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Results of quantum statistical mechanical calculations and thermodynamic evaluation of the structure of H2CO3 and its stability against dissociation are reported. Under temperature and pressure conditions near the surface of Venus, carbonic acid would predominatly dissociate into H2O and CO2 and, hence, could not contribute to any significant absorption there.
An HgCdTe electron avalanche photodiode (e-APD) detector has been developed for lidar receivers, one application of which is integrated path differential absorption lidar measurements of such atmospheric trace gases as CO2 and CH4. The HgCdTe APD has a wide, visible to mid-wave-infrared, spectral response, high dynamic range, substantially improved sensitivity, and an expected improvement in operational lifetime. A demonstration sensor-chip assembly consisting of a 4.3 lm cutoff HgCdTe 4 9 4 APD detector array with 80 micrometer pitch pixels and a custom complementary metal-oxide-semiconductor readout integrated circuit was developed. For one typical array the APD gain was 654 at 12 V with corresponding gain normalized dark currents ranging from 1.2 fA to 3.2 fA. The 4 9 4 detector system was characterized at 77 K with a 1.55 micrometer wavelength, 1 microsecond wide, laser pulse. The measured unit gain detector photon conversion efficiency was 91.1%. At 11 V bias the mean measured APD gain at 77 K was 307.8 with sigma/mean uniformity of 1.23%. The average, noise-bandwidth normalized, system noise-equivalent power (NEP) was 1.04 fW/Hz(exp 1/2) with a sigma/mean of 3.8%. The measured, electronics-limited, bandwidth of 6.8 MHz was more than adequate for 1 microsecond pulse detection. The system had an NEP (3 MHz) of 0.4 fW/Hz(exp 1/2) at 12 V APD bias and a linear dynamic range close to 1000. A gain-independent quantum-limited SNR of 80% of full theoretical was indicative of a gain-independent excess noise factor very close to 1.0 and the expected APD mode quantum efficiency.
IRAS19312+1950 is a peculiar object that has eluded firm characterization since its discovery, with combined maser properties similar to an evolved star and a young stellar object (YSO). To help determine its true nature, we obtained infrared spectra of IRAS19312+1950 in the range 5-550 microns using the Herschel and Spitzer space observatories. The Herschel PACS maps exhibit a compact, slightly asymmetric continuum source at 170 microns, indicative of a large, dusty circumstellar envelope. The far-IR CO emission line spectrum reveals two gas temperature components: approx. = 0.22 Stellar Mass of material at 280+/-18 K, and ≈1.6 Me of material at 157+/-3 K. The OI 63 micron line is detected on-source but no significant emission from atomic ions was found. The HIFI observations display shocked, high-velocity gas with outflow speeds up to 90 km/s along the line of sight. From Spitzer spectroscopy, we identify ice absorption bands due to H2O at 5.8 microns and CO2 at 15 microns. The spectral energy distribution is consistent with a massive, luminous (approx. 2 × 10(exp 4) Stellar Luminosity) central source surrounded by a dense, warm circumstellar disk and envelope of total mass approx. 500-700 Stellar Mass with large bipolar outflow cavities. The combination of distinctive far-IR spectral features suggest that IRAS19312+1950 should be classified as an accreting, high-mass YSO rather than an evolved star. In light of this reclassification, IRAS19312+1950 becomes only the fifth high-mass protostar known to exhibit SiO maser activity, and demonstrates that 18 cm OH maser line ratios may not be reliable observational discriminators between evolved stars and YSOs.
The applicability of the Electrochemically Regenerable Carbon Dioxide and Moisture Absorption Technology to the advanced extravehicular mobility unit was demonstrated by designing, fabricating, and testing a breadboard Absorber Module and an Electrochemical Regenerator. Test results indicated that the absorber module meets or exceeds the carbon dioxide removal requirements specified for the design and can meet the moisture removal requirement when proper cooling is provided. CO2 concentration in the vent gas stream was reduced from 0.52 to 0.027 kPa (3.9 to 0.20 mm Hg) for the full five hour test period. Vent gas dew point was reduced from inlet values of 294 K (69 F) to 278 K (41 F) at the outlet. The regeneration of expended absorbent was achieved by the electrochemical method employed in the testing. An absorbent bed using microporous hydrophobic membrane sheets with circulating absorbent is shown to be the best approach to the design of an Absorber Module based on sizing and performance. Absorber Module safety design, comparison of various absorbents and their characteristics, moisture absorption and cooling study and subsystem design and operation time-lining study were also performed.
A pulsed dual-laser direct-detection differential-absorption lidar DIAL system, operating near 10.6 microns, is used to measure the temporal correlation and statistical properties of backscattered returns from specular and diffuse topographic targets. Results show that atmospheric-turbulence fluctuations can effectively be frozen for pulse separation times on the order of 1-3 msec or less. The diffuse target returns, however, yielded a much lower correlation than that obtained with the specular targets; this being due to uncorrelated system noise effects and different statistics for the two types of target returns.
Possible scenarios for the evolution of the Martian climate are discussed. In the interest of determining an upper limit on the absorptive capacity of the Martian regolith, researchers examined the results of Fanale and Cannon (1971, 1974) for CO2 adsorption on nontronite and basalt. There appeared to be a strong proportionality between the capacity of the absorbent and its specific surface area. A model of the Martian climate is given that allows the researchers to make some estimates of exchangeable CO2 abundances.
A tunable diode laser has been used to observe rotational collisional narrowing or line mixing in the IR absorption spectrum of the Q branch of the (1 1 exp-1 0,0 3 exp-1 0) sub II - 0 0 exp-0 0 band of CO2 at 1932.47/cm over the 100-745 Torr pressure range. The observed absorption coefficients below the band origin are up to 80 percent lower than those calculated on the basis of an isolated Lorentz line approxmation. A simple fitting law is derived for the state-to-state, rotationally inelastic rate constants, on the basis of the known line broadening coefficients; a calculation of the mixing using these rates agrees with observed absorption coefficients to within several percent.
Measurements of NH3 absorption coefficients are presented for several transitions of a C-13(O-16)2 laser for small concentrations of NH3(p less than 1 torr) for absorption lines broadened to 1 atm with N2. NH3 absorption coefficients were determined for laser transitions R(8)(920.2194 wavelengths/cm) to R(28)(933.8808 wavelengths/cm) of the 00 1 - (10 0,02 0)I band. The strongest absorption coefficient K = 36.09 + or - 1.43 per (atm-cm) was measured for the R(18) transition for the NH3 line, aQ(6,6), and is larger than has been found in any previous measurements with a CO2 laser. The dependence of K on total pressure was also obtained for select transitions, and the frequency separation between the R(18) laser transition and the neighboring NH3 line aQ(6,6) was determined to be 550 + or - 50 MHz. These results are significant for long path absorption monitoring of NH3 with CO2 lasers since the path length can be reduced by approximately 40% and for heterodyne detection of NH3 since the relative position of the laser transition to the NH3 absorption line is well within the bandpass of Hg-Cd-Te photomixers.
The vertical CO2 flux in the atmospheric boundary layer (ABL) is investigated with a Doppler differential absorption lidar (DIAL). The instrument was operated next to the WLEF instrumented tall tower in Park Falls, Wisconsin during three days and nights in June 2007. Profiles of turbulent CO2 mixing ratio and vertical velocity fluctuations are measured by in-situ sensors and Doppler DIAL. Time and space scales of turbulence are precisely defined in the ABL. The eddy-covariance method is applied to calculate turbulent CO2 flux both by lidar and in-situ sensors. We show preliminary mean lidar CO2 flux measurements in the ABL with a time and space resolution of 6 h and 1500 m respectively. The flux instrumental errors decrease linearly with the standard deviation of the CO2 data, as expected. Although turbulent fluctuations of CO2 are negligible with respect to the mean (0.1 %), we show that the eddy-covariance method can provide 2-h, 150-m range resolved CO2 flux estimates as long as the CO2 mixing ratio instrumental error is no greater than 10 ppm and the vertical velocity error is lower than the natural fluctuations over a time resolution of 10 s.
The formalism developed previously for the calculation of the far-wing line shape function and the corresponding absorption coefficient using a single-component anisotropic interaction term and the binary collision and quasistatic approximations is generalized to multicomponent anisotropic potential functions. Explicit expressions are presented for several common cases, including the long-range dipole-dipole plus dipole-quadrupole interaction and a linear molecule interacting with a perturber atom. After determining the multicomponent functional representation for the interaction between the CO2 and Ar from previously published data, we calculate the theoretical line shape function and the corresponding absorption due to the nu(sub 3) band of CO2 in the frequency range 2400-2580 cm(exp -1) and compare our results with previous calculations carried out using a single-component anisotropic interaction, and with the results obtained assuming Lorentzian line shapes. The principal uncertainties in the present results, possible refinements of the theoretical formalism, and the applicability to other systems are discussed briefly.
The Atmospheric Chemistry Experiment ACE satellite (SCISAT-1) was launched into an inclined orbit on 12 August 2003 and is now recording high signal-to-noise 0.02 per centimeter resolution solar absorption spectra covering 750-4400 per centimeter (2.3-13 micrometers). A procedure has been developed for retrieving average dry air CO2 mole fractions (X(sub CO2)) in the altitude range 7-10 kilometers from the SCISAT-1 spectra. Using the N2 continuum absorption in a window region near 2500 per centimeter, altitude shifts are applied to the tangent heights retrieved in version 2.2 SCISAT-1 processing, while cloudy or aerosol-impacted measurements are eliminated. Monthly-mean XCO2 covering 60 S to 60 N latitude for February 2004 to March 2008 has been analyzed with consistent trends inferred in both hemispheres. The ACE XCO2 time series have been compared with previously-reported surface network measurements, predictions based on upper tropospheric aircraft measurements, and space-based measurements. The retrieved X(sub CO2) from the ACE-FTS spectra are higher on average by a factor of 1.07 plus or minus 0.025 in the northern hemisphere and by a factor of 1.09 plus or minus 0.019 on average in the southern hemisphere compared to surface station measurements covering the same time span. The ACE derived trend is approximately 0.2% per year higher than measured at surface stations during the same observation period.
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Analytical techniques for measuring CO2 were evaluated and rated for use with the advanced extravehicular mobility unit. An infrared absorption concept using a dual-wavelength monochromator was selected for investigation. A breadboard carbon dioxide sensor (CDS) was assembled and tested. The CDS performance showed the capability of measuring CO2 over the range of 0 to 4.0 kPa (0 to 30 mmHg) P sub (CO2). The volume and weight of a flight configured CDS should be acceptable. It is recommended that development continue to complete the design of a flight prototype.
The collisionless dissociation of SF6 has been studied using simultaneous irradiation by two frequencies from a CO2 laser which are both nearly resonant with the SF6nu3 absorption band. It was found that the dissociation was enhanced, and occurred over a wider frequency range, than for single frequency dissociation. No threshold effect was observed for a weak resonant and a much higher energy field pumping slightly off-resonance. For such two frequency irradiation, the peak in the dissociation curve was found to be shifted to lower frequencies with respect to that for single frequency dissociation.
The Orbiting Carbon Observatory is scheduled for launch from Vandenberg Air Force Base in California in January 2009. This Earth System Science Pathfinder (ESSP) mission carries and points a single instrument that incorporates 3 high-resolution grating spectrometers designed to measure the absorption of reflected sunlight by near-infrared carbon dioxide (CO2) and molecular oxygen bands. These spectra will be analyzed to retrieve estimates of the column-averaged CO2 dry air mole fraction, X(sub CO2). Pre-flight qualification and calibration tests completed in early 2008 indicate that the instrument will provide high quality X(sub CO2) data. The instrument was integrated into the spacecraft, and the completed Observatory was qualified and tested during the spring and summer of 2008, in preparation for delivery to the launch site in the fall of this year. The Observatory will initially be launched into a 635 km altitude, near-polar orbit. The on-board propulsion system will then raise the orbit to 705 km and insert OCO into the Earth Observing System Afternoon Constellation (A-Train). The first routine science observations are expected about 45 days after launch. Calibrated spectral radiances will be archived starting about 6 months later. An exploratory X(sub CO2) product will be validated and then archived starting about 3 months after that.
The vertical profiling ofCO2 turbulent fluxes in the atmospheric boundary layer (ABL) is investigated using a coherent differential absorption lidar (CDIAL) operated nearby a tall tower in Wisconsin during June 2007. A CDIAL can perform simultaneous range-resolved CO2 DIAL and velocity measurements. The lidar eddy covariance technique is presented. The aims of the study are (i) an assessment of performance and current limitation of available CDIAL for CO2 turbulent fluxes and (ii) the derivation of instrument specifications to build a future CDIAL to perform accurate range-resolved CO2 fluxes. Experimental lidar CO2 mixing ratio and vertical velocity profiles are successfully compared with in situ sensors measurements. Time and space integral scales of turbulence in the ABL are addressed that result in limitation for time averaging and range accumulation. A first attempt to infer CO2 fluxes using an eddy covariance technique with currently available 2-mm CDIAL dataset is reported.
Microwave absorption measurements at wavelengths of 13.4 and 3.6 cm were made in gaseous H2SO4 in a CO2 atmosphere under simulated conditions for the Venus middle atmosphere. The results suggest that abundances of gaseous H2SO4 on the order of 15-30 ppm could account for the absorption observed by radio occultation measurements at these wavelengths. They also imply that such abundances would correspond to saturation vapor pressure existing at or above the 46-48-km range, which correlates with the observed cloud base.
Using direct radar ranging of surface heights on Mars and spectrophotometric observations of absorptions produced by carbon dioxide molecules in the Martian atmosphere, data have been obtained on Martian topographical variations at spatial resolutions ranging from about 100 to 1000 km. These data have been studied and analyzed. As a result, a surface height contour map has been produced which clearly reveals a structural complex of blocks and basins whose distribution enhances the magnitude of low-degree surface harmonics. It is emphasized that Mars possesses unexpectedly pronounced topography which can have important geophysical consequences.