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At least 127 records · Page 7

Stratospheric Heterogeneous Chemistry and Microphysics: Model Development, Validation and Applications

The objectives of this project are to: define the chemical and physical processes leading to stratospheric ozone change that involve polar stratospheric clouds (PSCS) and the reactions occurring on the surfaces of PSC particles; study the formation processes, and the physical and chemical properties of PSCS, that are relevant to atmospheric chemistry and to the interpretation of field measurements taken during polar stratosphere missions; develop quantitative models describing PSC microphysics and heterogeneous chemical processes; assimilate laboratory and field data into these models; and calculate the extent of chemical processing on PSCs and the impact of specific microphysical processes on polar composition and ozone depletion. During the course of the project, a new coupled microphysics/physical-chemistry/ photochemistry model for stratospheric sulfate aerosols and nitric acid and ice PSCs was developed and applied to analyze data collected during NASA's Arctic Airborne Stratospheric Expedition-II (AASE-II) and other missions. In this model, detailed treatments of multicomponent sulfate aerosol physical chemistry, sulfate aerosol microphysics, polar stratospheric cloud microphysics, PSC ice surface chemistry, as well as homogeneous gas-phase chemistry were included for the first time. In recent studies focusing on AASE measurements, the PSC model was used to analyze specific measurements from an aircraft deployment of an aerosol impactor, FSSP, and NO(y) detector. The calculated results are in excellent agreement with observations for particle volumes as well as NO(y) concentrations, thus confirming the importance of supercooled sulfate/nitrate droplets in PSC formation. The same model has been applied to perform a statistical study of PSC properties in the Northern Hemisphere using several hundred high-latitude air parcel trajectories obtained from Goddard. The rates of ozone depletion along trajectories with different meteorological histories are presently being systematically evaluated to identify the principal relationships between ozone loss and aerosol state. Under this project, we formulated a detailed quantitative model that predicts the multicomponent composition of sulfate aerosols under stratospheric conditions, including sulfuric, nitric, hydrochloric, hydrofluoric and hydrobromic acids. This work defined for the first time the behavior of liquid ternary-system type-1b PSCS. The model also allows the compositions and reactivities of sulfate aerosols to be calculated over the entire range of environmental conditions encountered in the stratosphere (and has been incorporated into a trajectory/microphysics model-see above). Important conclusions that derived from this work over the last few years include the following: the HNO3 content of liquid-state aerosols dominate PSCs below about 195 K; the freezing of nitric acid ice from sulfate aerosol solutions is likely to occur within a few degrees K of the water vapor frost point; the uptake and reactions of HCl in liquid aerosols is a critical component of PSC heterogeneous chemistry. In a related application of this work, the inefficiency of chlorine injection into the stratosphere during major volcanic eruptions was explained on the basis of nucleation of sulfuric acid aerosols in rising volcanic plumes leading to the formation of supercooled water droplets on these aerosols, which efficiently scavenges HCl via precipitation.

Turco, Richard P.↗

Heterogeneous Combustion of Porous Graphite Particles in Normal and Microgravity

Combustion of solid fuel particles has many important applications, including power generation and space propulsion systems. The current models available for describing the combustion process of these particles, especially porous solid particles, include various simplifying approximations. One of the most limiting approximations is the lumping of the physical properties of the porous fuel with the heterogeneous chemical reaction rate constants. The primary objective of the present work is to develop a rigorous model that could decouple such physical and chemical effects from the global heterogeneous reaction rates. For the purpose of validating this model, experiments with porous graphite particles of varying sizes and porosity are being performed at NASA Lewis Research Center. The details of the experimental and theoretical model development effort are described.

Chelliah, Harsha↗

Sulfuric Acid Monohydrate: Formation and Heterogeneous Chemistry in the Stratosphere

We have investigated some thermodynamic properties (i.e., freezing/melting points) and heterogeneous chemistry of sulfuric acid monohydrate (SAM, H2SO4.H2O), using a fast flow reactor coupled to a quadrupole mass spectrometer. The freezing point observations of thin liquid sulfuric acid films show that for acid contents between 75 and 85 wt % the monohydrate crystallizes readily at temperatures between 220 and 240 K on a glass substrate. Once formed, SAM can be thermodynamically stable in the H2O partial pressure range of (1-4) x 10(exp -4) torr and in the temperature range of 220-240 K. For a constant H2O partial pressure, lowering the temperature causes SAM to melt when the temperature and water partial pressure conditions are out of its stability regime. The reaction probability measurements indicate that the hydrolysis of N2O5 is significantly suppressed owing to the formation of crystalline SAM: The reaction probability on water-rich SAM (with higher relative humidity, or RH) is of the order of 10(exp -3) at 210 K and decreases by more than an order of magnitude for the acid-rich form (with lower RH). The hydrolysis rate of ClONO2 on water-rich SAM is even smaller, of the order of 10(exp -4) at 195 K. These reported values on crystalline SAM are much smaller than those on liquid solutions. No enhancement of these reactions is observed in the presence of HCl vapor at the stratospheric concentrations. In addition, Brunauer, Emmett, and Teller analysis of gas adsorption isotherms and photomicrography have been performed to characterize the surface roughness and porosities of the SAM substrate. The results suggest the possible formation of SAM in some regions of the middle- or low-latitude stratosphere and, consequently, much slower heterogeneous reactions on the frozen aerosols.

Zhang, Renyi↗

Heterogeneous reactions of HNO3(g) + NaCl(s) yields HCl(g) + NaNO3(s) and N2O5(g) + NaCl(s) yields ClNO2(g) + NaNO3(s)

The heterogeneous reactions of HNO3(g) + NaCl(s) yields HCl(g) + NaNO3(s) (eq 1) and N2O5(g) + NaCl(s) yields ClNO2(g) + NaNO3(S) (eq 2) were investigated over the temperature range 223-296 K in a flow-tube reactor coupled to a quadrupole mass spectrometer. Either a chemical ionization mass spectrometer (CIMS) or an electron-impact ionization mass spectrometer (EIMS) was used to provide suitable detection sensitivity and selectivity. In order to mimic atmospheric conditions, partial pressures of HNO3 and N2O5 in the range 6 x 10(exp -8) - 2 x 10(exp -6) Torr were used. Granule sizes and surface roughness of the solid NaCl substrates were determined by using a scanning electron microscope. For dry NaCl substrates, decay rates of HNO3 were used to obtain gamma(1) = 0.013 +/- 0.004 (1sigma) at 296 K and > 0.008 at 223 K, respectively. The error quoted is the statistical error. After all corrections were made, the overall error, including systematic error, was estimated to be about a factor of 2. HCl was found to be the sole gas-phase product of reaction 1. The mechanism changed from heterogeneous reaction to predominantly physical adsorption when the reactor was cooled from 296 to 223 K. For reaction 2 using dry salts, gamma(2) was found to be less than 1.0 x 10(exp -4) at both 223 and 296 K. The gas-phase reaction product was identified as ClNO2 in previous studies using an infrared spectrometer. An enhancement in reaction probability was observed if water was not completely removed from salt surfaces, probably due to the reaction of N2O5(g) + H2O(s) yields 2HNO3(g). Our results are compared with previous literature values obtained using different experimental techniques and conditions. The implications of the present results for the enhancement of the hydrogen chloride column density in the lower stratosphere after the El Chichon volcanic eruption and for the chemistry of HCl and HNO3 in the marine troposphere are discussed.

Leu, Ming-Taun↗

Enstatite Meteorites and the Original Heterogeneity of Mn-53 Distribution in the Solar Nebula

We have shown earlier that the relative abundance of radiogenic Cr-53 in bulk ordinary chondrites (approximately 0.48 epsilon) is clearly different from that in the earth-moon system (0 epsilon). The SNC parent body (Mars) is characterized by an intermediate Cr-53 excess (approximately 0.23 epsilon). We have also shown that the Mn-Cr systematics of the howardite-eucrite-diogenite parent body (HED PB, the asteroid Vesta) is consistent with the chondritic Mn/Cr ratio in the bulk HED PB and that it has a Cr-53 excess of approximately 0.5 epsilon units which is within error the same as that of chondrites. It appears that the excesses of Cr-53 in these planets are a function of their present heliocentric distance. The study of some other meteorite classes (angrites, pallasites, primitive achondrites) has shown that their Mn-CR systematics is consistent with that of the ordinary chondrites. The observed gradient in the radiogenic Cr-53 abundances can be explained by a). an early volatility controlled radial Mn/Cr fractionation in the nebula or b). an original heterogeneity of Mn-53. The first assumption, however, requires the Mn/Cr ratios of the bulk Earth and Mars to be considerably lower than the inferred model Mn/Cr ratios for these two planets. For this reason, we suggested that the observed gradient is due to an original radial Mn-53 heterogeneity in the late nebula.

Lugmair, Guenter W.↗

The Influence of Particle Charge on Heterogeneous Reaction Rate Coefficients

The effects of particle charge on heterogeneous reaction rates are presented. Many atmospheric particles, whether liquid or solid are charged. This surface charge causes a redistribution of charge within a liquid particle and as a consequence a perturbation in the gaseous uptake coefficient. The amount of perturbation is proportional to the external potential and the square of the ratio of debye length in the liquid to the particle radius. Previous modeling has shown how surface charge affects the uptake coefficient of charged aerosols. This effect is now included in the heterogeneous reaction rate of an aerosol ensemble. Extension of this analysis to ice particles will be discussed and examples presented.

Aikin, A. C.↗

Heterogeneous Integration, An Approach to High Density and High Flexibility Electronic Packaging

Key to the design of spacecraft for exploration of the outer planets will be the development of highly integrated and mass/volume efficient electronic systems. Exploration of the outer planets will require optimized propulsion approaches which mandates mass minimization. If one looks at a mission such as the Europa Lander, a high mass/volume efficiency feeds back directly into lower mass for radiation shielding. Concurrently the long mission lengths will drive the need for fault isolation and fault tolerance. The ability to build distributed electronic systems is an inherent requirement and one which is enabled by heterogeneous integration. The electronic packaging approach must be capable of interconnecting various components at a scale comparable with that on the components themselves (chip scale) and it must facilitate efficient integration of the electronics with elements of the spacecraft such as structure or antennae. The concept of 'Heterogeneous Integration' is being explored in the System On A Chip (SOAC) Project at JPL. The goal, of this approach to electronic packaging, is to enable the fabrication and assembly of complete electronic subsystems from components fabricated by a range of processes. Included in such a system could be MEMS sensors, SOI mixed signal ASICs, micro scale passive components and micro power. Secondarily the compact size will enable distributed architectures and integrated assemblies. Additional information is contained in the original extended abstract.

DAgostino, S. A.↗

Heterogenous Combustion of Porous Graphite Particles in Normal and Microgravity

Combustion of solid fuel particles has many important applications, including power generation and space propulsion systems. The current models available for describing the combustion process of these particles, especially porous solid particles, include various simplifying approximations. One of the most limiting approximations is the lumping of the physical properties of the porous fuel with the heterogeneous chemical reaction rate constants. The primary objective of the present work is to develop a rigorous model that could decouple such physical and chemical effects from the global heterogeneous reaction rates. For the purpose of validating this model, experiments with porous graphite particles of varying sizes and porosity are being performed. The details of this experimental and theoretical model development effort are described.

Chelliah, Harsha K.↗

Laboratory Studies of Heterogeneous Chemical Processes of Atmospheric Importance

The objective of this study is to conduct measurements of chemical kinetics parameters for heterogeneous reactions of importance in the stratosphere and the troposphere. It involves the elucidation of the mechanism of the interaction of HC1 vapor with ice surfaces, which is the first step in the heterogeneous chlorine activation processes, as well as the investigation of the atmospheric oxidation mechanism of soot particles emitted by biomass and fossil fuels. The techniques being employed include turbulent flow- chemical ionization mass spectrometry and optical ellipsometry, among others. The next section summarizes our research activities during the first year of the project, and the section that follows consists of the statement of work for the second year.

Molina, Mario J.↗

Laboratory Studies of Heterogeneous Chemical Processes of Atmospheric Importance

The objective of this study is to conduct measurements of chemical kinetics parameters for heterogeneous reactions of importance in the stratosphere and the troposphere. It involves the elucidation of the mechanism of the interaction of HCl vapor with ice surfaces, which is the first step in the heterogeneous chlorine activation processes, as well as the investigation of the atmospheric oxidation mechanism of soot particles emitted by biomass and fossil fuels. The techniques being employed include turbulent flow-chemical ionization mass spectrometry and optical ellipsometry, among others.

Molina, Mario J.↗

Heterogeneous Superconducting Low-Noise Sensing Coils

A heterogeneous material construction has been devised for sensing coils of superconducting quantum interference device (SQUID) magnetometers that are subject to a combination of requirements peculiar to some advanced applications, notably including low-field magnetic resonance imaging for medical diagnosis. The requirements in question are the following: The sensing coils must be large enough (in some cases having dimensions of as much as tens of centimeters) to afford adequate sensitivity; The sensing coils must be made electrically superconductive to eliminate Johnson noise (thermally induced noise proportional to electrical resistance); and Although the sensing coils must be cooled to below their superconducting- transition temperatures with sufficient cooling power to overcome moderate ambient radiative heat leakage, they must not be immersed in cryogenic liquid baths. For a given superconducting sensing coil, this combination of requirements can be satisfied by providing a sufficiently thermally conductive link between the coil and a cold source. However, the superconducting coil material is not suitable as such a link because electrically superconductive materials are typically poor thermal conductors. The heterogeneous material construction makes it possible to solve both the electrical- and thermal-conductivity problems. The basic idea is to construct the coil as a skeleton made of a highly thermally conductive material (typically, annealed copper), then coat the skeleton with an electrically superconductive alloy (typically, a lead-tin solder) [see figure]. In operation, the copper skeleton provides the required thermally conductive connection to the cold source, while the electrically superconductive coating material shields against Johnson noise that originates in the copper skeleton.

Hahn, Inseob↗

Influence of Satellite-Based Heterogeneous Vegetation Momentum Roughness on Mesoscale Model Dynamics During IHOP 2002

The sensitivity of mesoscale weather prediction model to a vegetation roughness initialization is investigated for the south central United States. Three different roughness databases are employed: i) a control or standard lookup table roughness that is a function only of land cover type, ii) a spatially heterogeneous roughness database previously derived using a physically based procedure and MODIS imagery, and iii) a MODIS climatologic roughness database that possesses the same spatial heterogeneity as (i) but with mean land class values from (ii). The model used is the Weather Research and Forecast Model (WRF) coupled to the Community Land Model within the Land Information System (LIS). For each simulation, a statistical comparison is made between modeled results and ground observations from meteorological stations within the Oklahoma mesonet and surrounding region during IHOP20O2. A sensitivity analysis on the impact the MODIS-based roughness fields is also made through a time-series intercomparison of temperature bias, probability of detection (POD), average wind speed, boundary layer height, and turbulent kinetic energy (TKE) the results that, for the current replacement of the standard land-cover type based roughness values with the satellite-derived fields statistically improves model performance for most of the observed variables. Further, the satellite-based roughness enhances the surface wind speed, PBL height and TKE production on the order of 3 to l0 percent, with a lesser effect over grassland and cropland domains, and the greater effect over mixed land cover domains

Jasinski, Michael↗

Issues and Solutions for Bringing Heterogeneous Water Cycle Data Sets Together

The water cycle research community has generated many regional to global scale products using data from individual NASA missions or sensors (e.g., TRMM, AMSR-E); multiple ground- and space-based data sources (e.g., Global Precipitation Climatology Project [GPCP] products); and sophisticated data assimilation systems (e.g., Land Data Assimilation Systems [LDAS]). However, it is often difficult to access, explore, merge, analyze, and inter-compare these data in a coherent manner due to issues of data resolution, format, and structure. These difficulties were substantiated at the recent Collaborative Energy and Water Cycle Information Services (CEWIS) Workshop, where members of the NASA Energy and Water cycle Study (NEWS) community gave presentations, provided feedback, and developed scenarios which illustrated the difficulties and techniques for bringing together heterogeneous datasets. This presentation reports on the findings of the workshop, thus defining the problems and challenges of multi-dataset research. In addition, the CEWIS prototype shown at the workshop will be presented to illustrate new technologies that can mitigate data access roadblocks encountered in multi-dataset research, including: (1) Quick and easy search and access of selected NEWS data sets. (2) Multi-parameter data subsetting, manipulation, analysis, and display tools. (3) Access to input and derived water cycle data (data lineage). It is hoped that this presentation will encourage community discussion and feedback on heterogeneous data analysis scenarios, issues, and remedies.

Acker, James↗

Numerical Model Sensitivity to Heterogeneous Satellite Derived Vegetation Roughness

The sensitivity of a mesoscale weather prediction model to a 1 km satellite-based vegetation roughness initialization is investigated for a domain within the south central United States. Three different roughness databases are employed: i) a control or standard lookup table roughness that is a function only of land cover type, ii) a spatially heterogeneous roughness database, specific to the domain, that was previously derived using a physically based procedure and Moderate Resolution Imaging Spectroradiometer (MODIS) imagery, and iii) a MODIS climatologic roughness database that like (i) is a function only of land cover type, but possesses domain specific mean values from (ii). The model used is the Weather Research and Forecast Model (WRF) coupled to the Community Land Model within the Land Information System (LIS). For each simulation, a statistical comparison is made between modeled results and ground observations within a domain including Oklahoma, Eastern Arkansas, and Northwest Louisiana during a 4-day period within IHOP 2002. Sensitivity analysis compares the impact the three roughness initializations on time-series temperature, precipitation probability of detection (POD), average wind speed, boundary layer height, and turbulent kinetic energy (TKE). Overall, the results indicate that, for the current investigation, replacement of the standard look-up table values with the satellite-derived values statistically improves model performance for most observed variables. Such natural roughness heterogeneity enhances the surface wind speed, PBL height and TKE production up to 10 percent, with a lesser effect over grassland, and greater effect over mixed land cover domains.

Jasinski, Michael↗

Radiative Impacts of Cloud Heterogeneity and Overlap in an Atmospheric General Circulation Model

The radiative impacts of introducing horizontal heterogeneity of layer cloud condensate, and vertical overlap of condensate and cloud fraction are examined with the aid of a new radiation package operating in the GEOS-5 Atmospheric General Circulation Model. The impacts are examined in terms of diagnostic top-of-the-atmosphere shortwave (SW) and longwave (LW) cloud radiative effect (CRE) calculations for a range of assumptions and parameter specifications about the overlap. The investigation is conducted for two distinct cloud schemes, the one that comes with the standard GEOS-5 distribution, and another which has been recently used experimentally for its enhanced GEOS-5 distribution, and another which has been recently used experimentally for its enhanced cloud microphysical capabilities; both are coupled to a cloud generator allowing arbitrary cloud overlap specification. We find that cloud overlap radiative impacts are significantly stronger for the operational cloud scheme for which a change of cloud fraction overlap from maximum-random to generalized results to global changes of SW and LW CRE of approximately 4 Watts per square meter, and zonal changes of up to approximately 10 Watts per square meter. This is because of fewer occurrences compared to the other scheme of large layer cloud fractions and of multi-layer situations with large numbers of atmospheric being simultaneously cloudy, conditions that make overlap details more important. The impact on CRE of the details of condensate distribution overlap is much weaker. Once generalized overlap is adopted, both cloud schemes are only modestly sensitive to the exact values of the overlap parameters. We also find that if one of the CRE components is overestimated and the other underestimated, both cannot be driven towards observed values by adjustments to cloud condensate heterogeneity and overlap alone.

Oreopoulos, L.↗

Heterogeneous Formation of Polar Stratospheric Clouds- Part 1: Nucleation of Nitric Acid Trihydrate (NAT)

Satellite-based observations during the Arctic winter of 2009/2010 provide firm evidence that, in contrast to the current understanding, the nucleation of nitric acid trihydrate (NAT) in the polar stratosphere does not only occur on preexisting ice particles. In order to explain the NAT clouds observed over the Arctic in mid-December 2009, a heterogeneous nucleation mechanism is required, occurring via immersion freezing on the surface of solid particles, likely of meteoritic origin. For the first time, a detailed microphysical modelling of this NAT formation pathway has been carried out. Heterogeneous NAT formation was calculated along more than sixty thousand trajectories, ending at Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) observation points. Comparing the optical properties of the modelled NAT with these observations enabled a thorough validation of a newly developed NAT nucleation parameterisation, which has been built into the Zurich Optical and Microphysical box Model (ZOMM). The parameterisation is based on active site theory, is simple to implement in models and provides substantial advantages over previous approaches which involved a constant rate of NAT nucleation in a given volume of air. It is shown that the new method is capable of reproducing observed polar stratospheric clouds (PSCs) very well, despite the varied conditions experienced by air parcels travelling along the different trajectories. In a companion paper, ZOMM is applied to a later period of the winter, when ice PSCs are also present, and it is shown that the observed PSCs are also represented extremely well under these conditions.

Hoyle, C. R.↗

Heterogeneity of Water Concentrations in the Mantle Lithosphere Beneath Hawaii

The amount and distribution of water in the oceanic mantle lithosphere has implications on its strength and of the role of volatiles during plume/lithosphere interaction. The latter plays a role in the Earth's deep water cycle as water-rich plume lavas could re-enrich an oceanic lithosphere depleted in water at the ridge, and when this heterogeneous lithosphere gets recycled back into the deep mantle. The main host of water in mantle lithologies are nominally anhydrous minerals like olivine, pyroxene and garnet, where hydrogen (H) is incorporated in mineral defects by bonding to structural oxygen. Here, we report water concentrations by Fourier transform infrared spectrometry (FTIR) on olivine, clino- and orthopyroxenes (Cpx & Opx) from spinel peridotites from the Pali vent and garnet pyroxenite xenoliths from Aliamanu vent, both part of the rejuvenated volcanism at Oahu (Hawaii). Pyroxenes from the Aliamanu pyroxenites have high water concentrations, similar to the adjacent Salt Lake Crater (SLC) pyroxenites (Cpx ~400-500 ppm H2O, Opx ~200 ppm H2O). This confirms that pyroxenite cumulates form water-rich lithologies within the oceanic lithosphere. In contrast, the Pali peridotites have much lower water concentrations than the SLC ones (<25 ppm vs. 50-96 ppm H2O respectively) despite being relatively fertile with >10% modal Cpx and low spinel Cr# (0.09-0.10). The contrast between the two peridotite suites is also evident in their trace elements and radiogenic isotopes. The Pali Cpx are depleted in light REE, consistent with minimal metasomatism. Those of SLC have enriched light REE patterns and Nd and Hf isotopes consistent with metasomatism by alkaline melts. These observations are consistent with heterogeneous water distribution in the oceanic lithosphere that may be related to metasomatism, as well as relatively dry peridotites cross-cut by narrow (?) water-rich melt reaction zones.

Bizimis, M.↗

Heterogeneous Spacecraft Networks

The present invention provides a heterogeneous spacecraft network including a network management architecture to facilitate communication between a plurality of operations centers and a plurality of data user communities. The network management architecture includes a plurality of network nodes in communication with the plurality of operations centers. The present invention also provides a method of communication for a heterogeneous spacecraft network. The method includes: transmitting data from a first space segment to a first ground segment; transmitting the data from the first ground segment to a network management architecture; transmitting data from a second space segment to a second ground segment, the second space and ground segments having incompatible communication systems with the first space and ground segments; transmitting the data from the second ground station to the network management architecture; and, transmitting data from the network management architecture to a plurality of data user communities.

Nakamura, Yosuke↗