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Stratospheric ClO and O3 vertical profiles were measured at 32-deg N in May 1985 and October 1986. The ClO profiles and diurnal variation are in general agreement with theory, but have somewhat less midday ClO near 34 km. Measured 35-45 km O3 is larger than theoretical, and no stratospheric O3 diurnal variation was observed, as expected. HNO3 was detected, and an H2O2 upper limit was obtained.
The photodissociation of pernitric acid (PNA) was studied at 248 nm. The quantum yield for production of OH radicals is 34 + or - 16 percent. The yield of OH from PNA was measured relative to that of H2O2. The translational and rotational energy content of the OH photofragment from PNA was characterized. A fluorescent emission was also observed and characterized. It is attributed to electronically excited NO2 produced in the PNA photodissociation. A maximum yield of 30 percent for NO2 production was determined. The intensity of this emission, and a mass spectrometric peak at m/e = 33, were found to be useful means of characterizing the purity of the PNA sample.
In situ stratospheric measurements of the concentrations of the reservoir species HNO3 and HCl made during two flights of the high-resolution (0.0005/cm) balloon-borne laser in situ sensor instrument from Palestine, Texas, are reported. A measured HNO3 volume mixing ratio of 4.3 parts per billion by volume (ppbv) at 31 km altitude is about 1 ppbv larger than previously reported measurements at 32 deg N. An HCl mixing ratio of 1.6 ppbv at 29 km is in agreement with values obtained from earlier remote sensing techniques within the experimental uncertainties. Upper limits at 31 km of 0.4 ppbv for H2O2 and 0.2 ppbv for HOCl are also derived from analyses of spectra recorded near 1252/cm.
Solar Mesosphere Explorer (SME) observations of the 3 a.m. 1.27 micron nightglow at 45 N latitude are reported. From the deduced volume emission rates, the O2(a 1 Delta g) nighttime production rates for the 80-100 km altitude range are derived. Utilizing the mean SME-acquired 3 p.m. ozone profile for the same latitude and time period and an updated photochemical model, nighttime O, O3, H, OH, HO2, and H2O2 profiles are determined. These are used in calculating the rates of reactions which are sufficiently exothermic to produce O2(1 Delta) or excited states of OH or HO2, which could transfer their energy to O2 to form O2(1 Delta). Yields of O2(1 Delta) based on published laboratory and observational studies are used to find that the sum of two reaction sequences can approximate the SME measurements: (1) O + O + M and (2) H + O3 followed by OH-asterisk + O2.
This paper describes the concept of a cryogenic IR imaging Fourier transform spectrometer, called the Tropospheric Emission Spectrometer (TES), designed for observations of the troposphere and lower stratosphere from a near-earth orbit, using natural thermal emission and reflected sunlight. The principal molecular species to be measured by TES are O3, CO, CO2, N2O, H2O, H2O2, NO, NO2, HNO3, NH3, CH4, C2H6, C2H2, SO2, COS, CFCl3, and CF2Cl2. The TES is scheduled for a launch on the second polar platform of the Earth Observing System in 1998.
A comparative study is made to identify the most advantageous fuel/oxidizer combinations which could be supplied to spacecraft from in situ resources or from the most economical earth-transported storable fuels. The performance of the unconventional fuel/oxidizer combinations in question are computed for a wide range of pressures, expansion ratios and initial temperatures. The propellants discussed are, (1) for LEO: H2 + O2, NH3 + N2O4; (2) for the moon: CH4 + O2, SiH4 + O2, H2 + Al + O2, butyl rubber + O2, silicone + O2, and polystyrene + O2; and (3) for Mars: CO + O2, CO + H2O2, CO + N2O4, C2H5OH + O2, and CH3OH + O2.
A practical synthesis and a discussion of some chemical properties of pure strontium peroxide and calcium peroxide are presented. The general synthesis of these peroxides involves precipitation of their octahydrates by addition of H2O2 to aqueous ammoniacal Sr(NO3)2 or CaCl2. The octahydrates are converted to the anhydrous peroxides by various dehydration techniques. A new x-ray diffraction powder pattern for CaO2 x 8H2O is given from which lattice parameters a=6.212830 and c=11.0090 were calculated on the basis of the tetragonal crystal system.
When Martian regolith samples are moistened with water, a strong oxidant and oxygen gas are released. The many possible oxidants which have been suggested as present, including superoxide (O2(-)) hydrogen peroxide (H2O2(-)), and manganese (IV) oxide (MnO2), as well as peroxonitrite (ONOO(-)), can be distinguished by their ability to account for the numerous observations of the Viking Labelled Release (LR) and Gas Exchange (GEX) experiments. The magnitudes, kinetics, and heat labilities of the LR experiments and the magnitudes and heat labilities of the GEX experiments have been quantitatively replicated with peroxonitrites. Further, it is to be expected from information about the photochemistry of nitrogen in the atmosphere, the calculated fluxes of the NO(x) to the surface, the known reactions of NO(x) with carbonates to produce nitrates and photolysis studies of nitrates, that peroxonitrites are present on Mars. However, considerable uncertainty has existed about the form in which oxygen is stored in photolyzed nitrate crystals. Models have ranged from micropores of O2 to chemically bound oxygen as peroxonitrite (O2NOO(-)), as well as peroxonitrite. Studies of the solution chemistry and solid state photochemistry were completed, which show that much of the oxygen evolved on wetting comes from thermal breakdown of peroxonitrite after it is dissolved. A chemical model is developed for the photochemical processes occurring during UV irradiation of solid nitrates which resolves the several contradictory models discussed in the literature in recent years.
An extensive experimental study was conducted using various electrolytes in an effort to find an appropriate electrolyte for anodic dissolution of InP. From the analysis of electrochemical characteristics in the dark and under different illumination levels, x ray photoelectron spectroscopy and SEM/Nomarski inspection of the surfaces, it was determined that the anodic dissolution of InP front surface layers by FAP electrolyte is a very good choice for rendering smooth surfaces, free of oxides and contaminants and with good electrical characteristics. The FAP electrolyte, based on HF, CH3COOH, and H2O2 appears to be inherently superior to previously reported electrolytes for performing accurate EC-V profiling of InP at current densities of up to 0.3 mA/sq cm. It can also be used for accurate electrochemical revealing of either precipitates or dislocation density with application to EPD mapping as a function of depth, and for defect revealing of multilayer InP structures at any depth and/or at the interfaces.
Direct extraction and reaction of the 50 ppm H found in mature lunar soil with a small fraction of the 1 percent ilmenite found in even the most Ti-poor lunar soils is a viable method of producing H2O2 and H2O for propellants and life support. A plant with a mass of approximately 62 metric tons can produce about 8 metric tons of LOX and 1.2 metric tons of LH2 per month. The concept is viable in even Ti-poor regions if the soils have long exposure to solar wind. The plant processes over 29,000 tons of soil with about 50 ppm H per month. The mine that feeds the plant excavates over 8600 sq m per month with a fleet of three front-end loaders and five haulers. Trade studies demonstrate that nuclear power accompanied by a high process plant duty cycle results in a far smaller installation than a solar-powered unit.
Infrared spectra of NO2 recorded during a recent flight of the Balloon-borne Laser In-Situ Sensor instrument have been analyzed to determine sensitivity limits for various signal integration times. Implications for direct detection of ClO, HOCl, H2O2, COF2, OH, and HO2 are discussed.
The effects of dimethyl sulfide (DMS) and methyl iodide (MI) emissions are analyzed using a two-dimensional photochemical model of a marine tropical tropospheric synoptic system. The model traces the atmospheric transformation cycles of the emissions to aerosols. The study is focused on remote tropical ocean regions and includes simulations of the spatial and diurnal variations of various iodine and sulfur species, and the species OH, HO2, and H2O2. One line of analysis leads to the conclusion that the reaction IO + DMS yields DMSO + I may play a significant role in destroying DMS if it proceeds at the published fast rate. Alternative lines of analyses are presented.
The Diagnostics Testbed Facility (DTF) located at the Stennis Space Center (SSC) is used for obtaining extensive sets of H2O2 exhaust plume emission spectral data for the SSME critical components related elements and materials. The SSME related elements and materials are simulated by mixing appropriate amounts of compounds of their respective constituent elements in an aqueous solution which is injected into the combustion chamber of the DTFT. Five of the most critical components of the SSME which have experienced very severe wear and tear problems in the past are analyzed. These are high pressure turbopump (HPTP) turbine blades, HPTP turbine disks, HPTP bearing, main injector LOX posts, and the main combustion chamber structural shell. The alloys used in the manufacturing of these components are MAR-M 246 + Hf, Waspaloy X, AISI 440C, Haynes 188, and Inconel 718, respectively. The experimental setup and procedures at the DTF are described; stratospheric data for the five alloys are presented; and strategies for the material identification in the SSME exhaust plume are discussed.
The first unequivocal measurement of hydrogen peroxide in the stratosphere have been made, a concentration profile obtained from a balloon platform using Fourier transform thermal emission spectroscopy in the far infrared. Measurements were made using the 112/cm R-Q5 branch of the rotational-torsional spectrum, with some confirmation from the 94/cm R-Q4 branch. The volume mixing ratio of H2O2 is 1.6 x 10 to the -10th at 38.4 km, decreasing to 0.6 x 10 to the -10th at 23.8 km, with uncertainties of about 16 percent. These measurements are compared to a recent stratospheric model calculation.
The aim of the measurements is to obtain vertical mixing of profiles of hydrogen and halogen trace gases and to study the related processes of diurnal change, OH/HO2 ratio, and HO sub x total budget involved in stratospheric ozone. The species to be measured in the first planned 1990 flight of this new series include OH, H2O2, HO2, HOCl, HBr, HCl, HF, H2O, HDO, O3, and isotopic O3. Recent analyses have been completed for the retrieval of the OH concentration profile and the first measurement of the HBr column concentration.
How ozone, clouds, and airborne dust affect CO2 ice formation and sublimation is examined to determine if they help explain the asymmetry in the residual polar caps. The radiative flux striking the surface is calculated for 57 solar and 10 IR wavelength intervals from 0 to 100 microns including the scatering, absorption, and emission by O3, CO2, clouds, and dust. UV absorption by H2O, O2, HO2, and H2O2 is also included, as is Rayleigh scattering. The discrete ordinate method of Stamnes et al. (1988) treats the emission, scattering, and absorption of monochromatic radiation.
Possible pathways for the evolution of oxygenic photosynthesis in the early reducing atmosphere of the earth are discussed. It is suggested that the abiotic production of atmospheric oxidants could have provided a mechanism by which locally oxidizing conditions were sustained within spatially confined habitats thus removing the available reductants and forcing photosynthetic organisms to utilize water (rather than ferrous or sulfide ions) as the electron donor. It is argued that atmospheric H2O2 played the key role in inducing oxygenic photosynthesis, because, as peroxide concentrations local environments increased, primitive organisms would not only be faced with a loss of a reductant, but would be also forced to develop a biochemical apparatus (such as catalase) that would protect them against the products of oxygenic photosynthesis. This scenario allows for the early evolution of oxygenic photosynthesis at the time when global conditions were still anaerobic.
In an effort to predict the effect that turbulent mixing has on the extent of combustion, a one-equation turbulence model is added to an existing Navier-Stokes solver with finite-rate chemistry. To average the chemical-source terms appearing in the species-continuity equations, an assumed pdf approach is also used. This code was used to analyze the mixing and combustion caused by the mixing layer formed by supersonic coaxial H2-air streams. The chemistry model employed allows for the formation of H2O2 and HO2. Comparisons are made with recent measurements using laser Raman diagnostics. Comparisons include temperature and its rms, and concentrations of H2, O2, N2, H2O, and OH. In general, good agreement with experiment was noted.