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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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NASA NTRS1994

H2O-H2SO4 system in Venus' clouds and OCS, CO, and H2SO4 profiles in Venus' troposphere

A coupled problem of diffusion and condensation is solved for the H2SO4-H2O system in Venus' cloud layer. The position of the lower cloud boundary and profiles of the H2O and H2SO4 vapor mixing ratios and of the H2O/H2SO4 ratio of sulfuric acid aerosol and its flux are calculated as functions of the column photochemical production rate of sulfuric acid, Phi(sub H2SO4). Variations of the lower cloud boundary are considered. Our basic model, which is constrained to yield f(sub H2O) (30 km) = 30 ppm (Pollack et al. 1993), predicts the position of the lower cloud boundary at 48.4 km coinciding with the mean Pioneer Venus value, the peak H2SO4 mixing ratio of 5.4 ppm, and the H2SO4 production rate Phi(sub H2SO4) = 2.2 x 10(exp 12)/sq cm/s. The sulfur to sulfuric acid mass flux ratio in the clouds is 1:27 in this model, and the mass loading ratio may be larger than this value if sulfur particles are smaller than those of sulfuric acid. The model suggests that the extinction coefficient of sulfuric acid particles with radius 3.7 micrometers (mode 3) is equal to 0.3/km in the middle cloud layer. The downward flux of CO is equal to 1.7 x 10(exp 12)/sq cm/s in this model. Our second model, which is constrained to yield f(sub H2O) = 10 ppm at the lower cloud boundary, close to the value measured by the Magellan radiooccultations, predicts the position of this boundary to be at 46.5 km, which agrees with the Magellan data; f(sub H2O) (30 km) = 90 ppm, close to the data of Moroz et al. (1983) at this altitude; Phi(sub H2SO4) = 6.4 x 10(exp 12)/sq cm/s; and Phi(sub co) = 4.2 x 10(exp 12)/sq cm/s. The S/H2SO4 flux mass ratio is 1:18, and the extinction coefficient of the mode 3 sulfuric acid particles is equal to 0.9 km in the middle cloud layer. A strong gradient of the H2SO4 vapor mixing ratio near the bottom of the cloud layer drives a large upward flux of H2SO4, which condenses and forms the excessive downward flux of liquid sulfuric acid, which is larger by a factor of 4-7 than the flux in the middle cloud layer. This is the mechanism of formation of the lower cloud layer. Variations of the lower cloud layer are discussed. Our modeling of the OCS and CO profiles in the lower atmosphere measured by Pollack et al. (1993) provides a reasonable explanation of these data and shows that the rate coefficient of the reaction SO3 + CO yields CO2 + SO2 is equal to 10(exp -11) exp(-(13,100 +/- 1000)/T) cc/s. The main channel of the reaction between SO3 and OCS is CO2 + (SO)2, and its rate coefficient is equal to 10(exp -11) exp(-(8900 +/- 500)/T) cc/s. In the conditions of Venus' lower atmosphere, (SO)2 is removed by the reaction (SO)2 + OCS yields CO + S2 + SO2. The model predicts an OCS mixing ratio of 28 ppm near the surface.

Krasnopolsky, V. A.↗
NASA NTRS2015

Volcanic Aerosol Radiative Properties

Large sporadic volcanic eruptions inject large amounts of sulfur bearing gases into the stratosphere which then get photochemically converted to sulfuric acid aerosol droplets that exert a radiative cooling effect on the global climate system lasting for several years.

Stratosphere↗
NASA NTRS1978

Planetary isophotes as a clue to aerosol characteristics. II - Observations of Venus from spacecraft

Contrary to published reports, the limb-darkening observed by Mariner 10 is consistent with the sulfuric-acid aerosol scattering that explains the polarization and spectroscopic features of Venus. A combination of both geometric and photometric systematic errors explains the previously reported discrepancy. Although the aerosol model cannot be distinguished from isotropic scattering at the Mariner 10 phase angle, Venera 9 data at larger phases clearly favor the aerosol model. There is no evidence for isotropic scattering in the clouds of Venus.

Young, A. T.↗
NASA NTRS1979

Oxides of nitrogen and the clouds of Venus

Nitric oxide may be produced in the atmosphere of Venus by lightning storms in the clouds. The paper suggests that the odd nitrogen thus formed may play an important part in the chemistry of the clouds. Specifically, production rates for NO2 in the limiting case of high NO concentrations are estimated. If the NO density is high, it is suggested that NO2 may catalyse the production of sulfuric acid aerosol from sulfur dioxide and water vapor, and may also form nitrogen-sulfur compounds such as nitrosyl sulfuric acid, NOHSO4. The large partricles seen by the Pioneer Venus sounder probe may contain considerable quantities of NOHSO4. If this is the case, odd nitrogen must be present in the atmosphere in at least a parts-per-million mixing ratio.

Watson, A. J.↗
NASA NTRS1992

The potential effects of volcanic aerosols on cirrus cloud microphysics

The potential impact of volcanic aerosols on nucleation of ice crystals in upper tropospheric cirrus clouds is examined from a microphysical perspective. The sulfuric acid aerosols which form in the stratosphere are presumably transported into the troposphere by sedimentation and tropopause folding. The tropospheric volcanic aerosol size distribution is estimated from 10-micron lidar backscatter and in situ measurements. Microphysical simulations suggest that at temperatures below about -50 C the concentration of ice crystals which nucleate may be as much as a factor of 5 larger when volcanic aerosols are present. The simulations suggest that the presence of volcanic aerosols may increase the net radiative forcing (surface warming) of certain types of cirrus near the tropopause by as much as 8 W/sq m. Further observations are required to determine whether these effects actually occur, and their global impact.

Jensen, Eric J.↗
NASA NTRS1994

Biospheric effects of a large extraterrestrial impact: Case study of the Cretaceous/Tertiary boundary crater

The Chicxulub Crater in Yucatan, Mexico, is the primary candidate for the impact that caused mass extinctions at the Cretaceous/Tertiary boundary. The target rocks at Chicxulub contain 750 to 1500 m of anhydrite (CaSO4), which was vaporized upon impact, creating a large sulfuric acid aerosol cloud. In this study we apply a hydrocode model of asteroid impact to calculate the amount of sulfuric acid produced. We then apply a radiative transfer model to determine the atmospheric effects. Results include 6 to 9 month period of darkness followed by 12 to 26 years of cooling.

Pope, Kevin O.↗
NASA NTRS1984

The photochemistry of a remote marine stratiform cloud

The coupled gas- and aqueous-phase photochemistry of a stratiform cloud in a remote region of the marine atmosphere is investigated with a time-dependent box model. Both scavenging of ambient acidic aerosols and gases as well as aqueous-phase chemical reactions within droplets are found to be important sources of acidity to cloud water and can lead to pH levels in cloud water in the remote marine atmosphere well below 5.6. The major sources of acidity via aqueous-phase chemical reactions are the generation of sulfuric acid from dissolved SO2 and the generation of formic acid from dissolved formaldehyde. In both cases, aqueous-phase free radicals can play a significant role either directly by oxidizing dissolved SO2 and HCHO or indirectly by producing the aqueous-phase oxidant H2O2. The rate of SO2 conversion to sulfuric acid is sensitive to a variety of parameters including the accommodation or sticking coefficient for SO2, H2O2, HO2, and OH, the liquid water content, and the ambient levels of SO2, HNO3, and other acidic or basic gases. Because high levels of SO2 tend to deplete cloud water of H2O3, the possibility exists that the pH of precipitation in polluted regions will respond nonlinearly to reduced SO2 emissions.

Chameides, W. L.↗
NASA NTRS1994

Ozone within the El Chichon aerosol cloud inferred from solar backscatter ultraviolet continuous-scan measurements

Large amounts of SO2 injected into the stratosphere by the El Chichon volcanic eruption greatly enhanced the sulfuric acid aerosol loading. According to laboratory studies, the increase in aerosol surface area would lead to a loss of ozone. Radiation measurements from the solar backscatter ultraviolet spectroradiometer are used to probe the absorbing and scattering properties of the stratosphere after the eruption. The backscattered radiation is enhanced for wavelengths greater than 290 nm, with a peak at about 302 nm. The enhancements associated with aerosol backscattering and ozone change can be separated. A decrease in column ozone of 8 to 30 Dobson units was deduced within the aerosol layer at an altitude between 20 and 30 km following the month of the eruption.

Wen, Guoyong↗
NASA NTRS1999

Instrumentation Working Group Summary

The Instrumentation Working Group compiled a summary of measurement techniques applicable to gas turbine engine aerosol precursors and particulates. An assessment was made of the limits, accuracy, applicability, and technology readiness of the various techniques. Despite advances made in emissions characterization of aircraft engines, uncertainties still exist in the mechanisms by which aerosols and particulates are produced in the near-field engine exhaust. To adequately assess current understanding of the formation of sulfuric acid aerosols in the exhaust plumes of gas turbine engines, measurements are required to determine the degree and importance of sulfur oxidation in the turbine and at the engine exit. Ideally, concentrations of all sulfur species would be acquired, with emphasis on SO2 and SO3. Numerous options exist for extractive and non-extractive measurement of SO2 at the engine exit, most of which are well developed. SO2 measurements should be performed first to place an upper bound on the percentage of SO2 oxidation. If extractive and non-extractive techniques indicate that a large amount of the fuel sulfur is not detected as SO2, then efforts are needed to improve techniques for SO3 measurements. Additional work will be required to account for the fuel sulfur in the engine exhaust. Chemical Ionization Mass Spectrometry (CI-MS) measurements need to be pursued, although a careful assessment needs to be made of the sampling line impact on the extracted sample composition. Efforts should also be placed on implementing non-intrusive techniques and extending their capabilities by maximizing exhaust coverage for line-of-sight measurements, as well as development of 2-D techniques, where feasible. Recommendations were made to continue engine exit and combustor measurements of particulates. Particulate measurements should include particle size distribution, mass fraction, hydration properties, and volatile fraction. However, methods to ensure that unaltered samples are obtained need to be developed. Particulate speciation was also assigned a high priority for quantifying the fractions of carbon soot, PAH, refractory materials, metals, sulfates, and nitrates. High priority was also placed on performing a comparison of particle sizing instruments. Concern was expressed by the workshop attendees who routinely make particulate measurements about the variation in number density measured during in-flight tests by different instruments. In some cases, measurements performed by different groups of researchers during the same flight tests showed an order of magnitude variation. Second priority was assigned to measuring concentrations of odd hydrogen and oxidizing species. Since OH, HO2, H2O2, and O are extremely reactive, non-extractive measurements are recommended. A combination of absorption and fluorescence is anticipated to be effective for OH measurements in the combustor and at the engine exit. Extractive measurements of HO2 have been made in the stratosphere, where the ambient level of OH is relatively low. Use of techniques that convert HO2 to OH for combustor and engine exit measurements needs to be evaluated, since the ratio of HO2/OH may be 1% or less at both the combustor and engine exit. CI-MS might be a viable option for H2O2, subject to sampling line conversion issues. However, H2O2 is a low priority oxidizing species in the combustor and at the engine exit. Two candidates for atomic oxygen measurements are Resonance Enhanced Multi-Photon Ionization (REMPI) and Laser-Induced Fluorescence (LIF). Particulate measurement by simultaneous extractive and non-extractive techniques was given equal priority to the oxidizer measurements. Concern was expressed over the ability of typical ground test sampling lines to deliver an unaltered sample to a remotely located instrument. It was suggested that the sampling probe and line losses be checked out by attempting measurements using an optical or non-extractive technique immediately upstream of the sampling probe. This is a possible application for Laser Induced Incandescence (LII) as a check on the volume fraction of soot. Optical measurements of size distribution are not well developed for ultrafine particles less than about 20 nm in diameter, so a non-extractive technique for particulate size distribution cannot be recommended without further development. Carbon dioxide measurements need to be made to complement other extractive measurement techniques. CO2 measurements enable conversion of other species concentrations to emission indices. Carbon monoxide, which acts as a sink for oxidizing species, should be measured using non-extractive techniques. CO can be rapidly converted to CO2 in extractive probes, and a comparison between extractive and non-extractive measurements should be performed. Development of non-extractive techniques would help to assess the degree of CO conversion, and might be needed to improve the concentration measurement accuracy. Measurements of NO(x) will continue to be critical due to the role of NO and NO2 in atmospheric chemistry, and their influence on atmospheric ozone. Time-resolved measurements of temperature, velocity, and species concentrations were included on the list of desired measurement. Thermocouples are typically adequate for engine exit measurements. PIV and LDV are well established for obtaining velocity profiles. The techniques are listed in the accompanying table; are divided into extractive and non-extractive techniques. Efforts were made to include a measurement uncertainty for each technique. An assessment of the technology readiness was included.

Zaller, Michelle↗
NASA NTRS2021

Evidence for the predictability of changes in the stratosphericaerosol size following volcanic eruptions of diverse magnitudesusing space-based instruments

An analysis of multiwavelength stratospheric aerosol extinction coefficient data from the Stratospheric Aerosol and Gas Experiment II and III/ISS instruments is used to demonstrate a coherent relationship between the perturbation in extinction coefficient in an eruption’s main aerosol layer and the wavelength dependence of that perturbation. This relationship spans multiple orders of magnitude in the aerosol extinction coefficient of stratospheric impact of volcanic events. The relationship is measurement-based and does not rely on assumptions about the aerosol size distribution. We note limitations on this analysis including that the presence of significant amounts of ash in the main sulfuric acid aerosol layer and other factors may significantly modulate these results. Despite these limitations, the findings suggest an avenue for improving aerosol extinction coefficient measurements from single-channel observations such as the Optical Spectrograph and Infrared Imager System as they rely on a prior assumptions about particle size. They may also represent a distinct avenue for the comparison of observations with interactive aerosol models used in global climate models and Earth system models.

Larry W Thomason↗
NASA NTRS1981

Implications of stratospheric aerosol measurements for models of aerosol formation and evolution

Calculations of the distribution of stratospheric sulfur gases and of stratospheric aerosols are compared with measurements obtained in Alaska during July 1979. Generally, the measurements are reasonably consistent with the model results. COS is the major sulfur-bearing gas in the stratosphere while CS2 plays a lesser role in the formation of sulfate aerosols. Ammonia, which earlier measurements suggested was a major aerosol constituent, is found to be a contaminant, so models without ammonia chemistry may be justified. The model and the measurements suggest that stratospheric sulfuric acid aerosols nucleate just above the tropopause, but they are older and have grown to larger sizes at higher altitudes.

Toon, O. B.↗
NASA NTRS1998

Modeling Macro- and Micro-Scale Turbulent Mixing and Chemistry in Engine Exhaust Plumes

Simulation of turbulent mixing and chemical processes in the near-field plume and plume-vortex regimes has been successfully carried out recently using a reduced gas phase kinetics mechanism which substantially decreased the computational cost. A detailed mechanism including gas phase HOx, NOx, and SOx chemistry between the aircraft exhaust and the ambient air in near-field aircraft plumes is compiled. A reduced mechanism capturing the major chemical pathways is developed. Predictions by the reduced mechanism are found to be in good agreement with those by the detailed mechanism. With the reduced chemistry, the computer CPU time is saved by a factor of more than 3.5 for the near-field plume modeling. Distributions of major chemical species are obtained and analyzed. The computed sensitivities of major species with respect to reaction step are deduced for identification of the dominant gas phase kinetic reaction pathways in the jet plume. Both the near field plume and the plume-vortex regimes were investigated using advanced mixing models. In the near field, a stand-alone mixing model was used to investigate the impact of turbulent mixing on the micro- and macro-scale mixing processes using a reduced reaction kinetics model. The plume-vortex regime was simulated using a large-eddy simulation model. Vortex plume behind Boeing 737 and 747 aircraft was simulated along with relevant kinetics. Many features of the computed flow field show reasonable agreement with data. The entrainment of the engine plumes into the wing tip vortices and also the partial detrainment of the plume were numerically captured. The impact of fluid mechanics on the chemical processes was also studied. Results show that there are significant differences between spatial and temporal simulations especially in the predicted SO3 concentrations. This has important implications for the prediction of sulfuric acid aerosols in the wake and may partly explain the discrepancy between past numerical studies (that employed parabolic or temporal approximations) and the measured data. Finally to address the major uncertainty in the near-field plume modeling related to the plume processing of sulfur compounds and advanced model was developed to evaluate its impact on the chemical processes in the near wake. A comprehensive aerosol model is developed and it is coupled with chemical kinetics and the axisymmetric turbulent jet flow models. The integrated model is used to simulate microphysical processes in the near-field jet plume, including sulfuric acid and water binary homogeneous nucleation, coagulation, non-equilibrium heteromolecular condensation, and sulfur-induced soot activation. The formation and evolution of aerosols are computed and analyzed. The computed results show that a large number of ultra-fine (0.3--0.6 nm in radius) volatile HSO4 - HO embryos are generated in the near-field plume. These embryos further grow in size by self coagulation and condensation. Soot particles can be activated by both heterogeneous nucleation and scavenging of H2SO4-H2O aerosols. These activated soot particles can serve as water condensation nuclei for contrail formation. Conditions under which ice contrails can form behind aircrafts are studied. The sensitivities of the threshold temperature for contrail formation with respect to aircraft propulsion efficiency, relative humidity, and ambient pressure are evaluated. The computed aerosol properties for different extent of fuel sulfur conversion to S(VI) (SO3 and H2SO4) in engine are examined and the results are found to be sensitive to this conversion fraction.

Menon, Suresh↗
NASA NTRS1994

Radiative Forcing of the Stratosphere by SO(sub 2) Gas, Silicate Ash, and H(sub 2)SO(sub 4) Aerosols Shortly after the 1982 Eruptions of El Chichon

The 1982 eruptions of El Chichon Volcano injected large quantities of sulfur dioxide gas and silicate ash into the stratosphere. Several studies have shown that the long-lived sulfuric acid aerosols derived from these volcanic effluents produced measurable changes in the radiative heating rates and the global circulation. The radiative and dynamical perturbations associated with the short-lived, but more strongly absorbing sulfur dioxide and ash clouds have received much less attention. We therefore used an atmospheric radiative transfer model and observations collected by satellites, aircraft, and ground based observers to estimate the amplitudes of the stratospheric radiative heating rate perturbations produced by each of these components during the first few weeks after the El Chichon eruption. One week after the April 4, 1982 eruption, net radiative heating rate perturbations exceeding 20 Kelvin per day were found at altitudes near 26 km.

El Chichon↗
NASA NTRS2001

Solubility of methanol in low-temperature aqueous sulfuric acid and implications for atmospheric particle composition

Using traditional Knudsen cell techniques, we find well-behaved Henry's law uptake of methanol in aqueous 45 - 70 wt% H2SO4 solutions at temperatures between 197 and 231 K. Solubility of methanol increases with decreasing temperature and increasing acidity, with an effective Henry's law coefficient ranging from 10(exp 5) - 10(exp 8) M/atm. Equilibrium uptake of methanol into sulfuric acid aerosol particles in the upper troposphere and lower stratosphere will not appreciably alter gas-phase concentrations of methanol. The observed room temperature reaction between methanol and sulfuric acid is too slow to provide a sink for gaseous methanol at the temperatures of the upper troposphere and lower stratosphere. It is also too slow to produce sufficient quantities of soluble reaction products to explain the large amount of unidentified organic material seen in particles of the upper troposphere.

Iraci, Laura T.↗
NASA NTRS1998

First results from the aerosol lidar and backscatter sonde intercomparison campaign STRAIT'1997 at table mountain facility during February-March 1997

First results of an intercomparison measurement campaign between three aerosol lidar instruments and in-situ backscatter sondes performed at Table Mountain Facility (34.4 deg N, 117.7 deg E, 2280 m asl) in February-March 1997 are presented. During the campaign a total of 414 hours of lidar data were acquired by the Aerosol-Temperature-Lidar (ATL, Goddard Space Flight Center) the Mobile-aerosol-Raman-Lidar (MARL, Alfred Wegener Institute), and the TMF-Aerosol-Lidar (TAL, Jet Propulsion Laboratory), and four backscatter sondes were launched. From the data set altitude profiles of backscatter ratio and volume depolarization of stratospheric background aerosols at altitudes between 15 and 25 km and optically thin high-altitude cirrus clouds at altitudes below 13 km are derived. On the basis of a sulfuric acid aerosol model color ratio profiles obtained from two wavelength lidar data are compared to the corresponding profiles derived from the sonde observations. We find an excellent agreement between the in-situ and ATL lidar data with respect to backscatter and color ratio. Cirrus clouds were present on 16 of 26 nights during the campaign. Lidar observations with 17 minute temporal and 120-300 m spatial resolution indicate high spatial and temporal variability of the cirrus layers. Qualitative agreement is found between concurrent lidar measurements of backscatter ratio and volume depolarization.

Beyerle, G.↗
NASA NTRS1995

Freezing Behavior of Stratospheric Sulfate Aerosols Inferred from Trajectory Studies

Temperature histories based on 10-day back growth trajectories for six ER-2 flights during AASE I (1989) and AAOE (1987) are presented. These trajectories along with the properties of the observed PSC (polar stratospheric cloud) particles are used here to infer the physical state of the pre-existing sulfuric acid aerosols. Of all the ER-2 flights described here, only the PSCs observed on the flights of January 24 and 25, 1989 are consistent with the thermodynamics of liquid ternary solutions of H2SO4/HNO3/H2O Ib PSCs). For these two days, back trajectories indicate that the air mass was exposed to SAT (sulfuric acid tetrahydrate) melting temperatures about 24 hours prior to being sampled by the ER-2. For the remaining ER-2 flights (January, 16, 19, and 20 for the AASE I campaign and August 17 for the AAOE campaign), the observed PSCs were probably composed of amorphous solid solutions of HNO3 and H2O (Type Ic PSCs). Formation of such Type Ic PSCs requires the presence of solid H2SO4 aerosols since liquid aerosols yield ternary solutions. The 10-day back trajectories of these flights indicate that the air mass was not exposed to SAT melting temperatures during the past week and had experienced cooling/warming cycles prior to being sampled by the ER-2. These temperature histories, recent laboratory measurements and the properties of glassy solids suggest that stratospheric H2SO4 aerosols may undergo a phase transition to SAT upon warming at approximately 198 K after going through a cooling cycle to about 194 K or lower.

Tabazadeh, A.↗
NASA NTRS2011

Influence of Aerosol Heating on the Stratospheric Transport of the Mt. Pinatubo Eruption

On June 15th, 1991 the eruption of Mt. Pinatubo (15.1 deg. N, 120.3 Deg. E) in the Philippines injected about 20 Tg of sulfur dioxide in the stratosphere, which was transformed into sulfuric acid aerosol. The large perturbation of the background aerosol caused an increase in temperature in the lower stratosphere of 2-3 K. Even though stratospheric winds climatological]y tend to hinder the air mixing between the two hemispheres, observations have shown that a large part of the SO2 emitted by Mt. Pinatubo have been transported from the Northern to the Southern Hemisphere. We simulate the eruption of Mt. Pinatubo with the Goddard Earth Observing System (GEOS) version 5 global climate model, coupled to the aerosol module GOCART and the stratospheric chemistry module StratChem, to investigate the influence of the eruption of Mt. Pinatubo on the stratospheric transport pattern. We perform two ensembles of simulations: the first ensemble consists of runs without coupling between aerosol and radiation. In these simulations the plume of aerosols is treated as a passive tracer and the atmosphere is unperturbed. In the second ensemble of simulations aerosols and radiation are coupled. We show that the set of runs with interactive aerosol produces a larger cross-equatorial transport of the Pinatubo cloud. In our simulations the local heating perturbation caused by the sudden injection of volcanic aerosol changes the pattern of the stratospheric winds causing more intrusion of air from the Northern into the Southern Hemisphere. Furthermore, we perform simulations changing the injection height of the cloud, and study the transport of the plume resulting from the different scenarios. Comparisons of model results with SAGE II and AVHRR satellite observations will be shown.

Aquila, Valentina↗
NASA NTRS1985

The University of Wyoming's small scientific balloon program

Over 500 small scientific balloons have been launched by the University of Wyoming's Atmospheric Physics Group from 26 locations over the globe in a study of stratospheric aerosol physics and chemistry which began in 1971. These flighs have led to a basic understanding of the evolution of sulfurous gases, injected into the stratosphere by major volcanic eruptions, into sulfuric acid aerosol droplets. The recent use of new, thin film balloon technology, to reduce cost and simplify launch techniques, has been a major advantage to the program.

Hofmann, D. J.↗