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The CH4 growth rate in the atmosphere showed large variations after the Pinatubo eruption in June 1991. A decrease of more than 10 ppb yr-1 in the growth rate over the course of 1992 was reported, and a partial recovery in the following year. Although several reasons have been proposed to explain the evolution of CH4 after the eruption, their contributions to the observed variations are not yet resolved. CH4 is removed from the atmosphere by the reaction with tropospheric OH, which in turn is produced by O3 photolysis under UV radiation. The CH4 removal after the Pinatubo eruption might have been affected by changes in tropospheric UV levels due to the presence of stratospheric SO2 and sulfate aerosols, and due to enhanced ozone depletion on Pinatubo aerosols. The perturbed climate after the eruption also altered both sources and sinks of atmospheric CH4. Furthermore, CH4 concentrations were influenced by other factors of natural variability in that period, such as El Niño-Southern Oscillation (ENSO) and biomass burning events. Emissions of CO, NOX and non-methane volatile organic compounds (NMVOCs) also affected CH4 concentrations indirectly by influencing tropospheric OH levels. Potential drivers of CH4 variability are investigated using the TM5 global chemistry model. The contribution that each driver had to the global CH4 variability during the period 1990 to 1995 is quantified. We find that a decrease of 8- 10 ppb yr-1 CH4 is explained by a combination of the above processes. However, the timing of the minimum growth rate is found 6-9 months later than observed. The long-term decrease in CH4 growth rate over the period 1990 to 1995 is well captured and can be attributed to an increase in OH concentrations over this time period. Potential uncertainties in our modelled CH4 growth rate include emissions of CH4 from wetlands, biomass burning emissions of CH4 and other compounds, biogenic NMVOC and the sensitivity of OH to NMVOC emission changes. Two inventories are used for CH4 emissions from wetlands, ORCHIDEE and LPJ, to investigate the role of uncertainties in these emissions. Although the higher climate sensitivity of ORCHIDEE improves the simulated CH4 growth rate change after Pinatubo, none of the two inventories properly captures the observed CH4 variability in this period. [ABSTRACT FROM AUTHOR]

This study presents a sensitivity analysis of multivariate regressions of recent springtime Antarctic vortex ozone trends using a "big data" ensemble approach. Our results indicate that the poleward heat flux (Eliassen-Palm flux) and the effective chlorine loading respectively explain most of the short-term and long-term variability in different Antarctic springtime total ozone records. The inclusion in the regression of stratospheric volcanic aerosols, solar variability and the quasi-biennial oscillation is shown to increase rather than decrease the overall uncertainty in the attribution of Antarctic springtime ozone because of large uncertainties in their respective records. Calculating the trend significance for the ozone record from the late 1990s onwards solely based on the fit of the effective chlorine loading is not recommended, as this does not take fit residuals into account, resulting in too narrow uncertainty intervals, while the fixed temporal change of the effective chlorine loading does not allow for any flexibility in the trends. When taking fit residuals into account in a piecewise linear trend fit, we find that approximately 30-60% of the regressions in the full ensemble result in a statistically significant positive springtime ozone trend over Antarctica from the late 1990s onwards. Analysis of choices and uncertainties in time series show that, depending on choices in time series and parameters, the fraction of statistically significant trends in parts of the ensemble can range from negligible to a complete 100% significance. We also find that, consistent with expectations, the number of statistically significant trends increases with increasing record length. Although our results indicate that the use multivariate regressions is a valid approach for assessing the state of Antarctic ozone hole recovery, and it can be expected that results will move towards more confidence in recovery with increasing record length, uncertainties in choices currently do not yet support formal identification of recovery of the Antarctic ozone hole. [ABSTRACT FROM AUTHOR]

The global methane (CH4) growth rate showed large variations after the eruption of Mount Pinatubo in June 1991. Both sources and sinks of tropospheric CH4 were altered following the eruption, by feedback processes between climate and tropospheric photochemistry. Such processes include Ultra Violet (UV) radiative changes due to the presence of volcanic sulfur dioxide (SO2) and sulphate aerosols in the stratosphere, and due to stratospheric ozone depletion. Changes in temperature and water vapour in the following years caused changes in tropospheric chemistry, as well as in natural emissions. We present a sensitivity study that investigates the relative effects that these processes had on tropospheric CH4 concentrations, using a simple onedimensional chemistry model representative for the global tropospheric column. To infer the changes in UV radiative fluxes, the chemistry model is coupled to a radiative transfer model.We find that the overall effect of natural processes after the eruption on the CH4 growth rate is dominated by the reduction in CH4 lifetime due to stratospheric ozone depletion. However, all the other processes are found to have non-negligible effects, and should therefore be taken into account in order to obtain a good estimate of CH4 concentrations after Pinatubo. We find that the overall effect was a small initial increase in the CH4 growth rate after the eruption, followed by a decrease of about 7 ppb yr-1 by mid-1993. When changes in anthropogenic emissions are employed according to emission inventories, an additional decrease of about 5 ppb yr-1 in the CH4 growth rate is obtained between the years 1991 and 1993. The results using the simplified single column model are in good qualitative agreement with observed changes in the CH4 growth rate. Further analysis, taking into account changes in the dynamics of the atmosphere, variations in emissions from biomass burning, and in biogenic emissions of non-methane volatile organic compounds (NMVOC), requires the use of a full threedimensional model. [ABSTRACT FROM AUTHOR]

We have developed an advanced chemical data assimilation system to combine observations of chemical compounds from multiple satellites. NO2, O3, CO, and HNO3 measurements from the Ozone Monitoring Instrument (OMI), Tropospheric Emission Spectrometer (TES), Measurement of Pollution in the Troposphere (MOPITT), and Microwave Limb Sounder (MLS) satellite instruments are assimilated into the global chemical transport model CHASER for the years 2006-2007. The CHASER data assimilation system (CHASER-DAS), based on the local ensemble transform Kalman filter technique, simultaneously optimizes the chemical species, as well as the emissions of O3 precursors, while taking their chemical feedbacks into account. With the available datasets, an improved description of the chemical feedbacks can be obtained, especially related to the NOx-CO-OH-O3 set of chemical reactions. Comparisons against independent satellite, aircraft, and ozonesonde data show that the data assimilation results in substantial improvements for various chemical compounds. These improvements include a reduced negative tropospheric NO2 column bias (by 40-85 %), a reduced negative CO bias in the Northern Hemisphere (by 40-90 %), and a reduced positive O3 bias in the middle and upper troposphere (from 30-40% to within 10 %). These changes are related to increased tropospheric OH concentrations by 5-15% in the tropics and the Southern Hemisphere in July. Observing System Experiments (OSEs) have been conducted to quantify the relative importance of each data set on constraining the emissions and concentrations. The OSEs confirm that the assimilation of individual data sets results in a strong influence on both assimilated and non-assimilated species through the inter-species error correlation and the chemical coupling described by the model. The simultaneous adjustment of the emissions and concentrations is a powerful approach to correcting the tropospheric ozone budget and profile analyses. [ABSTRACT FROM AUTHOR]

Three global Chemistry Transport Models - MOZART, MOCAGE, and TM5 - as well as MOZART coupled to the IFS meteorological model including assimilation of ozone (O3) and carbon monoxide (CO) satellite column retrievals, have been compared to surface measurements and MOZAIC vertical profiles in the troposphere over Western/ Central Europe for summer 2003. The models reproduce the meteorological features and enhancement of pollution during the period 2-14 August, but not fully the ozone and CO mixing ratios measured during that episode. Modified normalised mean biases are around -25% (except ~5% for MOCAGE) in the case of ozone and from -80% to -30% for CO in the boundary layer above Frankfurt. The coupling and assimilation of CO columns from MOPITT overcomes some of the deficiencies in the treatment of transport, chemistry and emissions in MOZART, reducing the negative biases to around 20%. The high reactivity and small dry deposition velocities in MOCAGE seem to be responsible for the overestimation of O3 in this model. Results from sensitivity simulations indicate that an increase of the horizontal resolution to around 1°×1° and potential uncertainties in European anthropogenic emissions or in long-range transport of pollution cannot completely account for the underestimation of CO and O3 found for most models. A process-oriented TM5 sensitivity simulation where soil wetness was reduced results in a decrease in dry deposition fluxes and a subsequent ozone increase larger than the ozone changes due to the previous sensitivity runs. However this latest simulation still underestimates ozone during the heat wave and overestimates it outside that period. Most probably, a combination of the mentioned factors together with underrepresented biogenic emissions in the models, uncertainties in the modelling of vertical/horizontal transport processes in the proximity of the boundary layer as well as limitations of the chemistry schemes are responsible for the underestimation of ozone (overestimation in the case of MOCAGE) and CO found in the models during this extreme pollution event. [ABSTRACT FROM AUTHOR]

Tropospheric O3 column estimates are produced and evaluated from spaceborne O3 observations by the subtraction of assimilated O3 profile observations from total column observations, the so-called Tropospheric O3 ReAnalysis or TORA method. Here we apply the TORA method to six years (1996-2001) of ERS-2 GOME/TOMS total O3 and ERS-2 GOME O3 profile observations using the TM5 global chemistry-transport model with a linearized O3 photochemistry parameterization scheme. Free running TM5 simulations show good agreement with O3 sonde observations in the upper-tropospheric and lower stratospheric region (UTLS), both for short day-to-day variability as well as for monthly means. The assimilation of GOME O3 profile observations counteracts the mid-latitude stratospheric O3 drift caused by the overstrong stratospheric meridional circulation in TM5. Assimilation of GOME O3 profile observations also improves the bias and correlations in the tropical UTLS region but slightly degrades the modelto- sonde correlations and bias of extra-tropical UTLS. We suggest that this degradation is related to the large ground pixel size of the GOME O3 measurements (960×100 km) in combination with retrieval and calibration errors. The added value of the assimilation of GOME O3 profiles compared to stand-alone model simulations lays in the long term variations of stratospheric O3, not in short term synoptic variations. The evaluation of daily and monthly tropospheric O3 columns obtained from total column observations and using the TORA methodology shows that the use of GOME UVVIS nadir O3 profiles in combination with the spatial resolution of the model does not result in satisfactory residual tropospheric ozone columns. [ABSTRACT FROM AUTHOR]

Air quality and surface emission inversions are likely to be focal points for future satellite missions on atmospheric composition. Most important for these applications is sensitivity to the atmospheric composition in the lowest few kilometers of the troposphere. Reduced sensitivity by clouds needs to be minimized. In this study we have quantified the increase in number of useful footprints, i.e. footprints which are sufficient cloud-free, as a function of sensor resolution (footprint area). High resolution (1 km x 1 km) MODIS TERRA cloud mask observations are aggregated to lower resolutions. Statistics for different thresholds on cloudiness are applied. For each month in 2004 four days of MODIS data are analyzed. Globally the fraction of cloud-free observations drops from 16% at 100 km² resolution to only 3% at 10 000 km² if not a single MODIS observation within a footprint is allowed to be cloudy. If up to 5% or 20% of a footprint is allowed to be cloudy, the fraction of cloud-free observations is 9% or 17%, respectively, at 10 000 km² resolution. The probability of finding cloud-free observations for different sensor resolutions is also quantified as a function of geolocation and season, showing examples over Europe and northern South America (ITCZ). [ABSTRACT FROM AUTHOR]