ALBERT

Description: Time series of CO and C2H, measurements have been derived from high-resolution infrared solar spectra recorded in Lauder, New Zealand (45.0 degrees S, 169.7 degrees E, altitude 0.37 km), and at the U.S. National Solar Observatory (31.9 degrees N, 11, 1.6 degrees W, altitude 2.09 km) on Kitt Peak. Lauder observations were obtained between July 1993 and November 1997, while the Kitt Peak measurements were recorded between May 1977 and December 1997. Both databases were analyzed with spectroscopic parameters that included significant improvements for C2H6 relative to previous studies. Target CO and C2H6 lines were selected to achieve similar vertical samplings based on averaging kernels. These calculations show that partial columns from layers extending from the surface to the mean tropopause and from the mean tropopause to 100 km are nearly independent. Retrievals based on a semiempirical application of the Rodgers optimal estimation technique are reported for the lower layer, which has a broad maximum in sensitivity in the upper troposphere. The Lauder CO and C2H, partial columns exhibit highly asymmetrical seasonal cycles with minima in austral autumn and sharp peaks in austral spring. The spring maxima are the result of tropical biomass burning emissions followed by deep convective vertical transport to the upper troposphere and long-range horizontal transport. Significant year-to-year variations are observed for both CO and C2H6, but the measured trends, (+0.37 +/- 0.57)% yr(exp -1) and (-0.64 +/- 0.79)% yr(exp -1), I sigma, respectively, indicate no significant long-term changes. The Kitt Peak data also exhibit CO and C2H6, seasonal variations in the lower layer with trends equal to (-0.27 +/- 0.17)% yr(exp -1) and (-1.20 +/- 0.35)% yr(exp -1), 1 sigma, respectively. Hence a decrease in the Kitt Peak tropospheric C2H6 column has been detected, though the CO trend is not significant. Both measurement sets are compared with previous observations, reported trends, and three-dimensional model calculations.

Description: Time series of CO and C2H6 measurements have been derived from high resolution infrared solar spectra recorded in Lauder, New Zealand (45.0 deg S, 169.7 deg E, altitude 0.37 km) and at the U. S. National Solar Observatory (31.90 deg N, 111.6 deg W, altitude 2.09 km) on Kitt Peak. Lauder observations were obtained between July 1993 and November 1997 while the Kitt Peak measurements were recorded between May 1977 and December 1997. Both databases were analyzed with spectroscopic parameters that included significant improvements for C2H6 relative to previous studies. Target CO and C2H6 lines were selected to achieve similar vertical samplings based on averaging kernels. These calculations show that partial columns from layers extending from the surface to the mean tropopause and from the mean tropopause to 100 km are nearly independent. Retrievals based on a semiempirical application of the Rodgers optimal estimation technique are reported for the lower layer, which has a broad maximum in sensitivity in the upper troposphere. The Lauder CO and C2H6 partial columns exhibit highly asymmetrical seasonal cycles with minima in austral autumn and sharp peaks in austral spring. The spring maxima are the result of tropical biomass burning emissions followed by deep convective vertical transport to the upper troposphere and long-range horizontal transport. Significant year-to-year variations are observed for both CO and C2H6, but the measured trends, (+0.37 +/- 0.57)%/ yr and (-0.64 +/- 0.79)%/ yr, 1 sigma, respectively, indicate no significant long-term changes. The Kitt Peak data also exhibit CO and C2H6 seasonal variations in the lower layer with trends equal to (-0.27 +/- 0.17)%/ yr and (-1.20 +/- 0.35)%/ yr, 1 sigma, respectively. Hence, a decrease in the Kitt Peak tropospheric C2H6 column has been detected, though the CO trend is not significant. Both measurement sets are compared with previous observations, reported trends, and three-dimensional model calculations.

Description: Lorentz air-broadening coefficients and relative intensities have been measured for forty-three lines in the pure rotational band and twenty lines in the nu2 band of H2O-16 between 800 and 1150/cm. The results were derived from analysis of nine 0.017/cm-resolution atmospheric absorption spectra recorded over horizontal paths of 0.5-1.5 km with the McMath Fourier transform spectrometer and main solar telescope operated on Kitt Peak by the National Solar Observatory. A nonlinear least-squares spectral fitting technique was used in the spectral analysis. The results are compared with previous measurements and calculations. In most cases, the measured pressure-broadening coefficients and intensities are significantly different from the values in the 1986 HITRAN line parameters compilation.

Description: Simultaneous ACE (Atmospheric Chemistry Experiment) upper tropospheric CO, C2H6, HCN, CH3Cl, CH4 , C2H2 , CH30H, HCOOH, and OCS measurements show plumes up to 185 ppbv (10 (exp -9) per unit volume) for CO, 1.36 ppbv for C2H6, 755 pptv (10(exp -12) per unit volume) for HCN, 1.12 ppbv for CH3C1, 1.82 ppmv, (10(exp -6) per unit volume) for CH4, 0.178 ppbv for C2H2, 3.89 ppbv for CH30H, 0.843 ppbv for HCOOH, and 0.48 ppbv for OCS in western Canada and Alaska at 50 deg N-68 deg N latitude between 29 June and 23 July 2004. Enhancement ratios and emission factors for HCOOH, CH30H, HCN, C2H6, and OCS relative to CO at 250-350 hPa are inferred from measurements of young plumes compared with lower mixing ratios assumed to represent background conditions based on a CO emission factor derived from boreal measurements. Results are generally consistent with the limited data reported for various vegetative types and emission phases measured in extratropical forests including boreal forests. The low correlation between fire product emission mixing ratios and the S176 mixing ratio is consistent with no significant SF6 emissions from the biomass fires.

Description: Model calculations using estimated reaction rates of sulfur hexafluoride (SF6) with OH and 0('D) indicate that the atmospheric lifetime due to these processes may be very long (25,000 years). An upper limit for the UV cross section would suggest a photolysis lifetime much longer than 1000 years. The possibility of other removal mechanisms are discussed. The estimated lifetimes are consistent with other estimated values based on recent laboratory measurements. There appears to be no known natural source of SF6. An estimate of the current production rate of SF6 is about 5 kt/yr. Based on historical emission rates, we calculated a present-day atmospheric concentrations for SF6 of about 2.5 parts per trillion by volume (pptv) and compared the results with available atmospheric measurements. It is difficult to estimate the atmospheric lifetime of SF6 based on mass balance of the emission rate and observed abundance. There are large uncertainties concerning what portion of the SF6 is released to the atmosphere. Even if the emission rate were precisely known, it would be difficult to distinguish among lifetimes longer than 100 years since the current abundance of SF6 is due to emission in the past three decades. More information on the measured trends over the past decade and observed vertical and latitudinal distributions of SF6 in the lower stratosphere will help to narrow the uncertainty in the lifetime. Based on laboratory-measured IR absorption cross section for SF6, we showed that SF6 is about 3 times more effective as a greenhouse gas compared to CFC 11 on a per molecule basis. However, its effect on atmospheric warming will be minimal because of its very small concentration. We estimated the future concentration of SF6 at 2010 to be 8 and 10 pptv based on two projected emission scenarios. The corresponding equilibrium warming of 0.0035 C and 0.0043 C is to be compared with the estimated warming due to CO2 increase of about 0.8 C in the same period.

Description: 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.