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NASA NTRS1998

Theoretical Studies of Important Processes in Planetary and Comet Atmospheres

Using theoretical quantum chemical calculations, I have successfully described the dissociative recombination (DR) of O2(+) leading to the excited S-1 state of atomic oxygen, the upper state of the well known green line emission. The process is described by O2(+) + e(-) yields O(S-1)) + O(D-1) (1) where e(-) is an electron and the product oxygen atoms are both excited. This process is important in the atmospheres of Venus, Mars and Earth. I have shown in prior calculations that only one repulsive potential curve of O2, f(sup l)Sigma(sub u, sup +) can generate O(S-1) from DR of the lowest vibrational levels of O2(+). However, in the prior results, the calculated quantum yield (i.e. the number of O(S-1) atoms produced for every two product atoms) from the O2(+) v = 0 level was smaller than the laboratory and atmospheric measurements by more than an order of magnitude. Including only direct recombination, the calculated quantum yield for O(S-1) is only 0.0016. In a calculation that accounts for both direct and indirect recombination, the quantum yield is 0.0012. The range of experimentally determined quantum yields is between 0.01 and 0.23. Because of this large difference between the theoretical and experimental quantum yields, it was thought for some time that the ionospheric and laboratory O2(+) must be vibrationally excited since for excited levels, theory gave quantum yields that are similar to experimental yields. It was also suggested that some other process was generating O(S-1) but none could be identified. Under current NASA support, I have found that reaction (1) proceeds via an unusual mechanism. The f(sup 1)Sigma(sub u, sup,+) state does not cross the ion between the turning points of the v = 0 level of the O2(+) ground state. The lack of a favorable crossing leads to a very small calculated DR rate coefficient. However, this mechanism assumes that initial electron capture must occur into the repulsive state that leads to )(S-1). Instead, I have found that initial electron capture occurs mostly into the B(sup 3)Sigma(sup u, sub -) state which crosses the ion between the turning points of the v = 0 ion level and has a large DR rate coefficient. The B state dissociates to O(D-1) and )(P-3). After capture, some of the flux is transferred to the f(sup 1)Sigma(sup u, sub +) state via symmetry mixed intermediate Rydberg states. The neutral Rydberg states are a mixture of Sigma(sub u, sup +)-1 and Sigma(sub u, sup -)-3 symmetry.

Guberman, Steven L.↗

NASA NTRS1990

Theoretical studies of important processes in planetary and comet atmospheres

Dissociative recombination (DR) reactions in planetary and comet atmospheres are discussed. A computer program was developed which determines DR cross sections and rates using potential curves and electronic capture widths. It uses Multi-Channel Quantum Defect Theory (MQDT) to include excited Rydberg resonance levels in the DR cross section and rate calculations. Each vibrational level of a molecular ion is the limit for an infinite series of Rydberg states. Above each ion vibrational level are Rydberg vibrational levels having higher ion levels as their series limit. These Rydberg vibrational levels are resonances, i.e., neutral states which are imbedded in the electron-molecular ion continuum. The process in which the Rydberg level causes an abrupt perturbation in the cross section for DR (because of interference between capture into the Rydberg level and capture into the repulsive dissociative state) is referred to as indirect recombination. The process in which the Rydberg levels are excluded and recombination goes from the entrance channel to the repulsive state is called direct recombination. The full DR process, i.e., both direct and indirect recombination, is the process of importance for planetary atmospheres. These ideas are illustrated with the new results for DR from excited ion vibrational levels of O2(+) into the dissociative state which leads to O(1S) + O(1D).

Guberman, Steven L.↗

NASA NTRS1989

Theoretical studies of important processes in planetary and comet atmospheres. Renewel request

Current efforts have focused on the dissociative recombination (DR) of O2(+), a process of great importance in planetary atmospheres. This process is difficult to study experimentally because of the need to determine the dependence of the product electronic states and kinetic energies upon the vibrational distribution of the ion and electron temperature. The knowledge of these characteristics of DR is needed to accurately model planetary ionospheres. Using a theoretical quantum chemical approach, the generation of O(1S) from DR was studied in detail.

Guberman, Steven L.↗

NASA NTRS1991

Theoretical studies of important processes in planetary and comet atmospheres

The dissociative recombination (DR) of the AB(+) molecular ion with an electron has been shown to be an important component in the detailed interpretation of planetary ionosphere data. A first principles theoretical approach is developed for calculating the DR cross sections and rates for AB(+) molecular ions. The calculations focus on O2(+) and N2(+) DR, and are the first to include the indirect DR mechanism (Ryberg vibrational levels below v = 0 level of ion) for a molecule larger than H2(+). The importance of electron capture width in calculating the cross sections and rates is also examined. Electron capture widths are given for all states of O2 that are of importance to DR (lowest 10 vibrational levels of ion). Knowledge of the details of dissociative recombination will be needed for interpretation of data from future interplanetary and comet atmospheric studies.

Guberman, Steven L.↗

NASA NTRS1985

A very important process of nucleosynthesis in stars

When some nuclei are free from strong gravitational field, they are unstable and will become stable nuclei by competitions of following processes: (1) neutron-evaporation; (2) spontaneous fission; and (3) beta prime 3-decay. At the initial stage, (1) and (2) are important and (3) can be ignored. The qualitative results are as follows: (1) it seems that nuclei with A 100 come from the spontaneous fission and beta prime decay of neutron-evaporated nuclei with A similiar to 140-440, which can replace the r-process; (2) the super-heavy elements with Z=114--126 (A similiar to 330--360) can be formed. They can be observed in cosmic rage if they have the halftime T 10 to the 7th poweer years; (3) the peak in the rare-earth elements comes from the symmetric fission of super-heavy elements; (4) there are more neutron-rich nuclei in the fragments; and (5) the abundances of a 83 elements in cosmic rays are one order of magnitude higher than that in the solar system.

Yu, C.↗

NASA NTRS1991

Theoretical studies of important processes in planetary and comet atmospheres

This is the fifth semi-annual progress report describing research on dissociative recombination reactions in planetary and comet atmospheres. The Appendix has two papers that describe NASA supported research. Both papers have been recently accepted for publication. The first paper, 'The Generation of O(S-1) from the Dissociative Recombination of O2(+)', describes in detail the Multichannel Quantum Defect (MQDT) theory used for the calculation of dissociative recombination (DR) cross sections and rates. The application to the generation of the upper state of the atomic oxygen green line emission is of great importance to the modelling of planetary atmospheres. The second paper in the Appendix, 'Dissociative Recombination of the Ground State of N2(+)', applies the methods described in the first paper to N2(+). We find remarkable agreement with the prior microwave afterglow experiments for both the total recombination rate and for its electron temperature dependence. However, the results disagree with recent merged beams results which gave cross sections that are a factor of five below the microwave afterglow experiments and the current results. DR of N2(+) is an important mechanism for generating energetic N atoms which can escape the atmosphere of Mars. Currently we are also continuing additional work on the DR of O2(+) which is aimed at calculating both the total DR rate as a function of ion vibrational level and the rate for production of O(D-1).

Guberman, Steven L.↗

NASA NTRS2005

Emission Process I

Important processes in X-ray plasmas are: 1. Ionization: Electron/proton collisions. Electron/proton (photoionization). innershell ionization. 2. Recombination: Radiative. Dielectronic. Charge exchange. 3. Excitation/Decay: Electron/proton collisions. Photoexcitation. Radiative decay.

Smith, Randall K.↗

NASA NTRS1990

An analysis of CCD images of the coma of Comet Halley

The analysis of selected CCD images of the coma of comet P/Halley is presented. The images were taken using specially designed filters that isolate regions of a comet's spectrum such that only sunlight which has been scattered by the dust in the coma is recorded. The modeling analysis objective is to make use of the skills developed in the development of Monte Carlo particle trajectory models for the distributions of gas species in cometary comae and to use those models as a basis for a new dust coma model. This model will include a self-consistant picture of the time-dependent dusty-gas dynamics of the inner coma and the three-dimensional time-dependent trajectories of the dust particles under the influence of solar gravity and solar radiation pressure in the outer coma. The model is intended to be used as a tool to analyze selected images from the two sets of CCD images with the hope that it will help the understanding of the effects of a number of important processes on the spatial morphology of the observed dust coma. The processes of importance to the observed dust coma include: (1) the dust particle size distribution function; (2) the terminal velocities of various sized dust particles in the inner coma; (3) the radiation scattering properties of dust particles, which are important both in terms of the observe scattered radiation and the radiation pressure acceleration on dust particles; (4) the fragmentation and/or vaporization of dust particles; and (5) the relative importance of CHON and silicate dust particles as they contribute both to the dusty-gasdynamics in the inner coma (that produce the dust particle terminal velocities) and to the observed spatial morphology on the outer dust coma.

Combi, Michael↗

NASA NTRS1992

Analysis of CCD images of the coma of comet P/Halley

The modeling analysis objective of this project is to make use of the skill acquired in the development of Monte Carlo particle trajectory models for the distributions of gas species in cometary comae as a basis for a new dust coma model. This model will include a self-consistent picture of the time-dependent dusty-gas dynamics of the inner coma and the three-dimensional time-dependent trajectories of the dust particles under the influence of solar gravity and solar radiation pressure in the outer coma. Our purpose is to use this model as a tool to analyze selected images from two sets of data of the comet P/Halley with the hope that we can help to understand the effects of a number of important processes on the spatial morphology of the observed dust coma. The study will proceed much in the same way as our study of the spatially extended hydrogen coma where we were able to understand the spatial morphology of the Lyman-alpha coma in terms of the partial thermalization of the hot H atoms produced by the photodissociation of cometary H2O and OH. The processes of importance to the observed dust coma include: (1) the dust particle size distribution function; (2) the terminal velocities of various sized dust particles in the inner coma; (3) the radiation scattering properties of dust particles, which are important both in terms of the observed scattered radiation and the radiation pressure acceleration on dust particles; (4) the fragmentation and/or vaporization of dust particles; (5) the relative importance of CHON and silicate dust particles as they contribute both to the dusty-gas dynamics in the inner coma (that produce the dust particle terminal velocities) and to the observed spatial morphology of the outer dust coma; and (6) the time and direction dependence of the source of dust.

Combi, Michael R.↗

NASA NTRS1988

Deciphering Martian climatic history using returned samples

By necessity, a Mars sample return mission must sample the upper few meters of the Martian surface. This material was subjected to a wide variety of physical processes. Presently, the most important processes are believed to be wind-driven erosion and deposition, and water ice accumulation at higher latitudes. A sample return mission represents an opportunity to better understand and quantify these important geological processes. By obtaining sample cores at key locations, it may be possible to interpret much of recent Martian climatic history.

Paige, D. A.↗

NASA NTRS1986

Carbon exchange between the mantle and the crust and its effect upon the atmosphere: Today compared to Archean time

Paleobiologists now recognize that the Earth's biosphere has been profoundly affected by geologic processes. One very important process is the dissipation of heat which has been generated by radioactivity and/or stored within the earth. Heat flow is responsible for crustal movements and therefore it is the principal architect for constructing the environments (e.g. shallow marine, continental, etc.) wherein life developed and flourished. Heat flow has also influenced the movements of volatile elements (e.g. C, N, H, S, rare gases, etc.) both within the Earth's crust and between the crust and mantle. The inventory of these elements in the Earth's crust is important, not just because some of them constitute the building blocks of organic matter, but also because they influence the biosphere's climate. The purpose of this work is to evaluate how the decline of heat flow over the course of the Earth's history has influenced the carbon inventory in the Earth's crust. Such an evaluation must first consider whether the rate at which carbon is presently being exchanged between the mantle and crust is sufficient to play an important role in controlling the crustal inventory. Secondly, this exchange of carbon must be reevaluated in the context of the Precambrian Earth's environment. One very important consideration is that the upper mantle was perhaps 300 C hotter 3 b.y. ago than it is today.

Desmarais, D.↗

NASA NTRS2003

Laboratory Studies of Homogeneous and Heterogeneous Chemical Processes of Importance in the Upper Atmosphere

The objective of this study was to conduct measurements of chemical kinetics parameters for reactions of importance in the stratosphere and upper troposphere, and to study the interaction of trace gases with ice surfaces in order to elucidate the mechanism of heterogeneous chlorine activation processes, using both a theoretical and an experimental approach. The measurements were carried out under temperature and pressure conditions covering those applicable to the stratosphere and upper troposphere. The main experimental technique employed was turbulent flow-chemical ionization mass spectrometry, which is particularly well suited for investigations of radical-radical reactions.

Molina, Mario J.↗

NASA NTRS2001

Laboratory Studies of Homogeneous and Heterogeneous Chemical Processes of Importance in the Upper Atmosphere

The objective of this study is to conduct measurements of chemical kinetics parameters for reactions of importance in the stratosphere and upper troposphere, and to study the interaction of trace gases such as HCl with ice surfaces in order to elucidate the mechanism of heterogeneous chlorine activation processes, using both a theoretical and an experimental approach. The measurements will be carried out under temperature and pressure conditions covering those applicable to the stratosphere and upper troposphere. The techniques to be employed include turbulent flow - chemical ionization mass spectrometry, and optical ellipsometry. The next section summarizes our research activities during the second year of the project, and the section that follows consists of the statement of work for the third year.

Molina, Mario J.↗

NASA NTRS1985

Laboratory studies of atomic collision processes of importance in planetary atmospheres

A series of differential cross sections for angular scattering and charge transfer was measured. These studies employ position-sensitive detectors (PSD's) to collect collision products scattered over a wide range of angles; and the research program includes investigation of differential cross sections for total angular scattering, charge transfer, stripping, and other collisions. All of these processes can be studied with the same basic apparatus, but minor modifications in the equipment details and in the data acquisition programs and techniques are required for each individual experiment.

Stebbings, R. F.↗

NASA NTRS1984

Laboratory studies of atomic collision processes of importance in planetary atmospheres

Progress in the following research supported under NSG 7386 is reported: (1) measurement of differential cross sections for atomic and molecular collisions relevant to analysis and modeling of data from Pioneer 11, Pioneer 12, Voyager 1, and Voyager 2; (2) analysis of measured differential cross section results to provide scattering data in forms that are easy to apply to atmospheric modeling work; (3) analysis of the data to give basic information on the molecular potentials involved in the scattering process; and (4) development and initial use of apparatus to study dissociative processes in neutral molecules.

Stebbings, R. F.↗

NASA NTRS2006

The Use of RGPS Kinematic Data to Estimate Nonlinear Sea Ice Motion

In current simulations of the interaction between sea ice and its environment, large significance is placed on the deformation of the sea ice. Sea ice deformation is an important process in determining the sea ice thickness distribution across a wide range of space and time scales. Changes in the sea ice thickness distribution affect energy and mass fluxes between the atmosphere and ocean and also the strength of the ice. While most current ice models assume linear variation in the ice motion field to calculate strain, deformation of sea ice occurs through the opening, closing and shearing of ice along discrete linear features. New numerical models are being developed which explicitly account for discontinuities in ice motion, and the need for requisite data sets for model validation has emerged. Multiple buoy data sets, as well as satellite data, have been used to examine the movement and deformation of sea ice. Generally it has been found that the ice motion field has been represented well by buoy data, as well as satellite data over a broad range of scales. However, the underlying deformation (spatial variation in displacement) as represented by different data sets may vary. For the work presented here, sea ice motion In current simulations of the interaction between sea ice and its environment, large significance is placed on the deformation of the sea ice. Sea ice deformation is an important process in determining the sea ice thickness distribution across a wide range of space and time scales. Changes in the sea ice thickness distribution affect energy and mass fluxes between the atmosphere and ocean and also the strength of the ice. While most current ice models assume linear variation in the ice motion field to calculate strain, deformation of sea ice occurs through the opening, closing and shearing of ice along discrete linear features. New numerical models are being developed which explicitly account for discontinuities in ice motion, and the need for requisite data sets for model validation has emerged. Multiple buoy data sets, as well as satellite data, have been used to examine the movement and deformation of sea ice. Generally it has been found that the ice motion field has been represented well by buoy data, as well as satellite data over a broad range of scales. However, the underlying deformation (spatial variation in displacement) as represented by different data sets may vary. For the work presented here, sea ice motio

Pruis, M.↗

NASA NTRS1993

Effect of metamorphism on isolated olivine grains in CO3 chondrites

The presence of a metamorphic sequence in the CO3 chondrite group has been shown previously to result in changes in properties of chondrule silicates. However, the role of isolated olivine grains during metamorphism of these chondrites has not been addressed. Isolated olivine grains in two metamorphosed CO3 chondrites, Lance and Isna, have been investigated in this study in order to assess the compositional properties of isolated olivine grains that may be attributable to metamorphism. Compositional changes in isolated olivines with increasing petrologic subtype are very similar to changes in chondrule olivines in the same chondrites. Olivine compositions from all occurrences (chondrules, isolated grains, and matrix) converge with increasing petrologic subtype. The degree of equilibration of minor elements is qualitatively related to the diffusion rate of each element in olivine, suggesting that diffusion-controlled processes are the most important processes responsible for compositional changes within the metamorphic sequence. The data are consistent with metamorphism taking place in a closed system on the CO3 chondrite parent body. Fe-poor olivine grains in metamorphosed chondrites are characterized by an Fe-rich rim, which is the result of diffusion of Fe into the grains from Fe-rich matrix. In some instances, 'complex', Fe-rich rims have been identified, which appear to have originated as igneous overgrowths and subsequently to have been overprinted by diffusion processes during metamorphism. Processes experienced by CO3 chondrites are more similar to those experienced by the ordinary chondrites than to those encountered by other carbonaceous chondrites, such as the CV3 group.

Jones, Rhian H.↗

NASA NTRS2001

Soil Moisture and Snow Cover: Active or Passive Elements of Climate?

A key question in the study of the hydrologic cycle is the extent to which surface effects such as soil moisture and snow cover are simply passive elements or whether they can affect the evolution of climate on seasonal and longer time scales. We have constructed ensembles of predictability studies using the NCAR CCM3 in which we compared the relative roles of initial surface and atmospheric conditions over the central and western U.S. GAPP region in determining the subsequent evolution of soil moisture and of snow cover. We have also made sensitivity studies with exaggerated soil moisture and snow cover anomalies in order to determine the physical processes that may be important. Results from simulations with realistic soil moisture anomalies indicate that internal climate variability may be the strongest factor, with some indication that the initial atmospheric state is also important. The initial state of soil moisture does not appear important, a result that held whether simulations were started in late winter or late spring. Model runs with exaggerated soil moisture reductions (near-desert conditions) showed a much larger effect, with warmer surface temperatures, reduced precipitation, and lower surface pressures; the latter indicating a response of the atmospheric circulation. These results suggest the possibility of a threshold effect in soil moisture, whereby an anomaly must be of a sufficient size before it can have a significant impact on the atmospheric circulation and hence climate. Results from simulations with realistic snow cover anomalies indicate that the time of year can be crucial. When introduced in late winter, these anomalies strongly affected the subsequent evolution of snow cover. When introduced in early winter, however, little or no effect is seen on the subsequent snow cover. Runs with greatly exaggerated initial snow cover indicate that the high reflectivity of snow is the most important process by which snow cover can impact climate, through lower surface temperatures and increased surface pressures. In early winter, the amount of solar radiation is very small and so this albedo, effect is inconsequential while in late winter, with the sun higher in the sky and period of daylight longer, the effect is much stronger. The results to date were obtained for model runs with present-day conditions. We are currently analyzing runs made with projected forcings for the 21st century to see if these results are modified in any way under likely scenarios of future climate change.

Oglesby, Robert J.↗