ALBERT

Description: A network of 10 southern hemisphere tropical and Subtropical stations, designated the Southern Hemisphere ADditional OZonesondes, (SHADOZ) project and established from operational sites, provided over 1000 ozone profiles during the period 1998-2000. Balloon-borne electrochemical concentration cell (ECC) ozonesondes, combined with standard radiosondes for pressure, temperature and relative humidity measurements, collected profiles in the troposphere and lower- to mid-stratosphere at: Ascension Island; Nairobi, Kenya; Irene, South Africa: Reunion Island, Watukosek Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil.

Description: Aerosol is any small particle of matter that rests suspended in the atmosphere. Natural sources, such as deserts, create some aerosols; consumption of fossil fuels and industrial activity create other aerosols. All the microscopic aerosol particles add up to a large amount of material floating in the atmosphere. You can see the particles in the haze that floats over polluted cities. Beyond this visible effect, aerosols can actually lower temperatures. They do this by blocking, or scattering, a portion of the sun's energy from reaching the surface. Because of this influence, scientists study the physical properties of atmospheric aerosols. Reliable numerical models for atmospheric aerosols play an important role in research.

Description: We provide an overview of the nadir measurements of carbon monoxide (CO) obtained thus far by the Tropospheric Emission Spectrometer (TES). The instrument is a high resolution array Fourier transform spectrometer designed to measure infrared spectral radiances from low Earth orbit. It is one of four instruments successfully launched onboard the Aura platform into a sun synchronous orbit at an altitude of 705 km on July 15, 2004 from Vandenberg Air Force Base, California. Nadir spectra are recorded at 0.06/cm spectral resolution with a nadir footprint of 5 x 8 km. We describe the TES retrieval approach for the analysis of the nadir measurements, report averaging kernels for typical tropical and polar ocean locations, characterize random and systematic errors for those locations, and describe instrument performance changes in the CO spectral region as a function of time. Sample maps of retrieved CO for the middle and upper troposphere from global surveys during December 2005 and April 2006 highlight the potential of the results for measurement and tracking of global pollution and determining air quality from space.

Description: Clouds exert an important influence on tropospheric photochemistry through modification of solar radiation that determines photolysis frequencies (J-values). We assess the radiative effect of clouds on photolysis frequencies and key oxidants in the troposphere with a global three-dimensional (3-D) chemical transport model (GEOS-CHEM) driven by assimilated meteorological observations from the Goddard Earth Observing System data assimilation system (GEOS DAS) at the NASA Global Modeling and Assimilation Office (GMAO). We focus on the year of 2001 with the GEOS-3 meteorological observations. Photolysis frequencies are calculated using the Fast-J radiative transfer algorithm. The GEOS-3 global cloud optical depth and cloud fraction are evaluated and generally consistent with the satellite retrieval products from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the International Satellite Cloud Climatology Project (ISCCP). Results using the linear assumption, which assumes linear scaling of cloud optical depth with cloud fraction in a grid box, show global mean OH concentrations generally increase by less than 6% because of the radiative effect of clouds. The OH distribution shows much larger changes (with maximum decrease of approx.20% near the surface), reflecting the opposite effects of enhanced (weakened) photochemistry above (below) clouds. The global mean photolysis frequencies for J[O1D] and J[NO2] in the troposphere change by less than 5% because of clouds; global mean O3 concentrations in the troposphere increase by less than 5%. This study shows tropical upper tropospheric O3 to be less sensitive to the radiative effect of clouds than previously reported (approx.5% versus approx.20-30%). These results emphasize that the dominant effect of clouds is to influence the vertical redistribution of the intensity of photochemical activity while global average effects remain modest, again contrasting with previous studies. Differing vertical distributions of clouds may explain part, but not the majority, of these discrepancies between models. Using an approximate random overlap or a maximum-random overlap scheme to take account of the effect of cloud overlap in the vertical reduces the impact of clouds on photochemistry but does not significantly change our results with respect to the modest global average effect.

Description: Processes that affect the concentration of tropospheric OH are considered, taking into account linkages between the chemistry of OH and the chemistry of H, HO2, and H2O2. A review is presented of observational data of special relevance to OH, notably the distributions of CO, CH4, O3, H2O, HNO3, NO, and NO2. Most of the results presented in connection with the description of the model were obtained by solving time-dependent continuity equations. Rates for photolytic processes were allowed to vary diurnally with insolation. It is found that a well-calibrated and reliable model for OH places important constraints on global budgets for a variety of gases including CH4, H2, and CH3Cl in addition to CO. Accurate measurements of species such as CH3CCl3 can provide valuable checks on global models that must integrate over a variety of atmospheric conditions. However, emission rates for the relevant gases must be adequately quantified.

Description: The cycle of nitrogen oxides in the troposphere is discussed from both global and regional perspectives. Global sources for NO(x) are estimated to be of magnitude 50 (+ or - 25) x 10 to the 12th gm N/yr. Nitrogen oxides are derived from combustion of fossil fuels (40 percent) and biomass burning (25 percent) with the balance from lightning and microbial activity in soils. Estimates for the rate of removal of NOx based on recent atmospheric and precipitation chemistry data are consistent with global source strengths derived here. Industrial and agricultural activities provide approximately two thirds of the global source for NOx. In North America, sources from combustion of fossil fuels exceed natural sources by a factor of 3-13. Wet deposition removes about one third of the combustion source of NOx over North America, while dry deposition removes a similar amount. The balance is exported from the continent. Deposition of nitrate in precipitation over eastern Canada and the western Atlantic is clearly influenced by sources of NOx in the eastern United States.

Description: A new altitude dependent ozone climatology has been produced for use with the latest Total Ozone Mapping Spectrometer (TOMS) and Solar Backscatter Ultraviolet (SBUV) retrieval algorithms. The climatology consists of monthly average profiles for ten degree latitude zones covering from 0 to 60 km. The climatology was formed by combining data from SAGE II (1988 to 2000) and MLS (1991-1999) with data from balloon sondes (1988-2002). Ozone below about 20 km is based on balloons sondes, while ozone above 30 km is based on satellite measurements. The profiles join smoothly between 20 and 30 km. The ozone climatology in the southern hemisphere and tropics has been greatly enhanced in recent years by the addition of balloon sonde stations under the SHADOZ (Southern Hemisphere Additional Ozonesondes) program. A major source of error in the TOMS and SBUV retrieval of total column ozone comes from their reduced sensitivity to ozone in the lower troposphere. An accurate climatology for the retrieval a priori is important for reducing this error on the average. The new climatology follows the seasonal behavior of tropospheric ozone and reflects its hemispheric asymmetry. Comparisons of TOMS version 8 ozone with ground stations show an improvement due in part to the new climatology.

Description: We present a first description and evaluation of GEOS-CHEM, a global three-dimensional (3-D) model of tropospheric chemistry driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Data Assimilation Office (DAO). The model is applied to a 1-year simulation of tropospheric ozone-NOx-hydrocarbon chemistry for 1994, and is evaluated with observations both for 1994 and for other years. It reproduces usually to within 10 ppb the concentrations of ozone observed from the worldwide ozonesonde data network. It simulates correctly the seasonal phases and amplitudes of ozone concentrations for different regions and altitudes, but tends to underestimate the seasonal amplitude at northern midlatitudes. Observed concentrations of NO and peroxyacetylnitrate (PAN) observed in aircraft campaigns are generally reproduced to within a factor of 2 and often much better. Concentrations of HNO3 in the remote troposphere are overestimated typically by a factor of 2-3, a common problem in global models that may reflect a combination of insufficient precipitation scavenging and gas-aerosol partitioning not resolved by the model. The model yields an atmospheric lifetime of methylchloroform (proxy for global OH) of 5.1 years, as compared to a best estimate from observations of 5.5 plus or minus 0.8 years, and simulates H2O2 concentrations observed from aircraft with significant regional disagreements but no global bias. The OH concentrations are approximately 20% higher than in our previous global 3-D model which included an UV-absorbing aerosol. Concentrations of CO tend to be underestimated by the model, often by 10-30 ppb, which could reflect a combination of excessive OH (a 20% decrease in model OH could be accommodated by the methylchloroform constraint) and an underestimate of CO sources (particularly biogenic). The model underestimates observed acetone concentrations over the South Pacific in fall by a factor of 3; a missing source from the ocean may be implicated.

Description: We interpret the distribution of tropical tropospheric ozone columns (TTOCs) from the Total Ozone Mapping Spectrometer (TOMS) by using a global three-dimensional model of tropospheric chemistry (GEOS-CHEM) and additional information from in situ observations. The GEOS-CHEM TTOCs capture 44% of the variance of monthly mean TOMS TTOCs from the convective cloud differential method (CCD) with no global bias. Major discrepancies are found over northern Africa and south Asia where the TOMS TTOCs do not capture the seasonal enhancements from biomass burning found in the model and in aircraft observations. A characteristic feature of these northern topical enhancements, in contrast to southern tropical enhancements, is that they are driven by the lower troposphere where the sensitivity of TOMS is poor due to Rayleigh scattering. We develop an efficiency correction to the TOMS retrieval algorithm that accounts for the variability of ozone in the lower troposphere. This efficiency correction increases TTOC's over biomass burning regions by 3-5 Dobson units (DU) and decreases them by 2-5 DU over oceanic regions, improving the agreement between CCD TTOCs and in situ observations. Applying the correction to CCD TTOCs reduces by approximately DU the magnitude of the "tropical Atlantic paradox" [Thompson et al, 2000], i.e. the presence of a TTOC enhancement over the southern tropical Atlantic during the northern African biomass burning season in December-February. We reproduce the remainder of the paradox in the model and explain it by the combination of upper tropospheric ozone production from lightning NOx, peristent subsidence over the southern tropical Atlantic as part of the Walker circulation, and cross-equatorial transport of upper tropospheric ozone from northern midlatitudes in the African "westerly duct." These processes in the model can also account for the observed 13-17 DU persistent wave-1 pattern in TTOCs with a maximum above the tropical Atlantic and a minimum over the tropical Pacific during all seasons. The photochemical effects of mineral dust have only a minor role on the modeled distribution of TTOCs, including over northern Africa, due to multiple competing effects. The photochemical effects of mineral dust globally decease annual mean OH concentrations by 9%. A global lightning NOx source of 6 Tg N yr(sup -1) in the model produces a simulation that is most consistent with TOMS and in situ observations.