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NASA NTRS1996

Seasonal Variations of Water Vapor in the Lower Stratosphere Inferred from ATMOS/ATLAS-3 Measurements of H2O and CH4

Stratospheric measurements of H2O and CH4 by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer on the ATLAS-3 shuttle flight in November 1994 have been examined to investigate the altitude and geographic variability of H2O and the quantity H = (H2O + 2CH4) in the tropics and at mid-latitudes (8 to 49 deg N) in the northern hemisphere. The measurements indicate an average value of 7.24 +/- 0.44 ppmv for H between altitudes of about 18 to 35 km, corresponding to an annual average water vapor mixing ratio of 3.85 +/- 0.29 ppmv entering the stratosphere. The H2O vertical distribution in the tropics exhibits a wave-like structure in the 16- to 25-km altitude range, suggestive of seasonal variations in the water vapor transported from the troposphere to the stratosphere. The hygropause appears to be nearly coincident with the tropopause at the time of observations. This is consistent with the phase of the seasonal cycle of H2O in the lower stratosphere, since the ATMOS observations were made in November when the H2O content of air injected into the stratosphere from the troposphere is decreasing from its seasonal peak in July-August.

Abbas, M. M.↗
NASA NTRS1996

Space-Borne H2O Observations in the Arctic Stratosphere and Mesosphere in the Spring of 1992

We report on stratospheric and mesospheric water vapor (H2O) observations obtained by the Millimeter wave Atmospheric Sounder (MAS) in the Arctic spring of 1992. In the lower stratosphere, the observations show enhanced H2O inside the vortex between 450 K and 625 K, in agreement with other H2O observations. In the upper stratosphere and lower mesosphere, at potential temperatures between 1850 K and 2200 K, we find regions of depressed H2O volume mixing ratio coincident with remnants of high potential vorticity. The depressed mesospheric H2O, as well as the enhanced lower stratospheric H2O, are consistent with wintertime descent. It also suggests effective containment of air up into the lower mesosphere.

Aellig, C. P.↗
NASA NTRS1996

Seasonal Variations of Water Vapor in the Lower Stratosphere Inferred from ATMOS/ATLAS-3 Measurements of H2O and CH4

Stratospheric measurements of H2O and CH4 by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer on the ATLAS-3 shuttle flight in November 1994 have been examined to investigate the altitude and geographic variability of H2O and the quantity H = (H2O + 2CH4) in the tropics and at mid-latitudes (8 to 49 deg N) in the northern hemisphere. The measurements indicate an average value of 7.24 plus or minus 0.44 ppmv for H between altitudes of about 18 to 35 km, corresponding to an annual average water vapor mixing ratio of 3.85 plus or minus 0.29 ppmv entering the stratosphere. The H2O vertical distribution in the tropics exhibits a wave-like structure in the 16- to 25-km altitude range, suggestive of seasonal variations in the water vapor transported from the troposphere to the stratosphere. The hygropause appears to be nearly coincident with the tropopause at the time of observations. This is consistent with the phase of the seasonal cycle of H2O in the lower stratosphere, since the ATMOS observations were made in November when the H2O content of air injected into the stratosphere from the troposphere is decreasing from its seasonal peak in July - August.

Abbas, M. M.↗
NASA NTRS1995

Simultaneous adsorption of CO2 and H2O under Mars-like conditions and application to the evolution of the Martian climate

The Martian regolith is the most substantial volatile reservoir on the planet; estimates of its adsorbed inventory have been based on simple measurements of the adsorption of either water or CO2 in isolation. Under some conditions, H2O can poison adsorbate surfaces, such that CO2 uptake is greatly reduced. We have made the first measurements of the simultaneous adsorption of CO2 and H2O under conditions appropriate to the Martian regolith and have found that at H2O monolayer coverage above about 0.5, CO2 begins to be displaced into the gas phase. We have developed an empirical expression that describes our co-adsorption data and have applied it to standard models of the Martian regolith. We find that currently, H2O does not substantially displace CO, implying that the adsorbate inventories previously derived may be accurate, not more than 3-4 kPa (30-40 mbar). No substantial increase in atmospheric pressure is predicted at higher obliquities because high-latitude ground ice buffers the partial pressure of H2O in the pores, preventing high monolayer coverages of H2O from displacing CO2. The peak atmospheric pressure at high obliquity does increase as the total inventory of exchangeable CO2 increases.

Zent, Aaron, P.↗
NASA NTRS2004

Laboratory Infrared Spectra of Polycyclic Aromatic Nitrogen Heterocycles: Quinoline, and Phenanthridine in Solid Argon and H2O

Polycyclic aromatic hydrocarbons (PAHs) are common throughout the universe. Their detection and identification are based on telescopic infrared (IR) spectra compared with laboratory data. Polycyclic Aromatic Nitrogen Heterocycles (PANHs) are heterocyclic aromatics i.e., PAHs with carbon atoms replaced by a nitrogen atom. These molecules should be present in the interstellar medium, but have received relatively little attention. We present mid-IR spectra of two PANHs, quinoline (C9H7N), and phenanthridine (C13H9N) isolated in solid argon and frozen in solid H2O at 12 K, conditions yielding data directly comparable to astronomical observations. In contrast to simple PAHs, that do not interact strongly with solid H2O, the nitrogen atoms in PANHs are potentially capable of hydrogen bonding with H2O. Whereas the IR spectrum of phenanthridine in H2O is similar to that of the same compound isolated in an argon matrix, quinoline absorptions shift up to 16 cm(sup -1) (0.072 mm) between argon and H2O. Thus, astronomers will not always be able to rely on IR band positions of matrix isolated PANHs to correctly interpret the absorptions of PANHs frozen in H2O ice grains. Furthermore, our data suggest that relative band areas also vary, so determining column densities to better than a factor of 3 will require knowledge of the matrix in which the PANH is embedded and laboratory studies of relevant samples.

Bernstein, M. P.↗
NASA NTRS2007

Effects of Convective Ice Lofting on H2O and HDO in the Tropical Tropopause Layer

We have added convective ice lofting to a Lagrangian trajectory model of near-tropopause water vapor (H2O) and its isotopologue HDO. The ice lofting simulation is based on a parameterization derived from Aura Microwave Limb Sounder (MLS) icewater content measurements. In previous papers, the Lagrangian model has accurately interannual and seasonal H2O abundances; there was no need for convection to be included in the model. We show here that this model does a poor job of simulating near-tropopause HDO, but that the addition of convective ice lofting greatly improves the HDO simulation. Convective ice lofting has a small effect on lower stratospheric H2O. H2O there is set by the minimum temperature encountered at the cold-point tropopause, so H2O added by convection below this level does not make it through this cold point and into the lower stratosphere. Thus, adding convection to the model does not degrade the model's previously demonstrated accurate simulations of H2O. We conclude that the HDO data suggest an important role for convective mass flux into the so-called tropical tropopause layer.

Dessler, A. E.↗
NASA NTRS1974

Exchange of adsorbed H2O and CO2 between the regolith and atmosphere of Mars caused by changes in surface insolation

Estimates have been made of the capacity of the Martian regolith to exchange adsorbed H2O and CO2 with the atmosphere-plus-cap system (APCS). These estimates are based upon measured isotherms for H2O and CO2 adsorption on pulverized basalt at low temperatures and on theoretical considerations. A unit column (1 sq cm) of regolith with a deep subsurface temperature of -77 C, considered average for the disk, will contain about 0.4 g of adsorbed CO2 and about 1 g of adsorbed H2O per meter of depth. Under favorable circumstances the top 3 cm can exchange much more H2O with the lower atmosphere each day than is necessary to produce the diurnal brightening. The process appears to be seasonally reversible. The total regolith may contain, in the adsorbed phase alone, as much as 1% of the H2O and 5% of the CO2 surface inventories expected for a hypothetical Mars that has experienced degassing as intensive as that of earth.

Fanale, F. P.↗
NASA NTRS1978

The effect of H2O and CO2 on planetary mantles

The peridotite-H2O-CO2 system is discussed, and it is shown that even traces of H2O and CO2, in minerals or vapor, lower mantle solidus temperatures through hundreds of degrees in comparison with the volatile-free solidus. The solidus for peridotite-H2O-CO2 is a divariant surface traversed by univariant lines that locate the intersections of subsolidus divariant surfaces for carbonation or hydration reactions occurring in the presence of H2O-CO2 mixtures. Vapor phase compositions are normally buffered to these lines, and near the buffered curve for the solidus of partly carbonated peridotite there is a temperature maximum on the peridotite-vapor solidus. Characteristics on the CO2 side of the maximum and on the H2O side of the maximum are described.

Wyllie, P. J.↗
NASA NTRS1980

Studies of H2O on beta-AgI surfaces - An effective pair potential model

The adsorption of a water molecule on surfaces of beta-AgI, the hexagonal crystal believed to be primarily responsible for the ice-nucleating properties of AgI, is studied on the basis of an effective pair potential model. The water molecule is represented by a rigid point charge ST-2 model and the AgI substrate by an array of point atoms, and maximal binding energy surfaces and optimal H2O configurations are generated for the water molecule adsorbed on the rigid and unrelaxed basal and prism faces. Modeling of H2O adsorption above a two-layer ledge, an iodine vacancy and an H2O molecule trapped in the vacancy indicates that H2O adsorption is favored at interstitial sites where no substrate atoms lie directly below. The prism face is found to attract the water molecule more strongly and provide larger energy barriers to surface diffusion than basal face sites, with the ideal basal faces providing hexagonal patterns of adsorption sites for the H2O with preferred dipole moments aligned.

Hale, B. N.↗
NASA NTRS1981

Ultraviolet absorption studies of H2O and other species in comet comae with satellite telescope-spectrometers

It is noted that ultraviolet absorption by H2O and other species in the comae of comets could be detected by studying, with satellite telescope-spectrometers, the occultation of hot stars by comets. Observations of this type could produce the first detection of H2O, the fundamental parent molecule in comet comae, and give measures of molecular level populations. The capabilities of the High Resolution Spectrograph on Space Telescope, the first instrument suitable for such observations, are discussed. A Haser model is used to estimate the molecular column densities and to predict equivalent widths for lines of H2O, OH, CO, C, and O as functions of time and angular distance from a comet with a high H2O production rate. The minimum detectable equivalent widths are determined, thereby giving the maximum angular separation from such a comet at which H2O, OH, and CO could be studied. Estimated equivalent widths for CO, OH, and the resonance lines of C and O suggest that these species may also be detected.

Smith, P. L.↗
NASA NTRS1983

On photochemical heating of cometary comae - The cases of H2O and CO-rich comets

It is found that the effect of energy addition due to photochemical processes in the cometary coma on the heating and accelerating of the expanding neutral gas is limited by the kinematic property of the energy transfer from the energetic fragments to the bulk flow. The effective scale length of the photochemical zone for an H2O comet is estimated to be only 10% of the dimension of the collision region due to the large mass ratio of H atom and H2O molecule. When this physical property is taken into consideration, the H2O gas is found to be expanding at a highly supersonic speed. In addition, it is shown that the addition of a mixture of CO and/or CO2 molecules in a medium-bright comet with total production rate of 10 to the 29th molecules/s would not change this conclusion since the photodissiation length scales of these molecules are a factor of 10-30 larger than that of the H2O molecules. Thus, most of the CO and CO2 molecules will be dissociated outside of the collision zone without depositing the excess kinetic energy to the neutral atmosphere. However, if the gas production rate is controlled by CO or CO2, the dimension of the collision zone of a CO comet at 1 AU will be increased by a factor of seven. The photochemical heating due to CO dissociation would thus be more effective, causing the atmospheric flow to be weakly supersonic. It is concluded that the neutral gas outflows from H2O comets and CO comets could be substantially different.

Ip, W.-H.↗
NASA NTRS1984

A search for interstellar H2O(+) in diffuse clouds

Searches for H2O(+) toward HD 187982, Zeta Oph, O micron Per, and Zeta Per have yielded significant upper limits for H2O(+) when compared with existing models for similar lines of sight. Using available oscillator strength data, the column density for HD 187982, for example, cannot exceed 3 x 10 to the 12th per sq cm H2O(+) molecules. The most sensitive measurement for H2O(+) toward Zeta Oph is apparently limited by a blend with upper atmospheric H2O(+), which is also present in the HD 187982 spectrum.

Federman, S. R.↗
NASA NTRS1985

CCD observations of comet Tuttle 1980 XIII - The H2O(+) ionosphere

A CCD spectrum of comet Tuttle 1980h has been analyzed with emphasis on the emission of H2O(+) ions. The fine angular resolution (1.5 arcsec) and the capability of absolute brightness calibration of the CCD instrument made it possible to determine the spatial concentration of the H2O(+) ions of this faint comet and the total number of these ions confined within a spherical region. Solar photoionization of the H2O atmosphere can account for the production of the H2O(+) ions observed in the confined region. The dimension of the H2O(+) ionosphere at the time of observation was found to be comparatively small, implying the possible existence of an ionopause sharply delineating the extension of the cometary ionosphere.

Ip, W.-H.↗
NASA NTRS1991

Distillation of H2O from hard-frozen Martian permafrost

The authors present a method for distillation of hard-frozen Martian permafrost. A cable-tool is drilled into hard frozem permafrost to a depth of 10 to 20 m. They calculate that a 10 m hole could be drilled in a few days. A 10 m shaft with a diameter equal to the bore is inserted into the hole, and a air tight tent-like structure is erected over the borehole. Photovoltaic cells mounted on the tent supply electrical energy that is dissipated in the shaft. Drilling power can be supplied by other sources. With 1000 watts, the shaft can be heated to near 350 K, producing relatively high temperatures in the vicinity of the borehole. Surrounding H2O is vaporized and diffuses up through the regolith. The authors calculate that a tent of a radius of no more than a few meters would intercept most of the H2O as it diffused to the surface. Calculations suggest that it would require perhaps 30 days to extract H2O from most of the volume drained by this technique. Assuming that the hard frozen regolith is no more than 10 percent ice, the author's calculate that that about 2890 kg of H2O could be extracted in 30 days. Since the nominal requirement for each crew member is about 5 kg/day, one such borehole might be expected to supply enough H2O to maintain a crew of 5 for perhaps 100 days. Additional engineering studies will be done to attempt to improve the capacity or efficiency of this method.

Zent, A. P.↗
NASA NTRS1994

H2O-H2SO4 system in Venus' clouds and OCS, CO, and H2SO4 profiles in Venus' troposphere

A coupled problem of diffusion and condensation is solved for the H2SO4-H2O system in Venus' cloud layer. The position of the lower cloud boundary and profiles of the H2O and H2SO4 vapor mixing ratios and of the H2O/H2SO4 ratio of sulfuric acid aerosol and its flux are calculated as functions of the column photochemical production rate of sulfuric acid, Phi(sub H2SO4). Variations of the lower cloud boundary are considered. Our basic model, which is constrained to yield f(sub H2O) (30 km) = 30 ppm (Pollack et al. 1993), predicts the position of the lower cloud boundary at 48.4 km coinciding with the mean Pioneer Venus value, the peak H2SO4 mixing ratio of 5.4 ppm, and the H2SO4 production rate Phi(sub H2SO4) = 2.2 x 10(exp 12)/sq cm/s. The sulfur to sulfuric acid mass flux ratio in the clouds is 1:27 in this model, and the mass loading ratio may be larger than this value if sulfur particles are smaller than those of sulfuric acid. The model suggests that the extinction coefficient of sulfuric acid particles with radius 3.7 micrometers (mode 3) is equal to 0.3/km in the middle cloud layer. The downward flux of CO is equal to 1.7 x 10(exp 12)/sq cm/s in this model. Our second model, which is constrained to yield f(sub H2O) = 10 ppm at the lower cloud boundary, close to the value measured by the Magellan radiooccultations, predicts the position of this boundary to be at 46.5 km, which agrees with the Magellan data; f(sub H2O) (30 km) = 90 ppm, close to the data of Moroz et al. (1983) at this altitude; Phi(sub H2SO4) = 6.4 x 10(exp 12)/sq cm/s; and Phi(sub co) = 4.2 x 10(exp 12)/sq cm/s. The S/H2SO4 flux mass ratio is 1:18, and the extinction coefficient of the mode 3 sulfuric acid particles is equal to 0.9 km in the middle cloud layer. A strong gradient of the H2SO4 vapor mixing ratio near the bottom of the cloud layer drives a large upward flux of H2SO4, which condenses and forms the excessive downward flux of liquid sulfuric acid, which is larger by a factor of 4-7 than the flux in the middle cloud layer. This is the mechanism of formation of the lower cloud layer. Variations of the lower cloud layer are discussed. Our modeling of the OCS and CO profiles in the lower atmosphere measured by Pollack et al. (1993) provides a reasonable explanation of these data and shows that the rate coefficient of the reaction SO3 + CO yields CO2 + SO2 is equal to 10(exp -11) exp(-(13,100 +/- 1000)/T) cc/s. The main channel of the reaction between SO3 and OCS is CO2 + (SO)2, and its rate coefficient is equal to 10(exp -11) exp(-(8900 +/- 500)/T) cc/s. In the conditions of Venus' lower atmosphere, (SO)2 is removed by the reaction (SO)2 + OCS yields CO + S2 + SO2. The model predicts an OCS mixing ratio of 28 ppm near the surface.

Krasnopolsky, V. A.↗
NASA NTRS1995

Interhemispheric differences in polar stratospheric HNO3, H2O, ClO, and O3

Simultaneous global measurements of nitric acid (HNO3), water (H2O), chlorine monoxide (ClO), and ozone (O3) in the stratosphere have been obtained over complete annual cycles in both hemispheres by the Microwave Limb Sounder on the Upper Atmosphere Research Satellite. A sizeable decrease in gas-phase HNO3 was evident in the lower stratospheric vortex over Antarctica by early June 1992, followed by a significant reduction in gas-phase H2O after mid-July. By mid-August, near the time of peak ClO, abundances of gas-phase HNO3 and H2O were extremely low. The concentrations of HNO3 and H2O over Antarctica remained depressed into November, well after temperatures in the lower stratosphere had risen above the evaporation threshold for polar stratospheric clouds, implying that denitrification and dehydration had occurred. No large decreases in either gas-phase HNO3 or H2O were observed in the 1992-1993 Arctic winter vortex. Although ClO was enhanced over the Arctic as it was over the Antarctic, Arctic O3 depletion was substantially smaller than that over Antarctica. A major factor currently limiting the formation of an Arctic ozone 'hole' is the lack of denitrification in the northern polar vortex, but future cooling of the lower stratosphere could lead to more intense denitrification and consequently larger losses of Arctic ozone.

Santee, M. L.↗
NASA NTRS2001

The Transition from Hydrogen Bonding to Ionization in (HCI)n(NH3)n and (HCI)n(H2O)n Clusters: Consequences for Anharmonic Vibrational Spectroscopy

Anharmonic vibrational frequencies and intensities are calculated for 1:1 and 2:2 (HCl)(sub n)(NH3)(sub n) and (HCl)(sub n)(H2O)(sub n) complexes, employing the correlation-corrected vibrational self-consistent field method with ab initio potential surfaces at the MP2/TZP computational level. In this method, the anharmonic coupling between all vibrational modes is included, which is found to be important for the systems studied. For the 4:4 (HCl)(sub n)(H2O)(sub n) complex, the vibrational spectra are calculated at the harmonic level, and anharmonic effects are estimated. Just as the (HCl)(sub n)(NH3)(sub n) structure switches from hydrogen-bonded to ionic for n=2, the (HCl)(sub n)(H2O)(sub n) switches to ionic structure for n=4. For (HCl)2(H2O)2, the lowest energy structure corresponds to the hydrogen-bonded form. However, configurations of the ionic form are separated from this minimum by a barrier of less than an O-H stretching quantum. This suggests the possibility of experiments on ionization dynamics using infrared excitation of the hydrogen-bonded form. The strong cooperative effects on the hydrogen bonding, and concomitant transition to ionic bonding, makes an accurate estimate of the large anharmonicity crucial for understanding the infrared spectra of these systems. The anharmonicity is typically of the order of several hundred wave numbers for the proton stretching motions involved in hydrogen or ionic bonding, and can also be quite large for the intramolecular modes. In addition, the large cooperative effects in the 2:2 and higher order (HCl(sub n)(H2O)(sub n) complexes may have interesting implications for solvation of hydrogen halides at ice surfaces.

Chaban, Galina M.↗
NASA NTRS2003

Production, Outflow Velocity, and Radial Distribution of H2O and OH in the Coma of Comet C/1995 O1 [Hale-Bopp] from Wide Field Imaging of OH

Observations of OH are a useful proxy of the water production rate (Q(sub H2O)) and outflow velocity (V(sub out)) in comets. From wide field images taken on 03/28/1997 and 04/08/1997 that capture the entire scale length of the OH coma of comet C/1995 O1 (Hale-Bopp), we obtain Q(sub H2O) from the model-independent method of aperture summation. With an adaptive ring summation algorithm, we extract the radial brightness distribution of OH 0-0 band emission out to cometocentric distances of up to 10(exp 6) km, both as azimuthal averages and in quadrants covering different position angles relative to the comet-Sun line. These profiles are fit using both fixed and variable velocity 2-component spherical expansion models to estimate V(sub OH) with increasing distance from the nucleus. The OH coma of Hale-Bopp was more spatially extended than previous comets, and this extension is best matched by a variable acceleration of H2O and OH that acted across the entire coma, but was strongest within 1-2 x 10(exp 4) km from the nucleus. Our models indicate that V(sub OH) at the edge of our detectable field of view (10(exp 6) km) was approx. 2-3 times greater in Hale-Bopp than for a 1P/Halley-class comet at 1 AU, which is consistent with the results of more sophisticated gas-kinetic models, extrapolation from previous observations of OH in comets with Q(sub H2O) greater than 10(exp 29)/s , and direct radio measurements of the outer coma Hale-Bopp OH velocity. The most probable source of this acceleration is thermalization of the excess energy of dissociation of H2O and OH over an extended collisional coma. When the coma is broken down by quadrants in position angle, we find an azimuthal asymmetry in the radial distribution that is characterized by an increase in the spatial extent of OH in the region between the orbit-trailing and anti-sunward directions. Model fits specific to this area and comparison with radio OH measurements suggest greater acceleration here, with V(sub OH) approx. 1.5 times greater at a 10(exp 6) km cometocentric distance than elsewhere in the coma. We discuss several mechanisms that may have acted within the coma to produce the observed effect.

Harris, Walter M.↗