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At least 73 records · Page 4

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NASA NTRS1986

A kinetics study of the homogeneous and heterogeneous components of the HCl + ClONO2 reaction

The kinetics of the reaction HCl + ClONO2 to Cl2 + HNO3 were investigated at 298 K using a flow reactor with FTIR analysis to assess the importance of this reaction for stratospheric chemistry. The observed reaction was characteristic of a heterogeneous process; an upper limit of 5 x 10 to the -18th cu cm/molecule per s was obtained for the homogeneous gas phase rate constant. From calculations of the first order wall rate constant, estimates were made of the reaction rate on stratospheric aerosols. Because both HCl and ClONO2 need to be adsorbed on the particle surface, the reaction will be of negligible importance under most stratospheric conditions.

Friedl, Randall R.↗

NASA NTRS1990

Theoretical predictions

In order to understand the impact of man made chemicals on the atmospheric ozone layer, it is essential to develop models that can perform long term predictions of future ozone changes. An advantage of using two dimensional models is that they can be used to predict latitudinal and seasonal changes in ozone. The formulation and recent improvements are described in 2-D models, which are used herein, along with the three dimensional models that are currently being developed to better simulate transport of chemically active trace gases, especially in polar regions. The range in 2-D model calculations is described. Selected fields calculated by these models are compared with observations. A number of scenarios have been defined, which encompass possible emission rates of different halocarbons. Because of the large uncertainties in the rates for heterogeneous processes, the calculated responses of the models include only the effects of homogeneous chemistry. One important distinction among the models is their ability to account for temperature feedbacks on the calculated ozone changes.

Brasseur, G.↗

NASA NTRS1992

A computer model for one-dimensional mass and energy transport in and around chemically reacting particles, including complex gas-phase chemistry, multicomponent molecular diffusion, surface evaporation, and heterogeneous reaction

Various chemically reacting flow problems highlighting chemical and physical fundamentals rather than flow geometry are presently investigated by means of a comprehensive mathematical model that incorporates multicomponent molecular diffusion, complex chemistry, and heterogeneous processes, in the interest of obtaining sensitivity-related information. The sensitivity equations were decoupled from those of the model, and then integrated one time-step behind the integration of the model equations, and analytical Jacobian matrices were applied to improve the accuracy of sensitivity coefficients that are calculated together with model solutions.

Cho, S. Y.↗

NASA NTRS1991

Predicted rocket and shuttle effects on stratospheric ozone

The major chemical effluents of either solid- or liquid-fueled rockets that can potentially perturb stratospheric ozone include chlorine compounds (HCl), nitrogen compounds (NO(x)), and hydrogen compounds (H2 and H2O). Radicals (Cl, ClO, H, OH, HO2, NO, and NO2) formed directly or indirectly from rocket exhaust can cause the catalytic destruction of ozone. Other exhaust compounds that could presumably lead to ozone destruction either by direct reaction with ozone or by providing a surface for heterogeneous processes include the particulates Al2O3, ice, and soot. These topics are discussed in terms of the possible effects of rocket exhausts on stratospheric ozone.

Harwood, Robert S.↗

NASA NTRS1993

CLAES observations of ClONO2 and HNO3 in the Antarctic stratosphere, between June 15 and September 17, 1992

The Cryogenic Array Etalon Spectrometer (CLAES) on the NASA Upper Atmosphere Research Satellite (UARS) began viewing the stratosphere in October 1991. This paper presents preliminary retrievals of ClONO2 and HNO3 from the CLAES measurements for selected days in June, July, August, and September of 1992 for the Southern Hemisphere. The data shows that by July 10, lower stratospheric ClONO2 and HNO3 have developed high 'collar' regions surrounding the polar vortex, and low values inside the vortex. This general structure is sustained through September 17, although the ClONO2 values inside the vortex increase significantly by this date. The data suggests that substantial sequestration of gaseous HNO3 in polar stratospheric clouds occurs in the early winter Antarctic stratosphere, accompanied by the conversion of ClONO2 to reactive chlorine through heterogeneous processes on the PSCs.

Roche, A. E.↗

NASA NTRS1994

A Monte Carlo study of photochemical model uncertainties affecting the calculation of subsonic perturbations in the upper troposphere

Monte Carlo methods are frequently applied to the evaluation of uncertainties in models with multiple inputs that themselves have associated imprecisions. In the case of photochemical models used to evaluate changes in O3 or OH, inputs analyzed include rate coefficients measured in the laboratory, and chemical and physical constituents measured in the atmosphere. The Monte Carlo method was used with the 1-dimensional GSFC tropospheric photochemical model to examine uncertainty propagation to calculation of NO(x) and the major oxidants (O3, OH) in the upper troposphere. In all cases chemical kinetics inputs are varied and the NO(x) perturbation of a subsonic fleet is simulated. A series of model runs is used to explore sensitivities of model-computed parameters to other parameters: heterogeneous processes, the uncertainty in upper tropospheric H2O vapor measurements, aircraft emissions at different latitudes.

Thompson, Anne M.↗

NASA NTRS1994

Observation of hydration of single, modified carbon aerosols

We have compared the hydration behavior of single carbon particles that have been treated by exposure to gaseous H2SO4 with that of untreated particles. Untreated carbon particles did not hydrate as the relative humidity varied from 0 to 80% at 23 C. In contrast, treated particles hydrated under subsaturation conditions; mass increases of up to 30% were observed. The mass increase is consistent with sulfuric acid equilibration with the ambient relative humidity in the presence of inert carbon. For the samples studied, the average amount of absorbed acid was 14% +/- 6% by weight, which corresponds to a surface coverage of approximately 0.1 monolayer. The mass fraction of surface-absorbed acid is comparable to the soluble mass fraction observed by Whitefield et al. (1993) in jet aircraft engine aerosols. Estimates indicate this mass fraction corresponds to 0.1% of the available SO2 exiting an aircraft engine ending up as H2SO4 on the carbon aerosol. If this heterogeneous process occurs early enough in the exhaust plume, it may compete with homogeneous nucleation as a mechanism for producing sulfuric acid rich aerosols.

Wyslouzil, B. E.↗

NASA NTRS1995

Estimation of polar stratospheric cloud infrared extinction climatology using visible satellite observations

Polar stratospheric clouds (PSC's) provide surfaces for heterogeneous processes which can dramatically alter the normal partitioning of odd nitrogen and chlorine families in the winter polar stratospheres, setting up conditions for significant ozone depletion as manifested in the springtime Antarctic ozone hole. The spatial and temporal distribution of PSC's is important for parameterizing PSC occurrence in multidimensional photochemical models whose use is essential for fully understanding observed Antarctic ozone losses as well as for accessing the possibility of a similar phemonenon occurring in the future in the Arctic. The Stratospheric Aerosol Measurement (SAM) 2 sensor, a single-channel (1mu m) photometer launched into a Sun-synchronous orbit aboard the Nimbus 7 satellite in October 1978, provided a unique database to establish the climatology of PSC's. Poole and Pitts (1994) used the record of high-latitude aerosol extinction obtained by SAM II from 1979-1989 to establish the climatology of PSC occurrences in the Arctic and Antarctic. Unfortunately, little information about PSC composition or type was detectable from the single-wavelength SAM II data.

Pitts, Michael C.↗

NASA NTRS1998

Contrast Between 1992 and 1997 High Latitude Spring Haloe Observations of Lower Stratospheric HCl

HCl measurements from HALOE in the northern hemisphere during mid-May 1997 revealed vortex fragments in which the chlorine reservoir partitioning was strongly pushed toward HCl (approx. 90% HCl, approx. 10% ClONO2), similar to partitioning previously observed in the Antarctic vortex region. In contrast, observations of ClONO2 and HCl in the northern polar spring, 1992, and in other years, show these species established the balance typical for gas phase photochemical reactions in this region (approx. 60% HCl, approx. 40% ClONO2). Annually, chlorine reservoirs in the winter lower stratosphere polar vortex are converted to chlorine radicals via heterogeneous reactions on particle surfaces at very cold temperatures (less than about 200 K). As temperatures warm in spring, the heterogeneous processes become insignificant compared with gas phase reactions, and the chlorine reservoirs are reformed. Measurements through the northern winter/spring in 1992 show rapid formation of ClONO2, followed by steady loss of ClONO2 and increasing HCl. Although ClONO2 measurements are not available for 1997, the HCl increase in 1997 is observed to be much more rapid and the eventual HCl mixing ratio is about 50% greater than that of 1992. The observations are examined through comparison with the Goddard three-dimensional chemistry and transport model. This model utilizes winds and temperatures from the Goddard Earth Observing System Data Assimilation System and a complete integration scheme for stratospheric photochemistry. Analysis of the evolution of HCl and ClONO2 shows that the observed difference in the overall rate of HCl formation is explained by the sensitivity of the gas-phase chemistry to the ozone mixing ratio and the temperature. The results show that the model accurately simulates HCl and ClONO2 evolution during these two winters. Model validity is further supported by comparisons with O3 and reactive nitrogen species NO and NO2. This analysis provides a sensitive test of the lower stratospheric chlorine photochemistry, particularly because the analysis considers constituent evolution at a time when the HCl and ClONO2 are far from a photochemical stationary state.

Douglass, A. R.↗

NASA NTRS2000

The Interaction Between Dynamics and Chemistry of Ozone in the Set-Up Phase of the Northern Hemisphere Polar Vortex

Understanding stratospheric ozone loss to the point of accurately predicting ozone in the future requires correctly distinguishing chemical from transport-induced changes in ozone. For example, evaluating the impact of chlorine reduction in controlling stratospheric ozone loss requires estimating the amount of ozone lost in chemical reactions in the polar winter and spring. The Northern Hemisphere winter polar region is a particularly crucial and interesting area because it appears that the Northern vortex may currently be poised near the threshold of extreme ozone destruction such as that which now occurs annually in the Antarctic ozone "hole." In this presentation we explore the interaction of ozone transport and chemistry through the Northern late summer and fall seasons as the vortex circulation becomes established. This phase of the seasonal cycle determines the starting point for heterogeneous processes and chlorine-driven loss that take control in the winter vortex. Using a combination of profile data from POAM, HALOE, and in situ measurements, we show that relatively low ozone at high latitudes in the middle stratosphere is associated with vortex airmasses and that these ozone abundances evolve photochemically from characteristically higher values at the end of the summer. The zonal variance of ozone mixing ratio also increases greatly at this time consistent with increasing wave-driven transport. Comparison with a three-dimensional chemistry-transport model is used to generalize the findings from the limited set of observations and quantify the relative roles of transport and chemistry in determining the ozone mixing ratio distributions.

Kawa, S.R.↗

NASA NTRS2000

Introduction to the SONEX (Subsonic Assessment Ozone and Nitrogen Oxides Experiment) and POLINAT-2 (Pollution from Aircraft Emissions in the North Atlantic Flight Corridor) Special Issue

Emissions of atmospheric species from the engines of subsonic aircraft at cruise altitude (roughly, above seven kilometers) are of concern to scientists, the aviation industry and policymakers for two reasons. First, water vapor, soot and sulfur oxides, and related heterogeneous processes, may modify clouds and aerosols enough to perturb radiative forcing in the UT/LS (upper troposphere/lower stratosphere). A discussion of these phenomena appears in Chapter 3 of the IPCC Aviation Assessment (1999). An airborne campaign conducted to evaluate aviation effects on contrail, cirrus and cloud formation, is described in Geophysical Research Letters. The second concern arises from subsonic aircraft emissions of nitrogen oxides (NO + NO2 = NO(sub x)), CO, and hydrocarbons. These species may add to the background mixture of photochemically reactive species that form ozone. In the UT/LS, ozone is a highly effective greenhouse gas. The impacts of subsonic aircraft emissions on tropospheric NO(sub x) and ozone budgets have been studied with models that focus on UT chemistry [e.g. see discussions of individual models in Brasseur et al., 1998; Friedl et al., 1997; IPCC, 1999]. Depending on the model used, projected increases in the global subsonic aircraft fleet from 1992 to 2015 will lead to a 50-100 pptv increase in UT/LS NO. at 12 km (compared to 50-150 pptv background) in northern hemisphere midlatitudes. The corresponding 12-km ozone increase is 7-11 ppbv, or 5-10% (Chapter 4 in IPCC, 1999). Two major sources of uncertainties in model estimates of aviation effects are: (1) the often limited degree to which global models - the scale required to evaluate aircraft emissions - realistically simulate atmospheric transport and other physical processes; (2) limited UT/LS observations of trace gases with which to evaluate model performance. In response to the latter deficiency, a number of airborne campaigns aimed at elucidating the effect of aircraft on atmospheric nitrogen oxides and ozone were performed between 1990 and 1996 (see descriptions in Friedl et al., 1997; Brasseur et al., 1998).

Thompson, Anne M.↗

NASA NTRS1990

Radiolysis of aqueous solutions of acetic acid in the presence of Na-montmorillonite

The gamma-irradiation of 0.8 mol dm-3 aqueous, oxygen-free acetic acid solutions was investigated in the presence or absence of Na-montmorillonite. H2, CH4, CO, CO2, and several polycarboxylic acids were formed in all systems. The primary characteristics observed in the latter system were: (1) Higher yield of the decomposition of acetic acid; (2) Lower yield of the formation of polycarboxylic acids; (3) No effect on the formation of methane; (4) Higher yield of the formation of carbon dioxide; and (5) The reduction of Fe3+ in the octahedral sites of Na-montmorillonite. A possible reaction scheme was proposed to account for the observed changes. The results are important in understanding heterogeneous processes in radiation catalysis and might be significant to prebiotic chemistry.

Non-NASA Center↗

NASA NTRS2004

Heterogeneous Chemistry Involving Methanol in Tropospheric Clouds

In this report we analyze airborne measurements to suggest that methanol in biomass burning smoke is lost heterogeneously in clouds. When a smoke plume intersected a cumulus cloud during the SAFARI 2000 field project, the observed methanol gas phase concentration rapidly declined. Current understanding of gas and aqueous phase chemistry cannot explain the loss of methanol documented by these measurements. Two plausible heterogeneous reactions are proposed to explain the observed simultaneous loss and production of methanol and formaldehyde, respectively. If the rapid heterogeneous processing of methanol, seen in a cloud impacted by smoke, occurs in more pristine clouds, it could affect the oxidizing capacity of the troposphere on a global scale.

Tabazadeh, A.↗

DOE OSTI2020

Markovian transport processes in a heterogeneous, variably saturated watershed: A multi-domain spatial Markov model

Transport processes in watersheds remain challenging to describe accurately with upscaled models because of their intricate complexities at multiple scales that can lead to multi-modal, non-Fickian breakthrough curves. One of the recent advances in solute transport modeling has been the Lagrangian spatial Markov model (SMM), which describes transport using velocity increments and models the correlated transitions between them. The method has been applied previously to saturated porous media and fractured media, but these successful applications suggest it may be useful for describing watershed scale processes as well. An existing, 3-D, heterogeneous variably saturated model of a headwaters catchment and classical random walk particle tracking were used to generate a forward simulation and the resulting transport was analyzed with a spatial Markov framework. Existing SMM methods were used to analyze the transport paths through the complex, unconfined domain and we found that the vadose zone plays an important role in the correlation structure. As such, a new kind of SMM is proposed, termed a multi-domain SMM (MD-SMM), that uses separate correlation models for auto-transitions in the vadose zone and the saturated zone, and for the cross-transitions between them. The MD-SMM improves representation of transport relative to the single domain model and can naturally delineate times when a particle is in the vadose zone or the saturated zone, adding an additional degree of realism to the upscaled model. Lastly, we show that the transition probability matrix for transport in the saturated portion of this unconfined system is approximately Markovian, which is an important validation of the proposed framework.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Heterogeneous data-processing optimization with CLARA’s adaptive workflow orchestrator

The hardware landscape used in HEP and NP is changing from homogeneous multi-core systems towards heterogeneous systems with many different computing units, each with their own characteristics. To achieve maximum performance with data processing, the main challenge is to place the right computing on the right hardware. In this paper, we discuss CLAS12 charge particle tracking workflow orchestration that allows us to utilize both CPU and GPU to improve the performance. The tracking application algorithm was decomposed into micro-services that are deployed on CPU and GPU processing units, where the best features of both are intelligently combined to achieve maximum performance. In this heterogeneous environment, CLARA aims to match the requirements of each micro-service to the strength of a CPU or a GPU architecture. A predefined execution of a micro-service on a CPU or a GPU may not be the most optimal solution due to the streaming data-quantum size and the data-quantum transfer latency between CPU and GPU. So, the CLARA workflow orchestrator is designed to dynamically assign micro-service execution to a CPU or a GPU, based on the online benchmark results analyzed for a period of real-time data-processing.

Gyurjyan, Vardan↗

NASA NTRS1985

Heterogeneous distributed query processing: The DAVID system

The objective of the Distributed Access View Integrated Database (DAVID) project is the development of an easy to use computer system with which NASA scientists, engineers and administrators can uniformly access distributed heterogeneous databases. Basically, DAVID will be a database management system that sits alongside already existing database and file management systems. Its function is to enable users to access the data in other languages and file systems without having to learn the data manipulation languages. Given here is an outline of a talk on the DAVID project and several charts.

Jacobs, Barry E.↗

NASA NTRS1989

Heterogeneous physicochemistry of the polar ozone hole

Processes occurring in the polar winter stratosphere, which involve polar stratospheric clouds (PSCs), are investigated using observations from the Airborne Antarctic Ozone Experiment. In particular, data on the properties of PSCs and their physical chemistry, the microphysical processes and time constants for cloud processes, the heterogeneous chemical processes and their time constants, and nonlinearities in the long-term ozone trend associated with physical and chemical processes are examined. The chemical reactions leading to the depletion of the inert chlorine reservoir in a presence of type I PSCs are established, and it is shown that type II PSCs contribute to chemical processing that sustains the chemical imbalance of the polar stratosphere. It is shown that, using a simple model, the decadal evolution of the Antarctic ozone hole may be understood through nonlinearities in the heterogeneous chemistry, with possible contributing effects of variations in stratospheric temperatures and water vapor concentrations.

Turco, Richard P.↗

DOE OSTI2020

Direct Measure of Electrode Spatial Heterogeneity: Influence of Processing Conditions on Anode Architecture and Performance

The spatial (in)homogeneity of aqueous processed silicon electrodes using standard poly(acrylic acid)-based binders and slurry preparation conditions is demonstrated in this work. X-ray nanotomography shows segregation of materials into submicron-thick layers depending on the mixing method and starting binder molecular weights. Using a dispersant, or in situ production of dispersant from the cleavage of the binder into smaller molecular weight species, increases the resulting lateral homogeneity while drastically decreasing the vertical homogeneity as a result of sedimentation and separation due to gravitational forces. This data explains some of the variability in the literature with respect to silicon electrode performance and demonstrates two potential ways to improve slurry-based electrode fabrications.

36 MATERIALS SCIENCE↗