAD implements a Graph Network-based Simulator (GNS), a machine learning framework that has been used to simulate particle-based fluid dynamics models. In GLAD, each particle is represented as a node in a graph, and the evolution of the particle population over time is simulated through learned message passing. Here, we demonstrate our GNS approach on a simple aerosol system that includes condensation of sulfuric acid onto particles composed of sulfate, black carbon, organic carbon, and water. A graph with particles as nodes is constructed, and a graph neural network (GNN) is then trained using the model output from PartMC-MOSAIC. The trained GNN can then be used for simulating and predicting aerosol dynamics over time. Results demonstrate the framework's ability to accurately learn chemical dynamics and generalize across different scenarios, achieving efficient training and prediction times. We evaluate the performance across four scenarios, highlighting the framework's robustness and adaptability in modeling aerosol microphysics and chemistry.

aerosol chemistry dynamics↗
NASA NTRS1994

Development of an upwind, finite-volume code with finite-rate chemistry

Under this grant, two numerical algorithms were developed to predict the flow of viscous, hypersonic, chemically reacting gases over three-dimensional bodies. Both algorithms take advantage of the benefits of upwind differencing, total variation diminishing techniques, and a finite-volume framework, but obtain their solution in two separate manners. The first algorithm is a zonal, time-marching scheme, and is generally used to obtain solutions in the subsonic portions of the flow field. The second algorithm is a much less expensive, space-marching scheme and can be used for the computation of the larger, supersonic portion of the flow field. Both codes compute their interface fluxes with a temporal Riemann solver and the resulting schemes are made fully implicit including the chemical source terms and boundary conditions. Strong coupling is used between the fluid dynamic, chemical, and turbulence equations. These codes have been validated on numerous hypersonic test cases and have provided excellent comparison with existing data.

Molvik, Gregory A.↗
NASA NTRS1995

Development of an upwind, finite-volume code with finite-rate chemistry

Under this grant, two numerical algorithms were developed to predict the flow of viscous, hypersonic, chemically reacting gases over three-dimensional bodies. Both algorithms take advantage of the benefits of upwind differencing, total variation diminishing techniques and of a finite-volume framework, but obtain their solution in two separate manners. The first algorithm is a zonal, time-marching scheme, and is generally used to obtain solutions in the subsonic portions of the flow field. The second algorithm is a much less expensive, space-marching scheme and can be used for the computation of the larger, supersonic portion of the flow field. Both codes compute their interface fluxes with a temporal Riemann solver and the resulting schemes are made fully implicit including the chemical source terms and boundary conditions. Strong coupling is used between the fluid dynamic, chemical and turbulence equations. These codes have been validated on numerous hypersonic test cases and have provided excellent comparison with existing data. This report summarizes the research that took place from August 1,1994 to January 1, 1995.

Molvik, Gregory A.↗
DOE OSTI2021

Experimental Studies of the Dynamics of Adsorbed and Condensed Phase Iodine Species Formed in Severe Reactor Accidents (Final Project Report)

We have studied the chemical transformations of semi-volatile organic iodide species (RI) in the condensed phase as well as adsorbed onto the surfaces of environmentally relevant particles, e.g., soot (carbon) and dust (silica) under real-world conditions. The combination of chosen experimental methods provide a molecular-level insight into the chemical dynamics of organic iodides. Throughout this project, we have developed new experimental, quantum chemistry, and data analysis capabilities. All experimental work was performed with 127 I.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Energy-conserving coupled trajectory mixed quantum–classical dynamics

The coupled-trajectory mixed quantum–classical method (CTMQC), derived from the exact factorization approach, has successfully predicted photo-chemical dynamics in a number of interesting molecules, capturing population transfer and decoherence from first principles. Furthermore, due to the approximations made, CTMQC does not guarantee energy conservation. We propose a modified algorithm, CTMQC-E, which redefines the integrated force in the coupled-trajectory term so to restore energy conservation, and demonstrate its accuracy on scattering in Tully’s extended coupling region model and photoisomerization in a retinal chromophore model.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗