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NASA NTRS1988

Geochemical cycles of atmospheric gases

The processes that control the atmosphere and atmospheric changes are reviewed. The geochemical cycles of water vapor, nitrogen, carbon dioxide, oxygen, and minor atmospheric constituents are examined. Changes in atmospheric chemistry with time are discussed using evidence from the rock record and analysis of the present atmosphere. The role of biological evolution in the history of the atmosphere and projected changes in the future atmosphere are considered.

Walker, J. C. G.↗

NASA NTRS1990

Chemical kinetics and modeling of planetary atmospheres

A unified overview is presented for chemical kinetics and chemical modeling in planetary atmospheres. The recent major advances in the understanding of the chemistry of the terrestrial atmosphere make the study of planets more interesting and relevant. A deeper understanding suggests that the important chemical cycles have a universal character that connects the different planets and ultimately link together the origin and evolution of the solar system. The completeness (or incompleteness) of the data base for chemical kinetics in planetary atmospheres will always be judged by comparison with that for the terrestrial atmosphere. In the latter case, the chemistry of H, O, N, and Cl species is well understood. S chemistry is poorly understood. In the atmospheres of Jovian planets and Titan, the C-H chemistry of simple species (containing 2 or less C atoms) is fairly well understood. The chemistry of higher hydrocarbons and the C-N, P-N chemistry is much less understood. In the atmosphere of Venus, the dominant chemistry is that of chlorine and sulfur, and very little is known about C1-S coupled chemistry. A new frontier for chemical kinetics both in the Earth and planetary atmospheres is the study of heterogeneous reactions. The formation of the ozone hole on Earth, the ubiquitous photochemical haze on Venus and in the Jovian planets and Titan all testify to the importance of heterogeneous reactions. It remains a challenge to connect the gas phase chemistry to the production of aerosols.

Yung, Yuk L.↗

NASA NTRS1991

Fractionation of terrestrial neon by hydrodynamic hydrogen escape from ancient steam atmospheres

Atmospheric neon is isotopically heavier than mantle neon. By contrast, nonradiogenic mantle Ar, Kr, and Xe are not known to differ from the atmosphere. These observations are most easily explained by selective neon loss to space; however, neon is much too massive to escape from the modern atmosphere. Steam atmospheres are a likely, if intermittent, feature of the accreting Earth. They occur because, on average, the energy liberated during accretion places Earth above the runaway greenhouse threshold, so that liquid water is not stable at the surface. It is found that steam atmospheres should have lasted some ten to fifty million years. Hydrogen escape would have been vigorous, but abundant heavy constituents would have been retained. There is no lack of plausible candidates; CO2, N2, or CO could all suffice. Neon can escape because it is less massive than any of the likely pollutants. Neon fractionation would have been a natural byproduct. Assuming that the initial Ne-20/Ne-22 ratio was solar, it was found that it would have taken some ten million years to effect the observed neon fractionation in a 30 bar steam atmosphere fouled with 10 bars of CO. Thicker atmospheres would have taken longer; less CO, shorter. This mechanism for fractionating neon has about the right level of efficiency. Because the lighter isotope escapes much more readily, total neon loss is pretty minimal; less than half of the initial neon endowment escapes.

Zahnle, K.↗

NASA NTRS1991

Gas chromatographic concepts for the analysis of planetary atmospheres

Over the last few years, new gas chromatographic (GC) concepts were developed for use on board spacecraft or any other restricted environments for determining the chemical composition of the atmosphere and surface material of various planetary bodies. Future NASA Missions include an entry probe that will be sent to Titan and various spacecraft that will land on Mars. In order to be able to properly respond to the mission science requirements and physical restrictions imposed on the instruments by these missions, GC analytical techniques are being developed. Some of these techniques include hardware and mathematical techniques that will improve GC sensitivity and increase the sampling rate of a GC descending through a planetary atmosphere. The technique of Multiplex Gas Chromatography (MGC) is an example of a technique that was studied in a simulated Titan atmosphere. In such an environment, the atmospheric pressure at instrument deployment is estimated to be a few torr. Thus, at such pressures, the small amount of sample that is acquired might not be enough to satisfy the detection requirements of the gas chromatograph. In MGC, many samples are pseudo-randomly introduced to the chromatograph without regard to elution of preceding components. The resulting data is then reduced using mathematical techniques such as cross-correlation of Fourier Transforms. Advantages realized from this technique include: improvement in detection limits of several orders of magnitude and increase in the number of analyses that can be conducted in a given period of time. Results proving the application of MGC at very low pressures emulating the same atmospheric pressures that a Titan Probe will encounter when the instruments are deployed are presented. The sample used contained hydrocarbons that are expected to be found in Titan's atmosphere. In addition, a new selective modulator was developed to monitor water under Martian atmospheric conditions. Since this modulator is selective only to water, the need for a GC column is eliminated. This results in further simplification of the instrument.

Valentin, J. R.↗

NASA NTRS1992

Laboratory evaluation and application of microwave absorption properties under simulated conditions for planetary atmospheres

Radio absorptivity data for planetary atmospheres obtained from spacecraft radio occultation experiments and earth-based radio astronomical observations can be used to infer abundances of microwave absorbing atmospheric constituents in those atmospheres, as long as reliable information regarding the microwave absorbing properties of potential constituents is available. The use of theoretically derived microwave absorption properties for such atmospheric constituents, or using laboratory measurements of such properties under environmental conditions which are significantly different than those of the planetary atmosphere being studied, often leads to significant misinterpretation of available opacity data. The recognition of the need to make such laboratory measurements of simulated planetary atmospheres over a range of temperatures and pressures which correspond to the altitudes probed by both radio occultation experiments and radio astronomical observations, and over a range of frequencies which correspond to those used in both radio occultation experiments and radio astronomical observations, has led to the development of a facility at Georgia Tech which is capable of making such measurements. The goal of this investigation was to conduct such measurements and to apply the results to a wide range of planetary observations, both spacecraft and earth-based, in order to determine the identity and abundance profiles of constituents in those planetary atmospheres.

Steffes, Paul G.↗

NASA NTRS1992

Large-scale ocean-atmosphere interactions in a simplified coupled model of the midlatitude wintertime circulation

Midlatitude ocean-atmosphere interactions are studied in simulations from a simplified coupled model that includes synoptic-scale atmospheric variability, ocean current advection of SST, and air-sea heat exchange. Although theoretical dynamical ('identical twin') predictions using this model have shown that the SST anomalies in this model indeed influence the atmosphere, it is found here that standard cross correlation and empirical orthogonal function analyses of monthly mean model output yield the standard result, familiar from observational studies, that the atmosphere forces the ocean with little or no feedback. Therefore, these analyses are inconclusive and leave open the question of whether anomalous SST is influencing the atmosphere. In contrast, it is found that compositing strong warm events of model SST is a useful indicator of ocean forcing the atmosphere. Additional evidence is presented for oceanic influence on the atmosphere, namely, that ocean current advection appears to enhance the persistence of model SST anomalies through a feedback effect that is absent when only heat flux is allowed to influence SST anomaly evolution.

Miller, Arthur J.↗

NASA NTRS1992

Laboratory evaluation and application of microwave absorption properties under simulated conditions for planetary atmospheres

Radio absorptivity data for planetary atmospheres obtained from spacecraft radio occultation experiments and earth-based radio astronomical observations can be used to infer abundances of microwave absorbing atmospheric constituents in those atmospheres, as long as reliable information regarding the microwave absorbing properties of potential constituents is available. The use of theoretically-derived microwave absorption properties for such atmospheric constituents, or using laboratory measurements of such properties under environmental conditions which are significantly different than those of the planetary atmosphere being studied, often leads to significant misinterpretation of available opacity data. For example, laboratory measurements performed by Fahd and Steffes have shown that the opacity from gaseous SO2 under simulated Venus conditions can be well described by the Van Vleck-Weisskopf lineshape at wavelengths shortward of 2 cm, but that the opacity of wavelengths greater than 2 cm is best described by a different lineshape that was previously used in theoretical predictions. The recognition of the need to make such laboratory measurements of simulated planetary atmospheres over a range of temperatures and pressures which correspond to the altitudes probed by both radio occultation experiments and radio astronomical observations, and over a range of frequencies which correspond to those used in both radio occultation experiments and radio astronomical observations, has led to the development of a facility at Georgia Tech which is capable of making such measurements. It has been the goal of this investigation to conduct such measurements and to apply the results to a wide range of planetary observations, both spacecraft and earth-based, in order to determine the identity and abundance profiles of constituents in those planetary atmospheres.

Steffes, Paul G.↗

NASA NTRS1991

Interpretation of Voyager UVS observations of occultations by the atmosphere of Neptune

We propose to continue our investigation of the upper atmosphere of Neptune based primarily on the solar occultation measurements made by the Voyager Ultraviolet Spectrometer (UVS). The ultimate goal of this research is to understand the structure and composition of Neptune's upper atmosphere as encoded in the data base obtained by the UVS during the Voyager 2 encounter with Neptune. The UVS occultations provide information essential to studies of atmospheric composition and structure, energy balance, photochemistry, global transport, ionospheric structure, and airglow production mechanisms. In conjunction with other research in progress at the University of Arizona and by our colleagues at other institutions, we not only analyze and interpret individual measurements or observations by the UVS, but also construct models of the upper atmosphere which are consistent with all available data obtained by the UVS. We derive constraints from measurements of the atmospheric emissions and we combine these with constraints derived from the occultation measurements. Principal sources for the atmospheric emissions include dayglow, resonance scattering and, at long wavelengths, the reflected solar spectrum. On the dark side of the planet, a weak H Ly alpha emission is due to resonance scattering of the sky background and perhaps another source. Thus a wide range of physical processes are at work, and each provides its own constraints on the atmosphere.

Sandel, Bill R.↗

NASA NTRS1985

Application of AVHRR vegetation index to study atmosphere-biosphere exchange of CO2: Results from a 3-D tracer transport model

The 'normalized difference vegetation indices' (NVI) derived from AVHRR radiances are combined with field data of soil respiration and a global map of net primary productivity to prescribe, for the globe, the seasonal exchange of CO2 between the atmosphere and the terrestrial biosphere. The monthly fluxes of CO2 thus obtained are used as inputs to a 3-D tracer transport model which uses winds generated by a 3-D atmospheric general circulation model to advect CO2 as an inert constituent. Analysis of the 3-D model results shows reasonable agreement between the simulated and observed annual cycles of atmospheric CO2 at the locations of the remote monitoring stations. The application is shown of atmospheric CO2 distributions to calibrate the NVI in terms of carbon fluxes. The approach suggests that the NVI may be used to provide quantitative information about long term and global scale variations of photosynthetic activity and of atmospheric CO2 concentrations provided that variations in the atmospheric circulation and in atmospheric composition are known.

Fung, Inez Y.↗

NASA NTRS1992

Integration of space and in-situ observations to study atmosphere, ocean and land processes

A research investigation was conducted into the possibility of using atmospheric observations made in the past from both terrestrial and space-based platforms to create a global, coherent four dimensional analysis for the purpose of studying atmospheric, oceanic, and land surface processes relevant to climate simulation, monitoring, and change. This investigation consisted of the following tasks: (1) a mature global data assimilation system was obtained from the National Meteorological Center and modified for use on a Cray X-MP computer system; (2) atmospheric observations for the period 20 Nov. 1982 through 1 Mar. 1983, including rawinsonde soundings, aircraft-based measurements, pilot balloons, and temperature soundings from polar orbiting satellites were obtained from several sources; and (3) the global data assimilation system was used to reassimilate the atmospheric observations to produce a new atmospheric analysis which was then compared with the contemporaneous analysis. The global hydrologic cycle, including fluxes between the atmosphere and both the land and ocean surfaces, was estimated. The flux of water from the ocean surface into the atmosphere, its transport in the form of latent heat to remote regions, and its return to the surface in the form of precipitation were estimated globally. In addition, several regional budgets for selected tropical oceanic and extratropical continental areas were also done.

Shukla, J.↗

NASA NTRS1993

Discovery Venera surface: Atmosphere geochemistry experiments mission concept

The phenomenal increase in our understanding of Venus provided by the Magellan Mission has raised a series of focused, fundamental scientific questions about the geochemistry of the surface of Venus, the nature of the lower atmosphere, and the relationship of the lower atmosphere and surface. First, surface geochemical measurements from the Venera/Vega spacecraft showed that widely spaced regions of the venusian plains are made of basalts; thus basalts are significant and may be the only component of the venusian crust. But we lack information on the composition of several key elements of Venus geology: (1) Tessera terrain (which may be outcrops of continental-like non-basaltic crustal material) and steep-sided domes/festoons are promising candidates for non-basaltic geochemically evolved material. The composition of the lower part of the Venusian crust is unknown: however, ejecta from large venusian craters provides us with the possibility of sampling this material on the surface; (2) bulk chemistry (structure and dynamics) of the venusian atmosphere are known. The altitude profiles of water vapor content and minor admixtures relevant to redox conditions in the lower atmosphere (less than 20 km altitude) remain uncertain. Lack of that knowledge means that we do not understand the fine chemical structure of the main mass of the Venusian atmosphere; and (3) thermodynamic models predict that igneous materials on the surface of Venus should react with gases of the venusian atmosphere. But because the water vapor content and redox conditions in the lower atmosphere are not well known, we do not understand the nature of venusian weathering: oxidation, sulfatization, carbonatization, and hydration. The answers to these questions are critical to the understanding of Venus, the most Earth-like of the terrestrial planets.

Surkov, Yuri A.↗

NASA NTRS1993

Eddy transport of water vapor in the Martian atmosphere

Viking orbiter measurements of the Martian atmosphere suggest that the residual north polar water-ice cap is the primary source of atmospheric water vapor, which appears at successively lower northern latitudes as the summer season progresses. Zonally symmetric studies of water vapor transport indicate that the zonal mean meridional circulation is incapable of transporting from north polar regions to low latitudes the quantity of water vapor observed. This result has been interpreted as implying the presence of nonpolar sources of water. Another possibility is the ability of atmospheric wave motions, which are not accounted for in a zonally symmetric framework, to efficiently accomplish the transport from a north polar source to the entirety of the Northern Hemisphere. The ability or inability of the full range of atmospheric motions to accomplish this transport has important implications regarding the questions of water sources and sinks on Mars: if the full spectrum of atmospheric motions proves to be incapable of accomplishing the transport, it strengthens arguments in favor of additional water sources. Preliminary results from a three dimensional atmospheric dynamical/water vapor transport numerical model are presented. The model accounts for the physics of a subliming water-ice cap, but does not yet incorporate recondensation of this sublimed water. Transport of vapor away from this water-ice cap in this three dimensional framework is compared with previously obtained zonally symmetric (two dimensional) results to quantify effects of water vapor transport by atmospheric eddies.

Murphy, J. R.↗

NASA NTRS1994

Mars atmospheric escape and isotopic fractionation: Synthesis of data and models

The present Mars atmosphere is relatively thin and cold. It is not at all like that which is presumed to have been responsible for the formation of valley networks and the heavy erosion of craters during the earliest epochs of martian history. An important goal of Mars exploration is to try to understand the properties of the early atmosphere, the initial inventory of volatiles at the planet's surface, the processes by which the atmosphere and climate have evolved over time, and the current location of volatiles presumed to have been in the atmosphere in the earlier times. The current status of understanding of the escape of volatiles to space over geologic time and the resulting fractionation of isotopes of stable atoms remaining in the atmosphere are described, and a scenario for volatile abundance and evolution that is consistent with the available information on the escape and fractionation of each species is constructed. In particular, the evolution of hydrogen, carbon, oxygen, and nitrogen, as contained in atmospheric (and non-atmospheric) water, carbon dioxide, and molecular nitrogen, is examined.

Jakosky, Bruce M.↗

NASA NTRS1994

Stability of the Martian atmosphere: Is heterogeneous catalysis essential?

A comprehensive homogeneous gas phase photochemical model is developed to study the problem of stability of the Martian atmosphere. The one-dimensional model extends from the ground up to 220 km, passing through the homopause at 125 km. The model thus couples the lower (neutral) atmosphere to the ionosphere above which provides significant downward flux of carbon monoxide and oxygen atoms. It is concluded on the basic of currently accepted values for globally and seasonally averaged water vapor abundance, dust opacity and the middle atmospheric eddy mixing coefficient, as well as the relevant laboratory data (particularly the temperature dependence of CO2 absorption cross section and the rate constant for CO+OH reaction), that the rate of re-formation of carbon dioxide exceeds its photolytic destruction rate by about 40%. Furthermore, it is found that this result is virtually independent of the choice of eddy mixing coefficient, unless its value in the middle atmosphere exceeds 10(exp 8) sq cm/sec or is far smaller than 10(exp 5)sq cm/sec, or the dust opacity, unless it exceeds unity, or the water vapor mixing ratio at the surface, unless it is far smaller (less than or = 1 ppm) or far greater (greater than or = 500 ppm) than the average value (approximately 150 ppm). Since none of these extremes represent globally and seasonally averaged conditions on Mars, we propose that the present model requires existence of a mechanism to throttle down the recycling rate of carbon dioxide on Mars. Therefore, it is suggested that a heterogeneous process which provides a sink to the species that participate in the recycling of CO2, i.e., H2O, H2O2, OH, CO or O, in particular, may be necessary to bring about the balance between the CO2 recycling rate and its photolytic destruction rate. Aerosols of dust or ice (pure or doped water or carbon dioxide ice present in the atmosphere of Mars) can provide the appropriate adsorption sites for the above heterogeneous process. Despite our conclusion that some heterogeneous process may be needed, it is important to recognize that one-dimensional models can only provide first-order results which, most likely, represent globally and seasonally averaged conditions. However, it is only after actual temporal, latitudinal and longitudinal variations of relevant atmospheric parameters are included in the model that one can determine fuly whether the problem of atmospheric stabiltiy still continues to persist and whether some heterogeneous process is required to correct it.

Atreya, Sushil K.↗

NASA NTRS1994

Detection of the SO2 atmosphere on Io with the Hubble Space Telescope

Observations of the trailing hemisphere of Io made with the Faint Object Spectrograph of the Hubble Space Telescope (HST) in March 1992 have resulted in the first detection of atmospheric SO2 absorption bands in the ultraviolet. These observations represent only the third positive means of detection of what is widely believed to be Io's primary atmospheric constituent. Below approximately 2130 A the geometric albedo of the satellite is dominated by SO2 gas absorption band signatures, which have been analyzed using models that include the effects of optical thickness, temperature, and spatial distribution. The disk-intergrated HST data cannot resolve the spatial distribution, but it is possible to define basic properties and set constraints on the atmosphere at the time of the observations. Hemispheric atmospheres with average column density N = 6 - 10 x 10(exp 15)/sq sm and T(gas) = 110 - 500 K fit the data, with preference for temperatures of approximately 200 - 250 K. Better fits are found as the atmosphere is spatially confined, with a limit of approximately 8% hemispheric areal coverage and N approximately equal to 3 x 10(exp 17)/sq cm with colder 110 - 250 K temepratures. A dense (N greater than or equal to 10(exp 16)/sq cm), localized component of SO2 gas, such as that possibly associated with active volcanoes, can generate the observed spectral constrast only when the atmosphere is cold (110 K) and an extended component such as Pele is included. The combination of a dense, localized atmosphere with a tenuous component (N less than 10(exp 16)/sq cm, either patchy or extended) also fits the data. In all cases the best fit models imply a disk-averaged column density larger than exospheric but approximately 10 - 30 times less than the previous upper limit from near-UV observations.

Ballester, G. E.↗

NASA NTRS1994

Mars atmospheric loss and isotopic fractionation by solar-wind-induced sputtering and photochemical escape

We examine the effects of the loss of Mars atmospheric constituents by solar-wind-induced sputtering and by photochemical escape during the past 3.8 billion years. Sputtering is capable of efficiently removing species from the upper atmosphere, including the light noble gases; nitrogen and oxygen are removed by photochemical processes as well. Due to diffusive separation (by mass) above the homopause, removal from the top of the atmosphere will fractionate the isotopes of each species, with the lighter mass being preferentially lost. For carbon and oxygen, this allows us to determine the size of nonatmospheric reservoirs which mix with the atmosphere; these reservoirs can be CO2 adsorbed in the regolith and H2O in the polar ice caps. We have constructed both simple analytical models and time-dependent models of the loss of volatiles from and supply to the martian atmosphere. Both argon and neon require continued replenishment from outgassing over geologic time. For argon, sputtering loss explains the fractionation of (Ar-36)/(Ar-38) without requiring a distinct epoch of hydrodynamic escape (although fractionation of Xe isotopes still requires very early hydrodynamic loss). For neon, the current (Ne-22)/(Ne-20) ratio represents a balance between loss to space and continued resupply from the interior; the similarity of the ratio to the terrestrial value is coincidental. For nitrogen, the loss by both sputtering and photochemical escape would produce a fractionation of (N-15)/(N-14) larger than observed; an early, thicker carbon dioxide atmosphere could mitigate the nitrogen loss and produce the observed fractionation, as could continued outgassing of juvenile nitorgen. Based on the isotopic constraints, the total amount of carbon dioxide lost over geologic time is probably on the order of tens of millibars rather than a substantial fraction of a bar. The total loss from solar-wind-induced sputtering and photochemical escape, therefore, does not seem able to explain the loss of a putative thick, early atmosphere withput requiring formation of extensive surface carbonate deposits or other nonatmospheric reservoirs for CO2.

Jakosky, Bruce M.↗

NASA NTRS1995

Atmospheric thermal lensing in laser resonators

Atmospheric absorption degrades laser performance both by absorbing laser energy within the laser resonator, which increases the loss, and by inducing a thermal lens in the atmosphere. Atmospheric thermal lensing can be quite severe, even when the absorption coefficient is quite modest. A model is developed which describes atmospheric thermal lensing; time constants, which are associated with the establishment and decay of the atmospheric thermal lens, are determined; experiments are performed using an injection seeded Ti:Al2O3 laser tuned to the H2O absorption lines near 0.815 microns to validate the model; dependence of the atmospheric thermal lens on the laser energy and absorption coefficient were measured and found to agree with the model. In addition, the decay of the atmospheric thermal lens with time was measured and also found to agree with the model predictions.

Barnes, Norman P.↗

NASA NTRS1995

Microwave Resonator Measurements of Atmospheric Absorption Coefficients: A Preliminary Design Study

A preliminary design study examined the feasibility of using microwave resonator measurements to improve the accuracy of atmospheric absorption coefficients and refractivity between 18 and 35 GHz. Increased accuracies would improve the capability of water vapor radiometers to correct for radio signal delays caused by Earth's atmosphere. Calibration of delays incurred by radio signals traversing the atmosphere has applications to both deep space tracking and planetary radio science experiments. Currently, the Cassini gravity wave search requires 0.8-1.0% absorption coefficient accuracy. This study examined current atmospheric absorption models and estimated that current model accuracy ranges from 5% to 7%. The refractivity of water vapor is known to 1% accuracy, while the refractivity of many dry gases (oxygen, nitrogen, etc.) are known to better than 0.1%. Improvements to the current generation of models will require that both the functional form and absolute absorption of the water vapor spectrum be calibrated and validated. Several laboratory techniques for measuring atmospheric absorption and refractivity were investigated, including absorption cells, single and multimode rectangular cavity resonators, and Fabry-Perot resonators. Semi-confocal Fabry-Perot resonators were shown to provide the most cost-effective and accurate method of measuring atmospheric gas refractivity. The need for accurate environmental measurement and control was also addressed. A preliminary design for the environmental control and measurement system was developed to aid in identifying significant design issues. The analysis indicated that overall measurement accuracy will be limited by measurement errors and imprecise control of the gas sample's thermodynamic state, thermal expansion and vibration- induced deformation of the resonator structure, and electronic measurement error. The central problem is to identify systematic errors because random errors can be reduced by averaging. Calibrating the resonator measurements by checking the refractivity of dry gases which are known to better than 0.1% provides a method of controlling the systematic errors to 0.1%. The primary source of error in absorptivity and refractivity measurements is thus the ability to measure the concentration of water vapor in the resonator path. Over the whole thermodynamic range of interest the accuracy of water vapor measurement is 1.5%. However, over the range responsible for most of the radio delay (i.e. conditions in the bottom two kilometers of the atmosphere) the accuracy of water vapor measurements ranges from 0.5% to 1.0%. Therefore the precision of the resonator measurements could be held to 0.3% and the overall absolute accuracy of resonator-based absorption and refractivity measurements will range from 0.6% to 1.

Walter, Steven J.↗