Abstract. In this study, we provide a comprehensive analysis of aerosol interaction with warm boundary layer clouds over the South-East Atlantic. We use aerosol and cloud parameters derived from MODIS observations, together with co-located CALIPSO estimates of the layer altitudes, to derive statistical relationships between aerosol concentration and cloud properties. The CALIPSO products are used to differentiate between cases of mixed cloud-aerosol layers from cases where the aerosol is located well-above the cloud top. This technique allows us to obtain more reliable estimates of the aerosol indirect effect than from simple relationships based on vertically integrated measurements of aerosol and cloud properties. Indeed, it permits us to somewhat distinguish the effects of aerosol and meteorology on the clouds, although it is not possible to fully ascertain the relative contribution of each on the derived statistics.Consistently with the results from previous studies, our statistics clearly show that aerosol affects cloud microphysics, decreasing the Cloud Droplet Radius (CDR). The same data indicate a concomitant strong decrease in cloud Liquid Water Path (LWP), which is inconsistent with the hypothesis of aerosol inhibition of precipitation (Albrecht, 1989). We hypothesise that the observed reduction in LWP is the consequence of dry air entrainment at cloud top. The combined effect of CDR decrease and LWP decrease leads to rather small sensitivity of the Cloud Optical Thickness (COT) to an increase in aerosol concentration. The analysis of MODIS-CALIPSO coincidences also evidences an aerosol enhancement of low cloud cover. Surprisingly, the Cloud Fraction (CLF) response to aerosol invigoration is much stronger when (absorbing) particles are located above cloud top than in cases of physical interaction. This result suggests a relevant aerosol radiative effect on low cloud occurrence: absorbing particles above the cloud top may heat the corresponding atmosphere layer, decrease the vertical temperature gradient, increase the low tropospheric stability and provide favourable conditions for low cloud formation.We also analyse the impact of anthropogenic aerosols on precipitation, through the statistical analysis of CDR-COT co-variations. A COT value of 10 is found to be the threshold beyond which precipitation is mostly formed, in both clean and polluted environments. For larger COT, polluted clouds show evidence of precipitation suppression.Results suggest the presence of two competing mechanisms governing LWP response to aerosol invigoration: a drying effect due to aerosol enhanced entrainment of dry air at cloud top (predominant for optically thin clouds) and a moistening effect due to aerosol inhibition of precipitation (predominant for optically thick clouds).

[1] Aerosol interaction with clouds is the main uncertainty for the quantification of the anthropogenic forcing on climate. The first step of the so-called "aerosol indirect effect" is the change of cloud droplet size distribution when seeded by anthropogenic aerosols. Satellite data provide the density and diversity of observations needed for a statistical estimate of this effect. Numerous such studies have demonstrated the correlation between aerosol load and Cloud Droplet Radius (CDR) and a few have quantified the impact of aerosol on the microphysics. Here, we go one step further by using the profiles from the spaceborne CALIPSO lidar that indicates the respective position of aerosol and cloud layers. The results show that, when aerosol and cloud layers are clearly separated, there is no correlation between aerosol load and CDR. On the other hand, when the lidar profile indicates mixing, there is a strong correlation. We focus on the stratocumulus cloud fields off the coast of Namibia and Angola that are seeded by biomass burning aerosols from Africa. The log-log slope of CDR and a proxy of the condensation nuclei number are −0.24 in excellent agreement with theoretical estimate. When the vertical profile information is not used, the slope is significantly smaller. Citation: Costantino, L., and F.-M.Bréon (2010), Analysis of aerosol-cloud interaction from multisensor satellite observations, Geophys.

Abstract. Present and future satellite observations offer great potential for monitoring air quality on a daily and global basis. However, measurements from currently orbiting satellites do not allow a single sensor to accurately probe surface concentrations of gaseous pollutants such as tropospheric ozone. Combining information from IASI (Infrared Atmospheric Sounding Interferometer) and GOME-2 (Global Ozone Monitoring Experiment-2) respectively in the TIR and UV spectra, a recent multispectral method (referred to as IASI+GOME-2) has shown enhanced sensitivity for probing ozone in the lowermost troposphere (LMT, below 3 km altitude) with maximum sensitivity down to 2.20 km a.s.l. over land, while sensitivity for IASI or GOME-2 alone only peaks at 3 to 4 km at the lowest.In this work we develop a pseudo-observation simulator and evaluate the potential of future EPS-SG (EUMET-SAT Polar System -Second Generation) satellite observations, from new-generation sensors IASI-NG (Infrared Atmospheric Sounding Interferometer -New Generation) and UVNS (Ultraviolet Visible Near-infrared Shortwaveinfrared), to observe near-surface O 3 through the IASI-NG+UVNS multispectral method. The pseudo-real state of the atmosphere is provided by the MOCAGE (MOdèle de Chimie Atmosphérique à Grande Échelle) chemical transport model. We perform full and accurate forward and inverse radiative transfer calculations for a period of 4 days (8-11 July 2010) over Europe.In the LMT, there is a remarkable agreement in the geographical distribution of O 3 partial columns between IASI-NG+UVNS pseudo-observations and the corresponding MOCAGE pseudo-reality. With respect to synthetic IASI+GOME-2 products, IASI-NG+UVNS shows a higher correlation between pseudo-observations and pseudo-reality, which is enhanced by about 12 %. The bias on high ozone retrieval is reduced and the average accuracy increases by 22 %. The sensitivity to LMT ozone is also enhanced. On average, the degree of freedom for signal is higher by 159 % over land (from 0.29 to 0.75) and 214 % over ocean (from 0.21 to 0.66). The mean height of maximum sensitivity for the LMT peaks at 1.43 km over land and 2.02 km over ocean, respectively 1.03 and 1.30 km below that of IASI+GOME-2. IASI-NG+UVNS also shows good retrieval skill in the surface-2 km altitude range. It is one of a kind for retrieving ozone layers of 2-3 km thickness, in the first 2-3 km of the atmosphere. IASI-NG+UVNS is expected to largely enhance the capacity to observe ozone pollution from space.

In this study, we provide a comprehensive analysis of aerosol interaction with warm boundary layer clouds, over South-East Atlantic. We use MODIS retrievals to derive statistical relationships between aerosol concentration and cloud properties, together with co-located CALIPSO estimates of cloud and aerosol layer altitudes. The latter are used to differentiate between cases of mixed and interacting cloud-aerosol layers from cases where the aerosol is located well-above the cloud top. This strategy allows, to a certain extent, to isolate real aerosol-induced effect from meteorology. <br><br> Similar to previous studies, statistics clearly show that aerosol affects cloud microphysics, decreasing the Cloud Droplet Radius (CDR). The same data indicate a concomitant strong decrease in cloud Liquid Water Path (LWP), in evident contrast with the hypothesis of aerosol inhibition of precipitation (Albrecht, 1989). Because of this water loss, probably due to the entrainment of dry air at cloud top, Cloud Optical Thickness (COT) is found to be almost insensitive to changes in aerosol concentration. The analysis of MODIS-CALIPSO coincidences also evidenced an aerosol enhancement of low cloud cover. Surprising, the Cloud Fraction (CLF) response to aerosol invigoration is much stronger when (absorbing) particles are located above cloud top, than in cases of physical interaction, This result suggests a relevant aerosol radiative effect on low cloud occurrence. Heating the atmosphere above the inversion, absorbing particles above cloud top may decrease the vertical temperature gradient, increase the low tropospheric stability and provide favorable conditions for low cloud formation. <br><br> We also focus on the impact of anthropogenic aerosols on precipitation, through the statistical analysis of CDR-COT co-variations. A COT value of 10 is found to be the threshold beyond which precipitation mostly forms, in both clean and polluted environments. For larger COT, polluted clouds showed evidence of precipitation suppression. Results suggest the presence of two competing mechanisms governing LWP response to aerosol invigoration: a drying effect due to aerosol enhanced entrainment of dry air at cloud top (predominant for optically thin clouds) and a moistening effect due to aerosol inhibition of precipitation (predominant for optically thick clouds)

The net effect of aerosol Direct Radiative Forcing (DRF) is the balance between the scattering effect that reflects solar radiation back to space (cooling), and the absorption that decreases the reflected sunlight (warming). The amplitude of these two effects and their balance depends on the aerosol load, its absorptivity, the cloud fraction and the respective position of aerosol and cloud layers.

In this study, we use the information provided by CALIOP (CALIPSO satellite) and MODIS (AQUA satellite) instruments as input data to a Rapid Radiative Transfer Model (RRTM) and quantify the shortwave (SW) aerosol direct atmospheric forcing, over the South-East Atlantic. The combination of the passive and active measurements allows estimates of the horizontal and vertical distributions of the aerosol and cloud parameters. We use a parametrization of the Single Scattering Albedo (SSA) based on the satellite-derived Angstrom coefficient.

The South East Atlantic is a particular region, where bright stratocumulus clouds are often topped by absorbing smoke particles. Results from radiative transfer simulations confirm the similar amplitude of the cooling effect, due to light scattering by the aerosols, and the warming effect, due to the absorption by the same particles. Over six years of satellite retrievals, from 2005 to 2010, the South-East Atlantic all-sky SW DRF is −0.03 W m⁻², with a spatial standard deviation of 8.03 W m⁻². In good agreement with previous estimates, statistics show that a cloud fraction larger than 0.5 is generally associated with positive all-sky DRF. In case of cloudy-sky and aerosol located only above the cloud top, a SSA larger than 0.91 and cloud optical thickness larger than 4 can be considered as threshold values, beyond which the resulting radiative forcing becomes positive

Abstract. Up-to-date and accurate emission inventories for air pollutants are essential for understanding their role in the formation of tropospheric ozone and particulate matter at various temporal scales, for anticipating pollution peaks and for identifying the key drivers that could help mitigate their emissions. This paper describes the Bayesian variational inverse system PYVAR-CHIMERE, which is adapted to the inversion of reactive species. Complementarily with bottom-up inventories, this system aims at updating and improving the knowledge on the high spatio-temporal variability of emissions of air pollutants and their precursors. The system is designed to use any type of observations, such as satellite observations or surface stations. The potential of PYVAR-CHIMERE is illustrated with one-day inversions of CO and NO2 emissions in Europe, using the MOPITT and OMI satellite observations (for CO and for NO2, respectively).

Abstract. Up-to-date and accurate emission inventories for air pollutants are essential for understanding their role in the formation of tropospheric ozone and particulate matter at various temporal scales, for anticipating pollution peaks and for identifying the key drivers that could help mitigate their concentrations. This paper describes the Bayesian variational inverse system PYVAR-CHIMERE, which is now adapted to the inversion of reactive species. Complementarily with bottom-up inventories, this system aims at updating and improving the knowledge on the high spatiotemporal variability of emissions of air pollutants and their precursors. The system is designed to use any type of observations, such as satellite observations or surface station measurements. The potential of PYVAR-CHIMERE is illustrated with inversions of both carbon monoxide (CO) and nitrogen oxides (NOx) emissions in Europe, using the MOPITT and OMI satellite observations, respectively. In these cases, local increments on CO emissions can reach more than +50 %, with increases located mainly over central and eastern Europe, except in the south of Poland, and decreases located over Spain and Portugal. The illustrative cases for NOx emissions also lead to large local increments (> 50 %), for example over industrial areas (e.g., over the Po Valley) and over the Netherlands. The good behavior of the inversion is shown through statistics on the concentrations: the mean bias, RMSE, standard deviation, and correlation between the simulated and observed concentrations. For CO, the mean bias is reduced by about 27 % when using the posterior emissions, the RMSE and the standard deviation are reduced by about 50 %, and the correlation is strongly improved (0.74 when using the posterior emissions against 0.02); for NOx, the mean bias is reduced by about 24 % and the RMSE and the standard deviation are reduced by about 7 %, but the correlation is not improved. We reported strong non-linear relationships between NOx emissions and satellite NO2 columns, now requiring a fully comprehensive scientific study.

Abstract. In this work we perform numerical simulations of convective gravity waves (GWs), using the WRF (Weather Research and Forecasting) model. We first run an idealized, simplified and highly resolved simulation with model top at 80 km. Below 60 km of altitude, a vertical grid spacing smaller than 1 km is supposed to reliably resolve the effects of GW breaking. An eastward linear wind shear interacts with the GW field generated by a single convective thunderstorm. After 70 min of integration time, averaging within a radius of 300 km from the storm centre, results show that wave breaking in the upper stratosphere is largely dominated by saturation effects, driving an average drag force up to −41 m s −1 day −1 . In the lower stratosphere, mean wave drag is positive and equal to 4.4 m s −1 day −1 .In a second step, realistic WRF simulations are compared with lidar measurements from the NDACC network (Network for the Detection of Atmospheric Composition Changes) of gravity wave potential energy (E p ) over OHP (Haute-Provence Observatory, southern France). Using a vertical grid spacing smaller than 1 km below 50 km of altitude, WRF seems to reliably reproduce the effect of GW dynamics and capture qualitative aspects of wave momentum and energy propagation and transfer to background mean flow. Averaging within a radius of 120 km from the storm centre, the resulting drag force for the study case (2 h storm) is negative in the higher (−1 m s −1 day −1 ) and positive in the lower stratosphere (0.23 m s −1 day −1 ).Vertical structures of simulated potential energy profiles are found to be in good agreement with those measured by lidar. E p is mostly conserved with altitude in August while, in October, E p decreases in the upper stratosphere to grow again in the lower mesosphere. On the other hand, the magnitude of simulated wave energy is clearly underestimated with respect to lidar data by about 3-4 times.