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NASA NTRS1993

Balloon-borne in situ measurements of ClO and ozone - Implications for heterogeneous chemistry and mid-latitude ozone loss

In situ measurements of chlorine oxide (ClO) obtained on 31 March 1991 with a new balloon-borne instrument are compared to results from a photochemical model which incorporates hydrolysis of N2O5 on sulfate aerosols. With the addition of this process, there is better agreement between calculation and measurement over most of the profile, except below 20 km where observed ClO is greater by as much as a factor of four. In a model which is constrained to reproduce the observed ClO below 20 km, ozone loss by catalytic cycles involving halogen oxides becomes larger than that from NO(x), which would dominate under gas-phase or standard heterogeneous conditions.

Avallone, L. M.↗
NASA NTRS1994

Electrokinetic transport of heterogeneous particles in suspension

The Smoluchowski equation for electrophoresis predicts that the electrophoretic velocity of a particle is proportional to its zeta potential but not its size, shape, or orientation. Furthermore, the equation predicts that the rotation rate is identically zero. The Smoluchowski equation fails for heterogeneous particles (i.e., those with nonuniform zeta potentials). Recent theories and experiments show that particles with a dipole moment of zeta potential rotate into alignment with an externally applied electric field. For doublets (particles composed of two spheres) the rotation rate depends on (1) whether the spheres are rigidly rocked or freely rotating, and (2) the gap distance between the spheres. The relative configuration of two coagulated spheres is determined by the colloidal forces of the system. The goal of our research is to use measurements of electrophoretic rotation to determine the gap between two spheres of a colloidal doublet and also to determine whether or not the doublet is rigid.

Velegol, D.↗
NASA NTRS1995

Remotely sensed indicators of habitat heterogeneity and biological diversity: A preliminary report

The relationship between habitat area, spatial dynamics of the landscape, and species diversity is an important theme in population and conservation biology. Of particular interest is how populations of various species are affected by increasing habitat edges due to fragmentation. Over the last decade, assumptions regarding the effects of habitat edges on biodiversity have fluctuated wildly, from the belief that they have a positive effect to the belief that they have a clearly negative effect. This change in viewpoint has been brought about by an increasing recognition of the importance of geographic scale and a reinterpretation of natural history observations. In this preliminary report from an ongoing project, we explore the use of remote sensing technology and geographic information systems to further our understanding of how species diversity and population density are affected by habitat heterogeneity and landscape composition. A primary feature of this study is the investigation of SAR for making more rigorous investigations of habitat structure by exploiting the interaction between radar backscatter and vegetation structure and biomass. A major emphasis will be on the use of SAR data to define relative structural types based on measures of structural consolidation using the vegetation surface area to volume ratio (SA/V). Past research has shown that SAR may be sensitive to this form of structural expression which may affect biodiversity.

Imhoff, Marc↗
NASA NTRS1994

Heterogeneous conversion of N2O5 to HNO3 in the post-Mount Pinatubo eruption stratosphere

Simultaneous stratospheric volume mixing ration (VMR) profiles of dinitrogen pentoxide (N2O5) and nitric acid (HNO3) at sunrise between 25 deg N and 15 deg S latitude and profiles of HNO3 at sunset between 42 deg S and 53 deg S latitude have been derived from 0.01/cm resolution infrared solar occultation spectra recorded 9.5 months after the massive eruption of the Mount Pinatubo volcano in the Philippine Islands. The measurements were obtained by the atmospheric trace molecule spectroscopy (ATMOS) Fourier transform spectrometer during the ATLAS 1 shuttle mission (March 24 to April 2, 1992). The measured HNO3 VMRs are higher at all altitudes and latitudes than corresponding values measured by the limb infrared monitor of the stratosphere (LIMS) instrument during the same season in 1979, when the aerosol loading was near background levels. The largest relative increase in the HNO3 VMR occurred near the equator at 30-km altitude, where the ATMOS/ATLAS 1 values are about a factor of 2 higher than the LIMS measurements. Two-dimensional model calculations show that the increase in HNO3 and the ATMOS/ATLAS 1 measurement of a steep decrease in the N2O5 VMR below 30 km can be explained by the enhanced conversion of N2O5 to HNO3 on the surfaces of the Mount Pinatubo sulfate aerosols. Our profile results demonstrate the global impact of the N2O5 + H2O yields 2HNO3 heterogeneous reaction in altering the partitioning of stratospheric odd nitrogen after a major volcanic eruption.

Rinsland, C. P.↗
NASA NTRS1994

Balloon profiles of stratospheric NO2 and HNO3 for testing the heterogeneous hydrolysis of N2O5 on sulfate aerosols

Simultaneous in situ measurements of stratospheric NO2, HNO3, HCl, and CH4 from 34 to 24 km were made in August 1992 from Palestine, Texas, using the Balloon-borne Laser In-Situ Sensor (BLISS) tunable diode laser spectrometer. Although the measurements of NO2, HNO3, and NO2/HNO3 agree well with gas-phase model calculations near 34 km where Stratospheric Aerosol and Gas Experiment (SAGE) 2 data show little sulfate aerosol, this is not true at the lower altitudes where SAGE 2 shows high aerosol loadings. At 24 km the BLISS NO2 and HNO3 measurements are 70% lower and 50% higher, respectively, than the gas phase model predictions, with a measured NO2/HNO3 ratio 5 times smaller. When the heterogeneous hydrolysis of N2O5 and ClONO2 on sulfate aerosol of surface area densities matching the SAGE 2 measurements is added to the model, good agreement with the BLISS measurements is found over the whole altitude range.

Webster, C. R.↗
NASA NTRS1994

Ozone loss in the lower stratosphere over the United States in 1992-1993: Evidence for heterogeneous chemistry on the Pinatubo aerosol

Ozone profiles obtained at Boulder, Colorado and Wallops Island, Virginia indicate that ozone was about 25% below normal during the winter and spring of 1992-93 in the 12-22 km region. This large ozone reduction in the lower stratosphere, though sometimes partially compensated by higher than normal ozone above 24 km, was responsible for the low total column ozone values observed across the United States during this period. Normal temperatures throughout the low ozone region suggest that transport-related effects are probably not the most important cause of the ozone deficits. This region of low ozone at Boulder corresponds closely with the location of the enhanced H2SO4/H2O aerosol from the Pinatubo eruption of 1991 as measured near Boulder and at Laramie, Wyoming. Trajectory analyses suggest that except at low altitudes in spring, air parcels on the days of the ozone measurements generally arrived at Boulder from higher latitude, although seldom higher than 60 deg N, and hence may have been subjected to heterogeneous chemical processing on the surface of Pinatubo aerosol droplets resulting in chlorine-catalyzed ozone destruction, a process which is believed to be more effective under the lower winter temperatures and sunlight levels of higher latitudes.

Hofmann, D. J.↗
NASA NTRS1993

Balloon-borne measurements of ClO, NO, and O3 in a volcanic cloud: An analysis of heterogeneous chemistry between 20 and 30 km

Balloon profiles of chlorine monoxide (ClO), nitric oxide (NO), and ozone (O3) were measured on March 11, 1992 from 100 to 10 mb over Greenland (67.0 deg N, 50.6 deg W). Measurements from SAGE II indicate that the aerosol surface area in the region was enhanced by sulfur from the eruption of Mt. Pinatubo, reaching 50 times background near 20 km. Concentrations of ClO were enhanced and concentrations of NO were suppressed relative to low aerosol conditions consistent with the effects of hydrolysis of N2O5 on the surface of sulfuric acid aerosols. The data are consistent with a value of 2 x 10(exp -4) for the reaction probability of the heterogeneous hydrolysis of ClONO2, indicating a minor role for this reaction at as temperature of 220 K. At these temperatures, we find no evidence for the catastrophic loss of ozone predicted to occur under conditions of enhanced aerosol surface area.

Dessler, A. E.↗
NASA NTRS1994

The diurnal variation of hydrogen, nitrogen, and chlorine radicals: Implications for the heterogeneous production of HNO2

In situ measurements of hydrogen, nitrogen, and chlorine radicals obtained through sunrise and sunset in the lower statosphere during SPADE are compared to results from a photochemical model constrained by observed concentrations of radical precursors and environmental conditions. Models allowing for heteogeneous hydrolysis of N2O5 on sulfate aerosols agree with measured concentrations of NO, NO2, and ClO throughout the day, but fail to account for high concentrations of OH and HO2 observed near sunrise and sunset. The morning burst of (OH) and (HO2) coincides with the rise of (NO) from photolysis of NO2, suggesting a new source of HO(x) that photolyzes in the near UV (350 to 400 nm) spectral region. A model that allow for the heterogeneous production of HNO2 results in an excellent simulation of the diurnal variations of (OH) and (HO2).

Salawitch, R. J.↗
NASA NTRS1994

Heterogeneous Reaction of ClONO2(g) + NaCl(s) to Cl2(g) + NaNO3(s)

The heterogeneous reaction of ClON02 + NaCl yields Cl2 + NaNO3 (eq 1) was investigated over a temperature range 220-300 K in a flow-tube reactor interfaced with a differentially pumped quadrupole mass spectrometer. Partial pressures of ClON02 in the range 10(exp -8) - 10(exp -5) Torr were used. Granule sizes and surface roughness of the NaCl substrates were determined by using a scanning electron microscope, and in separate experiments, surface areas of the substrates were measured by using BET analysis of gas-adsorption isotherms. For dry NaCl substrates, both the decay rates of ClON02 and the growth rates Of C12 were used to obtain reaction probabilities, gamma(sub l) = (4.6 +/- 3.0) x 10(exp -3) at 296 K and (6.7 +/- 3.2) x 10(exp -1) at 225 K, after considering the internal surface area, The error bars represent 1 standard deviation. The Cl2 yield based on the ClONO2 reacted was measured to be 1.0 +/- 0.2. In order to mimic the conditions encountered in the lower stratosphere, the effect of water vapor pressures between 5 x 10(exp -5) and 3 x 10(exp -4) Torr on reaction 1 was also studied. With added H20, reaction probabilities, gamma = (4.1 +/- 2.1) x 10(exp -3) at 296 K and (4.7 +/- 2.9) x 10(exp -3) at 225 K, were obtained. A trace of HOCl, the reaction product from the ClON02 + H20 yield HOCl + HN03 reaction, was observed in addition to the C12 product from reaction 1. The implications of this result for the enhancement of hydrogen chloride in the stratosphere after the El Chichon volcanic eruption and for the marine troposphere are discussed.

Timonen, Raimo S.↗
NASA NTRS1994

Heterogeneous Reactions of ClONO2, HCl, and HOCl on Liquid Sulfuric Acid Surfaces

The heterogeneous reactions of ClONO2 + H2O yields HNO3 + HOCl (1), ClONO2 + HCl yields C12 + HNO3 (2), and HOCl + HCl yields Cl2 + H2O (3) on liquid sulfuric acid surfaces have been studied using a fast flow reactor coupled to a quadrupole mass spectrometer. The main objectives of the study are to investigate: (a) the temperature dependence of these reactions at a fixed H2O partial pressure typical of the lower stratosphere (that is, by changing temperature at a constant water partial pressure, the H2SO4 content of the surfaces is also changed), (b) the relative importance or competition between reactions 1 and 2, and (c) the effect of HNO3 on the reaction probabilities due to the formation of a H2SO4/HNO3/H2O ternary system. The measurements show that all the reactions depend markedly on temperature at a fixed H2O partial pressure: they proceed efficiently at temperatures near 200 K and much slower at temperatures near 220 K. The reaction probability (gamma(sub 1)) for ClONO2 hydrolysis approaches 0.01 at temperatures below 200 K, whereas the values for gamma(sub 2) and gamma(sub 3) are on the order of a few tenths at 200 K. Although detailed mechanisms for these reactions are still unknown, the present data indicate that the competition between ClONO2 hydrolysis and ClONO2 reaction with HCl may depend on temperature (or H2SO4 Wt %): in the presence of gaseous HCl at stratospheric concentrations, reaction 2 is dominant at lower temperatures (less than 200 K), but reaction 1 becomes important at temperatures above 210 K. Furthermore, reaction probability measurements performed on the H2SO4/HNO3/ H2O ternary solutions do not exhibit noticeable deviation from those performed on the H2SO4/H2O binary system, suggesting little effect of HNO3 in sulfate aerosols on the ClONO2 and HOCl reactions with HCl. The results reveal that significant reductions in the chlorine-containing reservoir species (such as ClONO2 and HCl) can take place on stratospheric sulfate aerosols at high latitudes in winter and early spring, even at temperatures too warm for Polar Stratospheric Clouds (PSCs) to form or in regions where nucleation of PSCs is sparse. This is particularly true under elevated sulfuric acid loading, such as that after the eruption of Mt. Pinatubo. Comparisons between our results and those presently available have also been made.

Zhang, Renyi↗
NASA NTRS1993

Balloon-Borne Measurements of CLO, NO and O3 in a Volcanic Cloud: An Analysis of Heterogeneous Chemistry between 20 and 30 KM

Balloon profiles of chlorine monoxide (ClO), nitric oxide (NO), and ozone (O3) were measured on March 11, 1992 from 100 to 10 mb over Greenland (67.0 deg N, 50.6 deg W). Measurements from SAGE II indicate that the aerosol surface area in the region was enhanced by sulfur from the eruption of Mt. Pinatubo, reaching 50 times background near 20 km. Concentrations of ClO were enhanced and concentrations of NO were suppressed relative to low aerosol conditions consistent with the effects of hydrolysis of N2O5 on the surface of sulfuric acid aerosols. The data are consistent with a value of 2 x 10(exp -4) for the reaction probability of the heterogeneous hydrolysis of ClONO2, indicating a minor role for this reaction at a temperature of 220 K. At these temperatures, we find no evidence for the catastrophic loss of ozone predicted to occur under conditions of enhanced aerosol surface area.

Dessler, A. E.↗
NASA NTRS1995

Constructing Scientific Applications from Heterogeneous Resources

A new model for high-performance scientific applications in which such applications are implemented as heterogeneous distributed programs or, equivalently, meta-computations, is investigated. The specific focus of this grant was a collaborative effort with researchers at NASA and the University of Toledo to test and improve Schooner, a software interconnection system, and to explore the benefits of increased user interaction with existing scientific applications.

Schichting, Richard D.↗
NASA NTRS1998

Heterogeneity Determination and Purification of Commercial Hen Egg-White Lysozyme

Hen egg-white lysozyme (HEWL) is widely used as a model protein, although its purity has not been adequately characterized by modern biochemical techniques. We have identified and quantified the protein heterogeneities in three commercial HEWL preparations by sodium dodecyl sulfate polyacrylamide gel electrophoresis with enhanced silver staining, reversed-phase fast protein liquid chromatography (FPLC) and immunoblotting with comparison to authentic protein standards. Depending on the source, the contaminating proteins totalled 1-6%(w/w) and consisted of ovotransferrin, ovalbumin, HEWL dimers, and polypeptides with approximate M(sub r) of 39 and 18 kDa. Furthermore, we have obtained gram quantities of electrophoretically homogeneous [> 99.9%(w/w)] HEWL by single-step semi-preparative scale cation-exchange FPLC with a yield of about 50%. Parallel studies of crystal growth kinetics, salt repartitioning and crystal perfection with this highly purified material showed fourfold increases in the growth-step velocities and significant enhancement in the structural homogeneity of HEWL crystals.

Thomas, B. R.↗
NASA NTRS1996

Heterogeneous Chemistry of HONO on Liquid Sulfuric Acid: A New Mechanism of Chlorine Activation on Stratospheric Sulfate Aerosols

Heterogeneous chemistry of nitrous acid (HONO) on liquid sulfuric acid (H2SO4) Was investigated at conditions that prevail in the stratosphere. The measured uptake coefficient (gamma) of HONO on H2SO4 increased with increasing acid content, ranging from 0.03 for 65 wt % to about 0.1 for 74 wt %. In the aqueous phase, HONO underwent irreversible reaction with H2SO4 to form nitrosylsulfuric acid (NO(+)HSO4(-). At temperatures below 230 K, NO(+)HSO4(-) was observed to be stable and accumulated in concentrated solutions (less than 70 wt % H2SO4) but was unstable and quickly regenerated HONO in dilute solutions (less than 70 wt %). HCl reacted with HONO dissolved in sulfuric acid, releasing gaseous nitrosyl chloride (ClNO). The reaction probability between HCl and HONO varied from 0.01 to 0.02 for 60-72 wt % H2SO4. In the stratosphere, ClNO photodissociates rapidly to yield atomic chlorine, which catalytically destroys ozone. Analysis of the laboratory data reveals that the reaction of HCl with HONO on sulfate aerosols can affect stratospheric ozone balance during elevated sulfuric acid loadings after volcanic eruptions or due to emissions from the projected high-speed civil transport (HSCT). The present results may have important implications on the assessment of environmental acceptability of HSCT.

Zhang, Renyi↗
NASA NTRS1999

Validation of Land-Surface Mosaic Heterogeneity in the GEOS DAS

The Mosaic Land-surface Model (LSM) has been included into the current GEOS Data Assimilation System (DAS). The LSM uses a more advanced representation of physical processes than previous versions of the GEOS DAS, including the representation of sub-grid heterogeneity of the land-surface through the Mosaic approach. As a first approximation, Mosaic assumes that all similar surface types within a grid-cell can be lumped together as a single'tile'. Within one GCM grid-cell, there might be 1 - 5 different tiles or surface types. All tiles are subjected to the grid-scale forcing (radiation, air temperature and specific humidity, and precipitation), and the sub-grid variability is a function of the tile characteristics. In this paper, we validate the LSM sub-grid scale variability (tiles) using a variety of surface observing stations from the Southern Great Plains (SGP) site of the Atmospheric Radiation Measurement (ARM) Program. One of the primary goals of SGP ARM is to study the variability of atmospheric radiation within a G,CM grid-cell. Enough surface data has been collected by ARM to extend this goal to sub-grid variability of the land-surface energy and water budgets. The time period of this study is the Summer of 1998 (June I - September 1). The ARM site data consists of surface meteorology, energy flux (eddy correlation and bowen ratio), soil water observations spread over an area similar to the size of a G-CM grid-cell. Various ARM stations are described as wheat and alfalfa crops, pasture and range land. The LSM tiles considered at the grid-space (2 x 2.5) nearest the ARM site include, grassland, deciduous forests, bare soil and dwarf trees. Surface energy and water balances for each tile type are compared with observations. Furthermore, we will discuss the land-surface sub-grid variability of both the ARM observations and the DAS.

Bosilovich, Michael G.↗
NASA NTRS1999

Modeling of Sub-Grid Heterogeneity and its Impact on GCM Global Radiation Balance

The spatial and temporal variability of high, low, and mid-level clouds is obtained from ISCCP D1 data. Monthly mean global maps of the observed cloud variability are used to re-scale GCM prognostic cloud optical depths and radiative parameters via the Monte Carlo cloud heterogeneity parameterization that utilizes the existing plane-parallel GCM radiative transfer model to compute radiative fluxes for inhomogeneous cloud distributions. The GCM radiative fluxes at TOA and the ground surface are then compared to ERBE and GEBA results. These comparisons show that including sub-grid cloud variability in the GCM radiative model improves agreement between the GCM radiative energy budget components and observations,

Lacis, Andrew↗
NASA NTRS2000

Dynamic Load-Balancing for Distributed Heterogeneous Computing of Parallel CFD Problems

The developed methodology is aimed at improving the efficiency of executing block-structured algorithms on parallel, distributed, heterogeneous computers. The basic approach of these algorithms is to divide the flow domain into many sub- domains called blocks, and solve the governing equations over these blocks. Dynamic load balancing problem is defined as the efficient distribution of the blocks among the available processors over a period of several hours of computations. In environments with computers of different architecture, operating systems, CPU speed, memory size, load, and network speed, balancing the loads and managing the communication between processors becomes crucial. Load balancing software tools for mutually dependent parallel processes have been created to efficiently utilize an advanced computation environment and algorithms. These tools are dynamic in nature because of the chances in the computer environment during execution time. More recently, these tools were extended to a second operating system: NT. In this paper, the problems associated with this application will be discussed. Also, the developed algorithms were combined with the load sharing capability of LSF to efficiently utilize workstation clusters for parallel computing. Finally, results will be presented on running a NASA based code ADPAC to demonstrate the developed tools for dynamic load balancing.

Ecer, A.↗
NASA NTRS1999

Heterogeneous Clustering: Operational and User Impacts

Heterogeneous clustering can improve overall utilization of multiple hosts and can provide better turnaround to users by balancing workloads across hosts. Building a cluster requires both operational changes and revisions in user scripts.

Salm, Saita Wood↗