-
The transport pathways of carbon monoxide (CO) in the African Upper Troposphere (UT) during the West African Monsoon (WAM) is investigated through the assimilation of CO observations by the Aura Microwave Limb Sounder (MLS) in the MOCAGE Chemistry Transport Model (CTM). The assimilation setup, based on a 3-D First Guess at Assimilation Time (3-D-FGAT) variational method is described. Comparisons between the assimilated CO fields and in situ airborne observations from the MOZAIC program between Europe and both Southern Africa and Southeast Asia show an overall good agreement around the lowermost pressure level sampled by MLS (~215 hPa). The 4-D assimilated fields averaged over the month of July 2006 have been used to determine the main dynamical processes responsible for the transport of CO in the African UT. The studied period corresponds to the second AMMA (African Monsoon Multidisciplinary Analyses) aircraft campaign. At 220 hPa, the CO distribution is characterized by a latitudinal maximum around 5° N mostly driven by convective uplift of air masses impacted by biomass burning from Southern Africa, uplifted within the WAM region and vented predominantly southward by the upper branch of the winter hemisphere Hadley cell. Above 150 hPa, the African CO distribution is characterized by a broad maximum over northern Africa. This maximum is mostly controlled by the large scale UT circulation driven by the Asian Summer Monsoon (ASM) and characterized by the Asian Monsoon Anticyclone (AMA) centered at 30° N and the Tropical Easterly Jet (TEJ) on the southern flank of the anticyclone. Asian pollution uplifted to the UT over large region of Southeast Asia is trapped within the AMA and transported by the anticyclonic circulation over Northeast Africa. South of the AMA, the TEJ is responsible for the tranport of CO-enriched air masses from India and Southeast Asia over Africa. Using the high time resolution provided by the 4-D assimilated fields, we give evidence that the variability of the African CO distribution above 150 hPa and north of the WAM region is mainly driven by the synoptic dynamical variability of both the AMA and the TEJ.
-
Ground-based total ozone and surface UV irradiance measurements have been collected since 1992 using Brewer spectrophotometer at Rome station. Erythemal Dose Rates (EDRs) have been also determined by a broad-band radiometer (model YES UVB-1) operational since 2000. The methodology to retrieve the EDR and the Erythemal Daily Dose (EDD) from the radiometer observations is described. Ground-based measurements were compared with satellite-derived total ozone and UV data from the Ozone Monitoring Instrument (OMI). OMI, onboard the NASA EOS Aura spacecraft, is a nadir viewing spectrometer that provides total ozone and surface UV retrievals. The results of the validation exercise showed satisfactory agreement between OMI and Brewer total ozone data, for both OMI-TOMS and OMI-DOAS ozone algorithms (biases of −1.8% and −0.7%, respectively). Regarding UV data, OMI data overestimate ground based erythemally weighted UV irradiances retrieved from both Brewer and YES Radiometer (biases about 20%). The effect of aerosols on UV comparisons was investigated in terms of Aerosol Optical Depth (AOD), showing medium-large correlation at SZA larger than 55°. Further sources of uncertainty, such as the difference in the atmospheric conditions between local noon and OMI overpass time and the OMI spatial resolution, were also discussed.
-
Tropospheric chemistry and air quality processes were implemented on-line in the Global Environmental Multiscale weather prediction model. The integrated model, GEM-AQ, was developed as a platform to investigate chemical weather at scales from global to urban. The current chemical mechanism is comprised of 50 gas-phase species, 116 chemical and 19 photolysis reactions, and is complemented by a sectional aerosol module with 5 aerosols types. All tracers are advected using the semi-Lagrangian scheme native to GEM. The vertical transport includes parameterized subgrid-scale turbulence and large scale deep convection. Dry deposition is included as a flux boundary condition in the vertical diffusion equation. Wet deposition of gas-phase species is treated in a simplified way, and only below-cloud scavenging is considered. The emissions used include yearly-averaged anthropogenic, and monthly-averaged biogenic, ocean, soil, and biomass burning emission fluxes, as well as NO<sub>x</sub> from lightning. In order to evaluate the ability to simulate seasonal variations and regional distributions of trace gases such as ozone, nitrogen dioxide and carbon monoxide, the model was run for a period of five years (2001–2005) on a global uniform 1.5°×1.5° horizontal resolution domain and 28 hybrid levels extending up to 10 hPa. Model results were compared with observations from satellites, aircraft measurement campaigns and balloon sondes. We find that GEM-AQ is able to capture the spatial details of the chemical fields in the middle and lower troposphere. The modelled ozone consistently shows good agreement with observations, except over tropical oceans. The comparison of carbon monoxide and nitrogen dioxide with satellite measurements emphasizes the need for more accurate, year-specific emissions fluxes for biomass burning and anthropogenic sources. Other species also compare well with available observations.
-
The effect of Land Use Change and Forestry (LUCF) on terrestrial carbon fluxes can be regarded as a carbon credit or debit under the UNFCCC, but scientific uncertainty in the estimates for LUCF remains large. Here, we assess the LUCF estimates by examining a variety of models of different types with different land cover change maps in the 1990s. Annual carbon pools and their changes are separated into different components for separate geographical regions, while annual land cover change areas and carbon fluxes are disaggregated into different LUCF activities and the biospheric response due to CO<sub>2</sub> fertilization and climate change. We developed a consolidated estimate of the terrestrial carbon fluxes that combines book-keeping models with process-based biogeochemical models and inventory estimates and yields an estimate of the global terrestrial carbon flux that is within the uncertainty range developed in the IPCC 4th Assessment Report. We examined the USA and Brazil as case studies in order to assess the cause of differences from the UNFCCC reported carbon fluxes. Major differences in the litter and soil organic matter components are found for the USA. Differences in Brazil result from assumptions about the LUC for agricultural purposes. The effects of CO<sub>2</sub> fertilization and climate change also vary significantly in Brazil. Our consolidated estimate shows that the small sink in Latin America is within the uncertainty range from inverse models, but that the sink in the USA is significantly smaller than the inverse models estimates. Because there are different sources of errors at the country level, there is no easy reconciliation of different estimates of carbon fluxes at the global level. Clearly, further work is required to develop data sets for historical land cover change areas and models of biogeochemical changes for an accurate representation of carbon uptake or emissions due to LUC.
-
A system to record the ultraviolet (UV) spectra of atmospheric global irradiance with the miniature fiber optic spectrometer AvaSpec-256 was developed for continuous computer-aided spectrometry at Tartu Observatory in 2005. As a result, the database of spectra recorded with 15-min-interval round 24 h over 300–400 nm, has been developed. The quantities retrieved from the spectra have been compared with those measured by the Scintec erythemal UV-SET sensor and the Kipp & Zonen narrowband 306 nm sensor. Almost clear and overcast days were selected for comparison. Reliable results on the spectral distribution of the UV global irradiance as well as the integrated daily spectral doses could be obtained at least during the bright half-year. The results were compared with the calculations performed by means of the LibRadtran package. The biases in irradiance were significant at SZA above 70–75°. At dominating larger SZA the recorded values need sophisticated corrections and remain less reliable. At lower latitudes than that of the study site (58.3°), the reliability of the spectrometer is expected to increase due to a smaller contribution of data measured at large SZA. <br></br> The variations of the ratio of UV-A/UV-B irradiance, retrieved from the spectra, were investigated. Also the covariation of the narrowband 306 nm irradiance and the irradiance integrated over the whole UV-B range was studied. The biases between the UV-A/UV-B irradiances calculated by means of the LibRadtran package and measured with the AvaSpec were small at SZA below 70°. At larger SZA the values of the ratio as well as the biases increased, significantly depending on total ozone.
-
Using seven years of the Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical thickness (AOT) data and ground measurements of particulate matter mass over one site in the Southeastern United States (33.55° N, 86.82° W) we present a comprehensive analysis of various aspects of particulate matter air quality. Monthly, seasonal and inter-annual relationships are examined with emphasis on sampling biases, quality indicators in the AOT product and various cloud clearing criteria. Our results indicate that PM<sub>2.5</sub> mass concentration over Northern Birmingham has decreased by about 23% in year 2006 when compared to year 2002 and air quality during summer months was poor when compared to winter months. MODIS-Terra AOT data was available only about 50% of the time due to cloud cover and unfavorable surface conditions. However, the mean difference in monthly mean PM<sub>2.5</sub> was less than 2.2 μg m<sup>−3</sup> derived using all the data and from only those days when satellite AOT was available indicating that satellite data does not have sampling issues. The correlation between PM<sub>2.5</sub> and MODIS AOT increased from 0.52 to 0.62 when hourly PM<sub>2.5</sub> data were used instead of daily mean PM<sub>2.5</sub> data. Changing box size for satellite data around the ground station during comparisons produced less than ±0.03 difference in mean AOT values for 90% of observations. Application of AOT quality flags reduced the sample size but does not affect AOT-PM<sub>2.5</sub> relationship significantly. We recommend using AOT quality flags for daily analysis, whereas long time scale analysis can be performed by using all AOT retrievals to obtain better sampling. Our analysis indicates that satellite data is a useful tool for monitoring particulate matter air quality especially in regions where ground measurements are not available. While these results are representative for the region of interest, it is difficult to extrapolate these results to a larger context without detailed analysis using ancillary data sets.
-
The response of a selected number of chemical species is inspected with respect to climate change. The coupled Atmosphere-Ocean General Circulation Model ECHAM4-OPYC3 is providing meteorological fields for the Chemical long-range Transport Model DEHM. Three selected decades (1990s, 2040s and 2090s) are inspected. The 1990s are used as a reference and validation period. In this decade an evaluation of the output from the DEHM model with ECHAM4-OPYC3 meteorology input data is carried out. The model results are tested against similar model simulations with MM5 meteorology and against observations from the EMEP monitoring sites in Europe. <br><br> The test results from the validation period show that the overall statistics (e.g. mean values and standard deviations) are similar for the two simulations. However, as one would expect the model setup with climate input data fails to predict correctly the timing of the variability in the observations. The overall performance of the ECHAM4-OPYC3 setup as meteorological input to the DEHM model is shown to be acceptable according to the applied ranking method. It is concluded that running a chemical long-range transport model on data from a "free run" climate model is scientifically sound. From the model runs of the three decades, it is found that the overall trend detected in the evolution of the chemical species, is the same between the 1990 decade and the 2040 decade and between the 2040 decade and the 2090 decade, respectively. <br><br> The dominating impacts from climate change on a large number of the chemical species are related to the predicted temperature increase. Throughout the 21th century the ECHAM4-OPYC3 projects a global mean temperature increase of 3 K with local maxima up to 11 K in the Arctic winter based on the IPCC A2 emission scenario. As a consequence of this temperature increase, the temperature dependent biogenic emission of isoprene is predicted to increase significantly over land by the DEHM model. This leads to an increase in the O<sub>3</sub> production and together with an increase in water vapor to an increase in the number of free OH radicals. Furthermore this increase in the number of OH radicals contributes to a significant change in the typical life time of many species, since OH are participating in a large number of chemical reactions. It is e.g. found that more SO<sub>4</sub><sup>2−</sup> will be present in the future over the already polluted areas and this increase can be explained by an enhanced conversion of SO<sub>2</sub> to SO<sub>4</sub><sup>2−</sup>.
-
During the APE-THESEO mission in the Indian Ocean the Myasishchev Design Bureau stratospheric research aircraft M55 Geophysica performed a flight over and within the inner core region of tropical cyclone Davina. Measurements of total water, water vapour, temperature, aerosol backscattering, ozone and tracers were made and are discussed here in comparison with the averages of those quantities acquired during the campaign time frame. <br><br> Temperature anomalies in the tropical tropopause layer (TTL), warmer than average in the lower part and colder than average in the upper TTL were observed. Ozone was strongly reduced compared to its average value, and thick cirrus decks were present up to the cold point, sometimes topped by a layer of very dry air. Evidence for meridional transport of trace gases in the stratosphere above the cyclone was observed and perturbed water distribution in the TTL was documented. The paper discuss possible processes of dehydration induced by the cirrus forming above the cyclone, and change in the chemical tracer and water distribution in the lower stratosphere 400–430 K due to meridional transport from the mid-latitudes and link with Davina. Moreover it compares the data prior and after the cyclone passage to discuss its actual impact on the atmospheric chemistry and thermodynamics.
-
A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the "Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere" (EFEU) project. The combustion conditions were monitored with concomitant CO<sub>2</sub> and CO measurements. The mass scattering efficiencies of 8.9±0.2 m<sup>2</sup> g<sup>−1</sup> and 9.3±0.3 m<sup>2</sup> g<sup>−1</sup> obtained for aerosol particles from the combustion of savanna grass and an African hardwood (musasa), respectively, are larger than typically reported mainly due to differences in particle size distribution. The photoacoustically measured mass absorption efficiencies of 0.51±0.02 m<sup>2</sup> g<sup>−1</sup> and 0.50±0.02 m<sup>2</sup> g<sup>−1</sup> were at the lower end of the literature values. Using the measured size distributions as well as the mass scattering and absorption efficiencies, Mie calculations provided effective refractive indices of 1.60−0.010<i>i</i> (savanna grass) and 1.56−0.010<i>i</i> (musasa) (λ=0.55 μm). The apparent discrepancy between the low imaginary part of the refractive index and the high apparent elemental carbon (EC<sub>a</sub>) fractions (8 to 15%) obtained from the thermographic analysis of impactor samples can be explained by a positive bias in the elemental carbon data due to the presence of high molecular weight organic substances. Potential artefacts in optical properties due to instrument bias, non-natural burning conditions and unrealistic dilution history of the laboratory smoke cannot be ruled out and are also discussed in this study.
-
We investigate the ability of a mesoscale model to reconstruct CO<sub>2</sub> fluxes at regional scale. Formally, we estimate the reduction of error for a CO<sub>2</sub> flux inversion at 8 km resolution in the South West of France, during four days of the CarboEurope Regional Experiment Strategy (CERES) in spring 2005. Measurements from two towers and two airplanes are available for this campaign. The lagrangian particle dispersion model LPDM was coupled to the non-hydrostatic model Meso-NH and integrated in a matrix inversion framework. Impacts of aircraft and tower measurements are quantified separately and together. We find that the configuration with both towers and aircraft is able to significantly reduce uncertainties on the 4-day averaged CO<sub>2</sub> fluxes over about half of the 300×300 km<sup>2</sup> domain. Most of this reduction comes from the tower measurements, even though the impact of aircraft measurements remains noticeable. Imperfect knowledge of boundary conditions does not significantly impact the error reduction for surface fluxes. We test alternative strategies to improve the impact of aircraft measurements and find that most information comes from measurements inside the boundary layer. We find that there would be a large improvement in error reduction if we could improve our ability to model nocturnal concentrations at tower sites.
