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NASA NTRS1996

ATMOS/ATLAS-3 Observations of Long-Lived Tracers and Descent in the Antarctic Vortex in November 1994

Observations of the long-lived tracers N2O, CH4 and HF obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument in early November 1994 are used to estimate average descent rates during winter in the Antarctic polar vortex of 0.5 to 1.5 km/month in the lower stratosphere, and 2.5 to 3.5 km/month in the middle and upper stratosphere. Descent rates inferred from ATMOS tracer observations agree well with theoretical estimates obtained using radiative heating calculations. Air of mesospheric origin (N2O less than 5 ppbV) was observed at altitudes above about 25 km within the vortex. Strong horizontal gradients of tracer mixing ratios, the presence of mesospheric air in the vortex in early spring, and the variation with altitude of inferred descent rates indicate that the Antarctic vortex is highly isolated from midlatitudes throughout the winter from approximately 20 km to the stratopause. The 1994 Antarctic vortex remained well isolated between 20 and 30 km through at least mid-November.

Abrams, M. C.↗
NASA NTRS1996

Stratospheric Chlorine partitioning: Constraints from Shuttle-borne Measurements of [HCl], [ClNO3] and [ClO]

Measured stratospheric mixing ratios of HCl, ClNO3, and ClO from ATMOS and MAS are poorly reproduced by models using recommended kinetic parameters. This discrepancy is not resolved by new rates for the reactions Cl+CH4 and OH+HCl derived from weighted fits to laboratory measurements. A deficit in modeled [HCl] and corresponding overprediction of [ClNO3] and [ClO], which increases with altitude, suggests that production of HCl between 20 and 50 km is much faster than predicted from recommended rates.

Michelsen, H. A.↗
NASA NTRS1996

ATMOS/ATLAS-3 Measurements of Stratospheric Chlorine and Reactive Nitrogen Partitioning Inside and Outside the November 1994 Antarctic Vortex

Partitioning between HCl and ClONO2 and among the main components of the reactive nitrogen family (NO, NO2, HNO3, ClONO2, N2O5, and HO2NO2) has been studied inside and outside the Antarctic stratospheric vortex based on ATMOS profiles measured at sunrise during the 3-12 November 1994 ATLAS-3 Shuttle mission. Elevated mixing ratios of HCl in the lower stratosphere with a peak of approximately 2.9 ppbv (10(exp -9) parts per volume) were measured inside the vortex near 500 K potential temperature (approximately 19 km). Maximum ClONO2 mixing ratios of approximately 1.2, approximately 1.4, and approximately 0.9 ppbv near 700 K (approximately 25 km) were measured inside, at the edge, and outside the vortex, respectively. Model calculations reproduce the higher levels of HCl and NO(x) (NO + NO2) inside the lower stratospheric vortex both driven by photochemical processes initiated by low O3. The high HCl at low O3 results from chemical production of HC1 via the reaction of enhanced Cl with CH4, limited production of ClONO2, and the descent of inorganic chlorine from higher altitudes.

Rinsland, C. P.↗
NASA NTRS1996

Stratospheric Observations of CH3D and HDO from ATMOS Infrared Solar Spectra: Enrichments of Deuterium in Methane and Implications for HD

Stratospheric mixing ratios of CH3D from 100 mb to 17mb (approximately equals 15 to 28 km)and HDO from 100 mb to 10 mb (approximately equals 15 to 32 km) have been inferred from high resolution solar occultation infrared spectra from the Atmospheric Trace MOlecule Spectroscopy (ATMOS) Fourier-transform interferometer. The spectra, taken on board the Space Shuttle during the Spacelab 3 and ATLAS-1, -2, and -3 missions, extend in latitude from 70 deg S to 65 deg N. We find CH3D entering the stratosphere at an average mixing ratio of (9.9 +/- 0.8) x 10(exp -10) with a D/H ratio in methane (7.1 +/- 7.4)% less than that in Standard Mean Ocean Water (SMOW) (1 sigma combined precision and systematic error). In the mid to lower stratosphere, the average lifetime of CH3D is found to be (1.19 +/- 0.02) times that of CH4, resulting in an increasing D/H ratio in methane as air 'ages' and the methane mixing ratio decreases. We find an average of (1.0 +/- 0.1) molecules of stratospheric HDO are produced for each CH3D destroyed (1 sigma combined precision and systematic error), indicating that the rate of HDO production is approximately equal to the rate of CH3D destruction. Assuming negligible amounts of deuterium in species other than HDO, CH3D and HD, this limits the possible change in the stratospheric HD mixing ratio below about 10 mb to be +/- 0.1 molecules HD created per molecule CH3D destroyed.

Irion, F. W.↗
NASA NTRS1993

Stratospheric NO(y) Measurements on the NASA DC-8 during AASE 2

We survey measurements of stratospheric NO(y) on the NASA DC-8 during AASE 2 in early 1992. Emphasis is on correlations with other long-lived species: O3, N2O, and CH4. No cases of extremely high NO(y)/O3 ratios were seen in 1992. This suggests that denitrification at higher altitudes was less pervasive than in 1989. Values of NO(y)/O3 in 1992 are comparable to, though perhaps lower than, those measured in 1989. The correlation of NO(y) with N2O changes over the course of the mission. Relative to the correlation for the whole season, low values of NO(y) occur in February, most notably on the 22nd. The reason for the low NO(y) is unknown It is generally too warm at DC-8 altitudes for the presence of PSC particles, but denitrification at higher altitudes, followed by descent, might account for the low values seen on 22 February. However, this may be unlikely since the NASA ER-2, flying during the same period, saw no evidence of denitrification at higher altitudes.

Weinheimer, A. J.↗
NASA NTRS1996

Scientific Studies in Association with the Halogen Occultation Experiment

This work examines measurements of ozone, NO, NO2, and HCl made by the Halogen Occultation Experiment (HALOE) to track chemical change in the stratosphere. In addition, HALOE observations of two long-lived species, HF and CH4, are used as tracers to distinguish between change due to transport processes and change due to chemistry. The first study investigates the response of NO(x), (NO and NO2) and ozone to the presence of large amounts of sulfate aerosol in the stratosphere following the 1991 eruption of Mount Pinatubo. As the Pinatubo aerosol cleared the atmosphere at 17 mb (about 27-28 km), the partitioning of total reactive nitrogen shifted more toward NO(x), and ozone amounts declined. This trend is opposite that observed at lower altitudes. The second study examines the chemical aftermath of severe ozone depletion over Antarctica in spring. When ozone levels drop to a threshold amount (about 1 ppm near 20 km), the partitioning of the total chlorine family shifts rapidly from reactive species to the reservoir molecule HCl. This sudden repartitioning shuts down further ozone loss and may be significant as filaments of air peel off the polar vortex and mix with mid-latitude air.

Mickley, Lorretta J.↗
NASA NTRS1996

Observations and Analysis of Atmospheric Hydroxyl

Ground-based measurements of sunlight absorption at the OH P(sub 1)(l) resonance line at 308 nm have been made on a continuous basis at Fritz Peak, Colorado. The derived OH vertical column abundances show the persistence of a new seasonal regime which began in 1991. The fall minimum has been consistently depressed about 10-15% below the 1980-1990 average fall values. While the initial onset of depressed fall abundances occurred a few months after the Pinatubo eruption, there has been no fall OH recovery correlating with decreased amounts of volcanic aerosol found since spring 1993. The Colorado data also continues to exhibit an AM-PM asymmetry which varies seasonally, approximately in phase with local total ozone. These observations were presented at the Front Range AGU meeting in February 1996 and were published in Geophysical Research Letters in July 1996 (preprint enclosed). An update through the fall of 1996, when morning abundances were found to be extremely low, was presented at the Fall 1996 AGU meeting (abstract attached). A PEPSIOS instrument of identical design is currently operational and has been used since April 1996 for OH column measurements at New Mexico Tech, Socorro, NM. Title for both instruments was transferred from Florida Atlantic University to New Mexico Tech in February of 1996. Comparative measurements from the two instruments for April-July 1996 indicate small differences in OH column abundances, with New Mexico (34 deg N) abundances about 10% above Colorado (40 deg N) values for comparable solar zenith angles. A more detailed comparison will require at least one full year of data from both locations. New Mexico measurements were obtained on June 10, 1996, concurrently with a balloon launch of the NASA STRAT mission from Fort Sumner, New Mexico. We hope to make use of STRAT measurements H2O, CH4, and O3 which are particularly relevant to OH photochemistry. Additional work at New Mexico Tech involves a comparison of P(sub 1)(1) and Q(sub 1)(3) absorption by the method of Doppler shift of solar limb spectra. These are being used to infer path weighted temperatures and for validations studies on the standard method of analysis using the single P(sub 1)(1) line. Results were presented at the Fall 1996 AGU meeting (abstract attached). A graduate student in the Physics Department at New Mexico Tech has been supported since August 1996. The student is investigating column OH behavior using the NCAR 2-D model of the middle atmosphere. Graduate student support was not available until the start of the second year (Nov. 15, 1996), therefore funds have been transferred from the allocation for the research associate, who resigned from the project July 1, 1996.

Minschwaner, Ken R.↗
NASA NTRS1997

Planetary Habitability

This grant was entitled 'Planetary Habitability' and the work performed under it related to elucidating the conditions that lead to habitable, i.e. Earth-like, planets. Below are listed publications for the past two and a half years that came out of this work. The main thrusts of the research involved: (1) showing under what conditions atmospheric O2 and O3 can be considered as evidence for life on a planet's surface; (2) determining whether CH4 may have played a role in warming early Mars; (3) studying the effect of varying UV levels on Earth-like planets around different types of stars to see whether this would pose a threat to habitability; and (4) studying the effect of chaotic obliquity variations on planetary climates and determining whether planets that experienced such variations might still be habitable. Several of these topics involve ongoing research that has been carried out under a new grant number, but which continues to be funded by NASA's Exobiology program.

Kasting, James F.↗
NASA NTRS1997

Land-Use Change, Soil Process and Trace Gas Fluxes in the Brazilian Amazon Basin

We measured changes in key soil processes and the fluxes of CO2, CH4 and N2O associated with the conversion of tropical rainforest to pasture in Rondonia, a state in the southwest Amazon that has experienced rapid deforestation, primarily for cattle ranching, since the late 1970s. These measurements provide a comprehensive quantitative picture of the nature of surface soil element stocks, C and nutrient dynamics, and trace gas fluxes between soils and the atmosphere during the entire sequence of land-use change from the initial cutting and burning of native forest, through planting and establishment of pasture grass and ending with very old continuously-pastured land. All of our work is done in cooperation with Brazilian scientists at the Centro de Energia Nuclear na Agricultura (CENA) through an extant official bi-lateral agreement between the Marine Biological Laboratory and the University of Sao Paulo, CENA's parent institution.

Melillo, Jerry M.↗
NASA NTRS1997

Plasma-Sprayed Refractory Oxide Coatings on Silicon-Base Ceramics

Silicon-base ceramics are promising candidate materials for high temperature structural applications such as heat exchangers, gas turbines and advanced internal combustion engines. Composites based on these materials are leading candidates for combustor materials for HSCT gas turbine engines. These materials possess a combination of excellent physical and mechanical properties at high temperatures, for example, high strength, high toughness, high thermal shock resistance, high thermal conductivity, light weight and excellent oxidation resistance. However, environmental durability can be significantly reduced in certain conditions such as when molten salts, H2 or water vapor are present. The oxidation resistance of silicon-base materials is provided by SiO2 protective layer. Molten salt reacts with SiO2 and forms a mixture of SiO2 and liquid silicate at temperatures above 800C. Oxygen diffuses more easily through the chemically altered layer, resulting in a catastrophic degradation of the substrate. SiC and Si3N4 are not stable in pure H2 and decompose to silicon and gaseous species such as CH4, SiH, SiH4, N2, and NH3. Water vapor is known to slightly increase the oxidation rate of SiC and Si3N4. Refractory oxides such as alumina, yttria-stabilized zirconia, yttria and mullite (3Al2O3.2SiO2) possess excellent environmental durability in harsh conditions mentioned above. Therefore, refractory oxide coatings on silicon-base ceramics can substantially improve the environmental durability of these materials by acting as a chemical reaction barrier. These oxide coatings can also serve as a thermal barrier. The purpose of this research program has been to develop refractory oxide chemical/thermal barrier coatings on silicon-base ceramics to provide extended temperature range and lifetime to these materials in harsh environments.

Tewari, Surendra↗
NASA NTRS1995

Photochemistry of Triton's Atmosphere and Ionosphere

The photochemistry of 32 neutral and 21 ion species in Triton's atmosphere is considered. Parent species N2, CH4, and CO (with a mixing ratio of 3 x 10(exp -4) in our basic model) sublime from the ice with rates of 40, 208, and 0.3 g/sq cm/b.y., respectively. Chemistry below 50 km is driven mostly by photolysis of methane by the solar and interstellar medium Lyman-alpha photons, producing hydrocarbons C2H4, C2H6, and C2H2 which form haze particles with precipitation rates of 135, 28, and 1.3 g/sq cm/b.y., respectively. Some processes are discussed which increase the production of HCN (by an order of magnitude to a value of 29 g/sq cm/b.y.) and involve indirect photolysis of N2 by neutrals. Reanalysis of the measured methane profiles gives an eddy diffusion coefficient K = 4 x 10(exp 3)sq cm/s above the tropopause and a more accurate methane number density near the surface, (3.1 +/- 0.8)x IO(exp 11)/cu cm. Chemistry above 200 km is driven by the solar EUV radiation (lambda less than 1000 A) and by precipitation of magnetospheric electrons with a total energy input of 10(exp 8) W (based on thermal balance calculations). The most abundant photochemical species are N, H2, H, 0, and C. They escape with the total rates of 7.7 x 10(exp 24)/ s, 4.5 x 10(exp 25)/s, 2.4 x 10(exp 25)/s, 4.4 x 10(exp 22)/s, and 1.1 x 10(exp 24), respectively. Atomic species are transported to a region of 50-200 km and drive the chemistry there. Ionospheric chemistry explains the formation of an E region at 150-240 km with HCO(+) as a major ion, and of an F region above 240 km with a peak at 320 km and C(+) as a major ion. The ionosphere above 500 km consists of almost equal densities of C(+) and N(+) ions. The model profiles agree with the measured atomic nitrogen and electron density profiles. A number of other models with varying rate coefficients of some reactions, differing properties of the haze particles (chemically passive or active), etc., were developed. These models show that there are four basic unknown values which have strong impacts on the composition and structure of the atmosphere and ionosphere. These values and their plausible ranges are the CO mixing ratio f(sub co) = 10(exp -4) - 10(exp -3), the magnetospheric electron energy input (1 +/- 0.5) x 10(exp 8) W, the rate coefficient of charge-exchange reaction N2(+) + C(kappa) = 10(exp -11) - 10(exp -10)cu cm/s, and the ion escape velocity upsilon(sub i) approx. equals 150 cm/s.

Krasnopolsky, Vladimir A.↗
NASA NTRS1995

Photochemistry of Triton's Atmosphere and Ionosphere

The photochemistry of 32 neutral and 21 ion species in Triton's atmosphere is considered. Parent species N2, CH4, and CO (with a mixing ratio of 3 x 10(exp -4) in our basic model) sublime from the ice with rates of 40, 208, and 0.3 g/sq cm/b.y., respectively. Chemistry below 50 km is driven mostly by photolysis of methane by the solar and interstellar medium Lyman-alpha photons, producing hydrocarbons C2H4, C2H6, and C2H2 which form haze particles with precipitation rates of 135, 28, and 1.3 g/sq cm/b.y., respectively. Some processes are discussed which increase the production of HCN (by an order of magnitude to a value of 29 g/sq cm/b.y.) and involve indirect photolysis of N2 by neutrals. Reanalysis of the measured methane profiles gives an eddy diffusion coefficient K = 4 x 10(exp 3) sq cm/s above the tropopause and a more accurate methane number density near the surface, (3.1 +/- 0.8) x 10(exp 11)/cc cm. Chemistry above 200 km is driven by the solar EUV radiation (lambda less than 1000 A)) and by precipitation of magnetospheric electrons with a total energy input of 10(exp 8) W (based on thermal balance calculations). The most abundant photochemical species are N, H2, H, O, and C. They escape with the total rates of 7.7 x 10(exp 24)/ s, 4.5 x 10(exp 25)/ s, 2.4 x 10(exp 25)/ s, 4.4 x 10(exp 22)/ s, and 1.1 x 10(exp 24)/ s, respectively. Atomic species are transported to a region of 50-200 km and drive the chemistry there. Iono- spheric chemistry explains the formation of an E region at 150-240 km with HCO(+) as a major ion, and of an F region above 240 km with a peak at 320 km and C(+) as a major ion. The ionosphere above 500 km consists of almost equal densities of C(+) and N(+) ions. The model profiles agree with the measured atomic nitrogen and electron density profiles. A number of other models with varying rate coefficients of some reactions, differing properties of the haze particles (chemically passive or active), etc., were developed. These models show that there are four basic unknown values which have strong impacts on the composition and structure of the atmosphere and ionosphere. These values and their plausible ranges are the CO mixing ratio f(sub co) = 10(exp -4)- 10(exp -3), the magnetospheric electron energy input (1 +/- 0.5) x 10(exp 8) W, the rate coefficient of charge-exchange reaction N2(+) + Ck = 10(exp -11)-10(exp -10)cc cm/s, and the ion escape velocity upselon(sub i) approx. 150 cm/s.

Krasnopolsky, Vladimir A.↗
NASA NTRS1995

Organic Compounds Produced by Photolysis of Realistic Interstellar and Cometary Ice Analogs Containing Methanol

The InfraRed (IR) spectra of UltraViolet (UV) and thermally processed, methanol-containing interstellar / cometary ice analogs at temperatures from 12 to 300 K are presented. Infrared spectroscopy, H-1 and C-13 Nuclear Magnetic Resonance (NMR) spectroscopy, and gas chromatography-mass spectrometry indicate that CO (carbon monoxide), CO2 (carbon dioxide), CH4 (methane), HCO (the formyl radical), H2CO (formaldehyde), CH3CH2OH (ethanol), HC([double bond]O)NH2 (formamide), CH3C([double bond]O)NH2 (acetamide), and R[single bond]C[triple bond]N (nitriles) are formed. In addition, the organic materials remaining after photolyzed ice analogs have been warmed to room temperature contain (in rough order of decreasing abundance), (1) hexamethylenetetramine (HMT, C6H12N4), (2) ethers, alcohols, and compounds related to PolyOxyMethylene (POM, ([single bond]CH2O[single bond](sub n)), and (3) ketones (R[single bond]C([double bond]O)[single bond]R') and amides (H2NC([double bond]O)[single bond]R). Most of the carbon in these residues is thought to come from the methanol in the original ice. Deuterium and C-13 isotopic labeling demonstrates that methanol is definitely the source of carbon in HMT. High concentrations of HMT in interstellar and cometary ices could have important astrophysical consequences. The ultraviolet photolysis of HMT frozen in H2O ice readily produces the 'XCN' band observed in the spectra of protostellar objects and laboratory ices, as well as other nitriles. Thus, HMT may be a precursor of XCN and a source of CN in comets and the interstellar medium. Also, HMT is known to hydrolyze under acidic conditions to yield ammonia, formaldehyde, and amino acids. Thus, HMT may be a significant source of prebiogenic compounds on asteroidal parent bodies. A potential mechanism for the radiative formation of HMT in cosmic ices is outlined.

Bernstein, Max P.↗
NASA NTRS1997

High Pressure Gas Permeation and Liquid Diffusion Studies of Coflon and Tefzel Thermoplastics

The life of fluid-carrying flexible or umbilical pipes during service at elevated temperatures and pressures depends inter alia on their resistance to attack by the fluids present and the rate at which these fluids are absorbed by the pipe lining materials. The consequences of fluid ingress into the thermoplastic lining could mean a) a reduction in its mechanical strength, to increase chances of crack formation and growth and thus a loss of integrity, b) the occurrence of permeation right through the lining material, with pressure build- up in the outer pipe wall construction (of flexible pipes) or chemical attack (from a hostile permeant) on outer layers of reinforcements. Therefore it is important within this project to have relevant permeation data for Coflon and Tefzel thermoplastics: the former is plasticised, the latter is not. A previous report (CAPP/M.2) described experimental equipment and techniques used by MERL when measuring high pressure (up to 5000 psi) gas permeation and liquid diffusion through thermoplastic samples cut from extruded bar or pipe, and provided the basic theory involved. Norsk Hydro are also performing gas permeation tests on pipe sections, at up to 100 bars (1450 psi) pressure or so, and reporting separately. Some comparisons between data from Norsk Hydro and MERL have been made herein. The tests should be considered as complementary, as the Norsk Hydro test has the obvious benefit of using complete pipe sections, whilst MERL can test at much higher pressures, up to 1000 bar if necessary. The sophisticated analytical measuring equipment of Norsk Hydro can distinguish the individual components of mixed gases and hence the various permeation-linked coefficients whereas MERL, in using pressure increase at constant volume to determine permeation rate, is limited to obtaining single gas data, or apparent (or representative) coefficients for a mixed gas as a whole. Except for the initial fluid diffusion data for Tefzel described in CAPP/M.2, the present report covers all aspects of fluid permeation and diffusion for Coflon and Tefzel, including all the pen-neation data accumulated in the project to date. Test gases have mainly been methane (CH4) and carbon dioxide (CO2). More high pressure (HP) gas permeation tests have been performed since the last issue of this report, most being concerned with changes in permeation characteristics brought about by ageing in various relevant fluids. This revision supersedes previous issues.

Morgan, G. J.↗
NASA NTRS1996

Radioactive Transfer Models for Saturn and Titan

The infrared spectra of the earth's atmosphere and planetary atmospheres contains information about atmospheric physical and chemical processes. Atmospheric molecular constituents absorb and emit infrared radiation by rotational and vibrational transition. Observed spectra exhibit characteristic features in the electromagnetic spectrum region. Observation of the absorption or thermal emission spectra may be obtained with space-borne high resolution infrared spectrometers in the 10-5000 cm(exp -1) (2-1000 micro-m) spectral region. Information about the atmospheric thermal structure, composition, and the chemical and physical processes of the observed spectral was accomplished. A preliminary version of a P-T retrieval algorithm for Saturn using all three modes for temperature inversion, e.g., CH4-limb, and H2-nadir spectra was completed and tested for accuracy. Radiative transfer and inversion programs were studied and analyzed for applications to infrared limb thermal emission observations of Saturn and Titan from the Cassini Orbiter, as well as Earth's atmosphere. Analysis and modification of the existing radiative transfer and inversion programs for Earth and planetary atmospheres are being made. Data analysis and retrieval of information form the observations by digital calculations were carried out at UAH and MSFC computer. The working program for generating and reading g-k arrays for using the c-k arrays via the c-k method for radiative transfer calculations for desired atmospheric and instrumental parameters was completed, tested for accuracy and resides at the MSFC computer.

Wu, S. T.↗
NASA NTRS1996

Development of a Land Use Mapping and Monitoring Protocol for the High Plains Region: A Multitemporal Remote Sensing Application

The purpose of this project was to develop a practical protocol that employs multitemporal remotely sensed imagery, integrated with environmental parameters to model and monitor agricultural and natural resources in the High Plains Region of the United States. The value of this project would be extended throughout the region via workshops targeted at carefully selected audiences and designed to transfer remote sensing technology and the methods and applications developed. Implementation of such a protocol using remotely sensed satellite imagery is critical for addressing many issues of regional importance, including: (1) Prediction of rural land use/land cover (LULC) categories within a region; (2) Use of rural LULC maps for successive years to monitor change; (3) Crop types derived from LULC maps as important inputs to water consumption models; (4) Early prediction of crop yields; (5) Multi-date maps of crop types to monitor patterns related to crop change; (6) Knowledge of crop types to monitor condition and improve prediction of crop yield; (7) More precise models of crop types and conditions to improve agricultural economic forecasts; (8;) Prediction of biomass for estimating vegetation production, soil protection from erosion forces, nonpoint source pollution, wildlife habitat quality and other related factors; (9) Crop type and condition information to more accurately predict production of biogeochemicals such as CO2, CH4, and other greenhouse gases that are inputs to global climate models; (10) Provide information regarding limiting factors (i.e., economic constraints of pumping, fertilizing, etc.) used in conjunction with other factors, such as changes in climate for predicting changes in rural LULC; (11) Accurate prediction of rural LULC used to assess the effectiveness of government programs such as the U.S. Soil Conservation Service (SCS) Conservation Reserve Program; and (12) Prediction of water demand based on rural LULC that can be related to rates of draw-down of underground water supplies.

Price, Kevin P.↗
NASA NTRS1996

Endogenous Synthesis of Prebiotic Organic Molecules

The necessary condition for the synthesis of organic compounds on the primitive earth is the presence of reducing conditions. This means an atmosphere of CH4, CO, or CO2 + H2. The atmospheric nitrogen can be N2 with a trace of NH3, but NH4(+) is needed in the ocean at least for amino acid synthesis. Many attempts have been made to use CO2 + H2O atmospheres for prebiotic synthesis, but these give at best extremely low yields of organic compounds, except in the presence of H2. Even strong reducing agents such as FeS + H2S or the mineral assemblages of the submarine vents fail to give significant yields of organic compounds with CO2. There appears to be a high kinetic barrier to the non-biological reduction of CO2 at low temperatures using geological reducing agents. The most abundant source of energy for prebiotic synthesis is ultraviolet light followed by electric discharges, with electric discharges being more efficient, although it is not clear which was the important energy source. Photochemical process would also make significant contributions. In an atmosphere Of CO2, N2, and H2O with no H2, the production rates of HCN and H2CO would be very low, 0.001 or less than that of a relatively reducing atmosphere. The concentration of organic compounds under these non-reducing conditions would be so low that there is doubt whether the concentration mechanism would be adequate for further steps toward the origin of life. A number of workers have calculated the influx of comets and meteorites on the primitive earth as a source of organic compounds. We conclude that while some organic material was added to the earth from comets and meteorites the amount available from these sources at a given time was at best only a few percent of that from earth bases syntheses under reducing conditions.

Miller, Stanley L.↗
NASA NTRS1961

Stability of Titanium Nitride and Titanium Carbide When Exposed to Hydrogen Atoms from 298 to 1950 K

Titanium nitride and titanium carbide deposited on tungsten wires were exposed to hydrogen atoms (10(exp -4) atm pressure) produced by the action of microwave radiation on molecular hydrogen. The results of these experiments in the temperature range 298 to 1950 K indicate that no appreciable reaction takes place between atomic hydrogen and TiN or TiC. The formation of reaction products (NH3, CH4, C2H2) should be favored at lower temperatures. However, because of the high catalytic activity of Ti for H atom recombination, the rate of such reactions with H atoms is controlled by the rate of evaporation of Ti from the surface, this rate being low at temperatures below 1200 K. In order to interpret the stability of TiN and TiC in H atoms more fully, the stability of TiN and TiC in vacuum and H2 gas was also studied. The thermodynamic computations conform in order of magnitude to the experimentally found rates of decomposition of TiN and TiC in vacuum and are also consistent with the fact that no appreciable reaction is found with these compounds in molecular H2 at a pressure of 10(exp -3) atmosphere in the temperature range 2980 to 2060 K. When TiN or TiC was heated in atomic H or molecular H2, no reaction products other than those obtained from the simple decomposition of the nitride and carbide were observed. The gaseous products were analyzed in a mass spectrometer.

Philipp, Warren H.↗