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NASA NTRS1992

Chemical modeling constraints on Martian surface mineralogies formed in an early, warm, wet climate, and speculations on the occurrence of phosphate minerals in the Martian regolith

This is one in a series of reports summarizing our chemical modeling studies of water-rock-gas interactions at the martian surface through time. The purpose of these studies is to place constraints on possible mineralogies formed at the martian surface and to model the geochemical implications of martian surficial processes proposed by previous researchers. Plumlee and Ridley summarize geochemical processes that may have occurred as a result of inferred volcano- and impact-driven hydrothermal activity on Mars. DeBraal et al. model the geochemical aspects of water-rock interactions and water evaporation near 0 C, as a prelude to future calculations that will model sub-0 C brine-rock-clathrate interactions under the current martian climate. In this report, we discuss reaction path calculations that model chemical processes that may have occurred at the martian surface in a postulated early, warm, wet climate. We assume a temperature of 25 C in all our calculations. Processes we model here include (1) the reaction of rainwater under various ambient CO2 and O2 pressures with basaltic rocks at the martian surface, (2) the formation of acid rain by volcanic gases such as HCl and SO2, (3) the reactions of acid rain with basaltic surficial materials, and (4) evaporation of waters resulting from rainwater-basalt interactions.

Plumlee, Geoffrey S.↗

NASA NTRS1992

The effect of magnetospheric ion bombardment on the reflectance of Europa's surface

Laboratory investigations have been conducted to ascertain the role of sulphur ion implantation on differences in the reflectivity of the leading and trailing atmospheres of Europa in the visible and UV ranges. Under the laboratory conditions tested, neither S-implantation nor SO2 deposition can account for the general 'reddening' of the trailing hemisphere in the UV, relative to the leading hemisphere; this feature has been shown to be producible by fast penetrating ions.

Sack, N. J.↗

NASA NTRS1993

Tropical ozone loss following the eruption of Mt. Pinatubo

Total Ozone Mapping Spectrometer (TOMS) measurements of equatorial total ozone following the eruption of Mt. Pinatubo show a decrease of up to 6 percent over climatology. Ozone losses begin approximately a month following the eruption, consistent with the time required for the SO2 to convert to sulfuric acid aerosol. The thick aerosol layer interferes with the TOMS retrieval, but this interference is small and easily accounted for in the retrieval. Ozone values remain below climatology until December, 1991. Ozonesonde data from Natal, Brazil taken before and two months after the eruption support TOMS observations of ozone loss. These sondes show that the ozone loss region is confined to a 2-3 km thick layer between 24 and 28 km.

Schoeberl, Mark R.↗

NASA NTRS1992

The equilibrium of atmospheric sodium

We now have four examples of planetary objects with detectable sodium (and potassium) in their atmospheres: Earth, Io, Mercury and the moon. After a summary of the observational data, this survey discusses proposed sources and sinks. It appears that Io's surface material is rich in frozen SO2, but with around 1 percent of some sodium compound. The Io plasma torus contains ions of S, O and Na, also with at least one molecular ion containing Na. In turn, impact by these ions probably sustains the torus, as well as an extended neutral corona. A primary source for the Earth, Mercury and the moon is meteoroidal bombardment; at Mercury and perhaps the moon it may be supplemented by degassing of atoms from the regolith. Photoionization is important everywhere, although hot electrons are dominant at Io.

Hunten, Donald M.↗

NASA NTRS1993

Electron impact emission cross sections needed in modeling UV observations of the upper atmospheres of the planets

In recognition of the need for accurate collision cross-sections suitable for modeling spectroscopic observations of the planetary systems and calibrate flight instruments, NASA-JPL has determined the laboratory emission cross-sections of H, H2, N2, SO2, etc. Resonance excitation, predissociation, and non-Franck-Condon band intensity systems are determined by configuration interaction and must be taken into account in analyses of spacecraft observations. Attention is given to the application of the cross-sectional data obtained to both electron energy loss codes and models of Voyager, IUE, Galileo, and HST observations of the solar system.

Ajello, J. M.↗

NASA NTRS1993

A global three-dimensional model of the stratospheric sulfuric acid layer

A 3D model which encompasses SO2 production from OCS, followed by its oxidation to gaseous H2SO4, the condensation-evaporation equilibrium of gaseous and particulate H2SO4, and finally particle condensation and rainout, is presently used to study processes maintaining the nonvolcanically-perturbed stratosphere's sulfuric acid layer. A comparison of the results thus obtained with remotely sensed stratospheric aerosol extinction data shows the model to simulate the general behavior of stratospheric aerosol extinction.

Golombek, Amram↗

NASA NTRS1993

Twenty years of balloon-borne tropospheric aerosol measurements at Laramie, Wyoming

The paper examines the tropospheric aerosol record obtained over the period 1971 to 1990, during which high-altitude balloons with optical particle counters were launched at Laramie, Wyoming, in a long-term study of the stratospheric sulfate aerosol layer. All aerosol particle size ranges display pronounced seasonal variations, with the condensation nuclei concentration and the optically active component showing a summer maximum throughout the troposphere. Mass estimates, assuming spherical sulfate particles, indicate an average column mass between altitudes of 2.5 and 10 km of about 4 and 16 mg/sq m in winter and summer, respectively. Calculated optical depths vary between 0.01 and 0.04 from winter to summer; the estimated mass scattering cross section is about 3 sq m/g throughout the troposphere. There is evidence for a decreasing trend of 1.6-1.8 percent/yr in the optically active tropospheric aerosol over the past 20 yr, which may be related to a similar reduction in SO2 emission in the U.S. over this period.

Hofmann, David J.↗

NASA NTRS1993

An assessment of volatile release from recent volcanism in Elysium, Mars

The amount and rate of release of volatiles (H2O, CO2, etc.) from recent volcanism in Elysium, Mars, are estimated. Possible implications of these volatiles on the climate, weathering, and surface morphology are discussed. Total eruptic volcanics may amount to about 4 x 10 exp 5 cu km and would have released large quantities of volatiles into the Martian environment. Assuming that the lavas contained 1.0 wt pct water, about 7.6 x 10 exp 15 kg of the water, or about 1000 times the present atmospheric water inventory, would have been released. Release amounts of other volatiles are estimated to be 10 exp 15 kg of S, 10 exp 13 kg of Cl, and 10 exp 13 kg of F. The short-term effect of the SO2 gas would be to warm the climate due to its greenhouse properties. Conversion to sulfate aerosols might have resulted in a net surface cooling due to scattering of sunlight. As the sulfate aerosols settled from the atmosphere, the climate could have returned to its preeruption equilibrium.

Plescia, J. B.↗

NASA NTRS1993

Effect of plasma ion bombardment on the reflectance of Io's trailing and leading hemispheres

The possible effect of a net difference in the ion bombardment flux to the surface of Io on the ratio of the reflectance spectra is investigated. Io's vapor-deposited surface layers are simulated by a laboratory-produced film of vapor-deposited SO2 with a small admixture (about 3 percent) of H2S and (about 0.1 percent) H2O. It is shown that the reflectance ratio in the UV/visible of the surface bombarded by keV ions to the unbombarded surface is surprisingly similar to the observed ratio of Io's trailing to leading hemispherical reflectance. The changes produced are either structural or involve products of species originally present in the sample.

Sack, N. J.↗

NASA NTRS1993

Nimbus-7 Total Ozone Mapping Spectrometer (TOMS) data products user's guide

Two tape products from the Total Ozone Mapping Spectrometer (TOMS) aboard the Nimbus-7 have been archived at the National Space Science Data Center. The instrument measures backscattered Earth radiance and incoming solar irradiance; their ratio -- the albedo -- is used in ozone retrievals. In-flight measurements are used to monitor changes in the instrument sensitivity. The algorithm to retrieve total column ozone compares the observed ratios of albedos at pairs of wavelengths with pair ratios calculated for different ozone values, solar zenith angles, and optical paths. The initial error in the absolute scale for TOMS total ozone is 3 percent, the one standard-deviation random error is 2 percent, and the drift is +/- 1.5 percent over 14.5 years. The High Density TOMS (HDTOMS) tape contains the measured albedos, the derived total ozone amount, reflectivity, and cloud-height information for each scan position. It also contains an index of SO2 contamination for each position. The Gridded TOMS (GRIDTOMS) tape contains daily total ozone and reflectivity in roughly equal area grids (110 km in latitude by about 100-150 km in longitude). Detailed descriptions of the tape structure and record formats are provided.

Mcpeters, Richard D.↗

NASA NTRS1994

Studies for the loss of atomic and molecular species from Io

The general objective of this project is to advance theoretical understanding of Io's atmosphere and how various atomic and molecular species are lost from this atmosphere and are distributed in the circumplanetary environment of Jupiter. The major task for the University of Michigan portion of this work is the generalization of the Io sodium cloud model to simulate the ion-precursor of sodium that is the apparent source of the fast sodium jet observed by Schneider et al. (1991). The goal is a quantitative test of the molecular ion hypothesis with a model that is comparable to a general sodium cloud model published previously. A detailed comparison of observations with such a model will help to probe the feasibility of such a source and to examine the rates and scale lengths associated with the decay of the ion precursor so as to possibly uncover the identity of the parent ion. Another important task to be performed at Michigan is more support of AER in the general area of modeling the Na and SO2-family clouds.

Combi, Michael R.↗

NASA NTRS1994

Absolute determination of local tropospheric OH concentrations

Long path absorption (LPA) according to Lambert Beer's law is a method to determine absolute concentrations of trace gases such as tropospheric OH. We have developed a LPA instrument which is based on a rapid tuning of the light source which is a frequency doubled dye laser. The laser is tuned across two or three OH absorption features around 308 nm with a scanning speed of 0.07 cm(exp -1)/microsecond and a repetition rate of 1.3 kHz. This high scanning speed greatly reduces the fluctuation of the light intensity caused by the atmosphere. To obtain the required high sensitivity the laser output power is additionally made constant and stabilized by an electro-optical modulator. The present sensitivity is of the order of a few times 10(exp 5) OH per cm(exp 3) for an acquisition time of a minute and an absorption path length of only 1200 meters so that a folding of the optical path in a multireflection cell was possible leading to a lateral dimension of the cell of a few meters. This allows local measurements to be made. Tropospheric measurements have been carried out in 1991 resulting in the determination of OH diurnal variation at specific days in late summer. Comparison with model calculations have been made. Interferences are mainly due to SO2 absorption. The problem of OH self generation in the multireflection cell is of minor extent. This could be shown by using different experimental methods. The minimum-maximum signal to noise ratio is about 8 x 10(exp -4) for a single scan. Due to the small size of the absorption cell the realization of an open air laboratory is possible in which by use of an additional UV light source or by additional fluxes of trace gases the chemistry can be changed under controlled conditions allowing kinetic studies of tropospheric photochemistry to be made in open air.

Armerding, Wolfgang↗

NASA NTRS1993

Magmatic volatiles and the weathering of Mars

The sources for volatiles on Mars have been the subject of many hypotheses for exogenous influences including late accretion of volatile-enriched material, impact devolatilization to create massive early atmospheres, and even major bombardment by comets. However, the inventory of chemically active volatiles observable at the contemporary surface of Mars is consistent with domination by endogenous, subsequent planetary processes, viz., persistent magmatic outgassing. Volcanism on Mars has been widespread in both space and time. Notwithstanding important specific differences between the mantles of Earth and Mars, the geochemical similarities are such that the suite of gases emitted from Martian volcanic activity should include H2O, CO2, S-containing gases (e.g. H2S and/or SO2), and Cl-containing gases (e.g., Cl2 and/or HCl). H2O and CO2 exist in the atmosphere of Mars. Both are also present as surface condensates. However, spectroscopic observations of the Martian atmosphere clearly show that the S- and Cl-containing gases are severely depleted, with upper limits of less than or equal to 10(exp -7) the abundance of CO2. Likewise, there is no evidence of polar condensates of compounds of these elements as there is for CO2 and H2O. Within the soil, on the other hand, there has been direct measurement of incorporated H2O and abundant compounds containing S and Cl. Barring some as yet implausible geochemical sequestering process, the S/Cl ratio of about 6:1 in Martian soils implies a limit of 5% on the contribution of matter of solarlike composition (e.g., carbonaceous chondrite or cometary material) to these volatiles. Hence, exogenous sources are minor or not yet observed. From analysis of elemental trends in Martian soils, it has been recently shown that a simple two-component model can satisfy the Viking in situ measurements. Component A includes Si and most or all the Al, Ca, Ti, and Fe. Component B, taken as 16 +/- 3% by weight of the total, contains S and most or all the Cl and Mg. These results constrain several models of Martian soil mineralogy but are consistent with a mixture of silicates (such as Fe-rich clays and accessory minerals and soluble salts). The overall element profile is notably like shergottites, with significant incorporation of chemically reactive atmospheric gases from magmatic degassing.

Clark, B. C.↗

NASA NTRS1994

Comparison of TOMS and AVHRR imagery of volcanic clouds

This project consisted of merging volcanic cloud data from initial studies from TOMS and AVHRR sensors. Because of the different data acquisition platforms and processing algorithms and formats, the combination of the two data required special consideration. Once the registration technique was perfected, several eruptions with data from both sensors were studied. The conclusion showed that, from the initial work, the positions of the volcanic clouds as detected by the two sensors are very similar. Because the AVHRR algorithm is now capable of retrieving masses of ash and sulfate aerosol, the capability of comparing data from the two sensors now allows changes in SO2, H2SO4, and silicated ash in drifting clouds to be described. The results of this study culminated in several presentations, and a master's thesis, which in turn was converted into a paper submitted to the Journal of Geophysical Research. Abstracts of two presentations are attached.

Rose, William I.↗

NASA NTRS1994

An analysis of the impacts of global climate and emissions changes on regional tropospheric ozone

Many of the synergistic impacts resulting from future changes in emissions as well as changes in ambient temperature, moisture, and UV flux have not been quantified. A three-dimensional regional-scale photo-chemical model (STEM-2) is used in this study to evaluate these perturbations to trace gas cycles over the eastern half of the United States of America. The model was successfully used to simulate a regional-scale ozone episode (base case - June 1984) and four perturbations scenarios - viz., perturbed emissions, temperature, water vapor column, and incoming UV flux cases, and a future scenario (for the year 2034). The impact of these perturbation scenarios on the distribution of ozone and other major pollutants such as SO2 and sulfates were analyzed in detail. The spatial distribution and the concentration of ozone at the surface increased by about 5-15 percent for most cases except for the perturbed water vapor case. The regional scale surface ozone concentration distribution for the year 2034 (future scenario) showed an increase of non-attainment areas. The rural areas of Pennsylvania, West Virginia, and Georgia showed the largest change in the surface ozone field for the futuristic scenario when compared to the base case.

John, Kuruvilla↗

NASA NTRS1994

The sensitivity of tropospheric chemistry to cloud interactions

Clouds, although only occupying a relatively small fraction of the troposphere volume, can have a substantial impact on the chemistry of the troposphere. In newly formed clouds, or in clouds with air rapidly flowing through, the chemistry is expected to be far more active than in aged clouds with stagnant air. Thus, frequent cycling of air through shortlived clouds, i.e. cumulus clouds, is likely to be a much more efficient media for altering the composition of the atmosphere than an extensive cloud cover i.e. frontal cloud systems. The impact of clouds is tested out in a 2-D channel model encircling the globe in a latitudinal belt from 30 to 60 deg N. The model contains a detailed gas phase chemistry. In addition physiochemical interactions between the gas and aqueous phases are included. For species as H2O2, CH2O, O3, and SO2, Henry's law equilibria are assumed, whereas HNO3 and H2SO4 are regarded as completed dissolved in the aqueous phase. Absorption of HO2 and OH is assumed to be mass-transport limited. The chemistry of the aqueous phase is characterized by rapid cycling of odd hydrogen, (H2O2, HO2, and OH). O2(-) (produced through dissociation of HO2) reacting with dissolved O3 is a major source of OH in the aqueous phase. This reaction can be a significant sink for O3 in the troposphere. In the interstitial cloud air, odd hydrogen is depleted, whereas NO(x) remains in the gas phase, thus reducing ozone production due to the reaction between NO and HO2. Our calculations give markedly lower ozone levels when cloud interactions are included. This may in part explain the overpredictions of ozone levels often experienced in models neglecting cloud chemical interactions. In the present study, the existence of clouds, cloud types, and their lifetimes are modeled as pseudo random variables. Such pseudo random sequences are in reality deterministic and may, given the same starting values, be reproduced. The effects of cloud interactions on the overall chemistry of the troposphere are discussed. In particular, tests are performed to determine the sensitivity of cloud frequencies and cloud types.

Jonson, Jan E.↗

NASA NTRS1994

Comparison between Brewer spectrometer, M 124 filter ozonometer and Dobson spectrophotometer

Concurrent measurements were taken using the Brewer spectrometer no. 30, the filter ozonometer M 124 no. 200 and the Dobson spectrophotometer no. 71 from September 1987 to December 1988 at Potsdam. The performance of the instrument types and the compatibility of ozone data was checked under the conditions of a field measuring station. Total ozone values derived from Dobson AD direct sun measurements were considered as standard. The Dobson instrument had been calibrated at intercomparisons with the World Standard Dobson instrument no. 83 (Boulder) and with the Regional Standard instrument no. 64 (Potsdam), while the Brewer instrument was calibrated several times with the Travelling Standard Brewer no. 17 (Canada). The differences between individual Brewer DS (direct sun) ozone data and Dobson ADDS are within plus or minus 3 percent with half of all differences within plus or minus 1 percent. Less than 0.7 percent of the systematic difference can be due to atmospheric SO2. Due to inadequate regression coefficients Brewer ZB (zenith blue) ozone measurements are by (3...4) percent higher than Dobson ADDS ozone values. M124 DS ozone data are systematically by (1...2) percent higher than Dobson ADDS ozone with 50 percent of the differences within plus or minus 4 percent, but with extreme differences up to plus or minus (20...25) percent. M124 ZB ozone values are by (3...5) percent higher than Dobson ADDS with all the differences within plus or minus 10 percent, i.e. the scatter of differences is smaller for ZB than for M 124 DS measurements, Results for differences in the daily mean ozone values are also addressed. The differences include the uncertainties in the ozone values derived from both types of measurements. They provide an indication of the uncertainty in ozone data and the comparability of ozone values derived from different types of instruments.

Feister, U.↗

NASA NTRS1994

Quantitative understanding of the cycles of oxidized and reduced sulfur on Venus

The evolution of the Venus atmosphere is determined by the supply of gases from the interior of the planet and outer space, and by the loss of particles to space over time. In particular, questions pertaining to the initial inventory of water and the current and past rates of outgassing can be addressed by studying the loss rates of H, D, He3 and He4. The photochemistry of the H2SO4 clouds may also have played an important role in regulating the amount of water above the cloud tops, and hence limit the rate of escape of hydrogen from the planet. Thus the problems of evolution and chemistry are intimately related. In our proposal the principal tasks we undertook to advance our understanding of the origin and evolution of water on Venus included: (1) escape of light atoms from Venus and (2) develop a photochemical model of sulfate formation. In the last two years we have made progress on Task 1 regarding how light atoms can escape from the exosphere of Venus with the development of a Monte Carlo program and in Task 2 have developed a thorough update on the SO2 photochemistry that had been previously carried out.

Yung, Yuk L.↗