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A unique Rayleigh-Mie Doppler lidar capable of wind measurements in the 5-50 km altitude range is operated routinely at La Reunion island (21° S, 55° E) since 2015. We evaluate instrument’s capacities in capturing fine structures in stratospheric wind profiles and their temporal and spatial variability through comparison with collocated radiosoundings and ECMWF analysis. Perturbations in the wind velocity are used to retrieve gravity wave frequency spectrum.

A unique Rayleigh-Mie Doppler wind lidar, measuring Doppler shift between the emitted and backscattered light using directdetection technique is deployed at Observatory of Haute Provence Southern France) and at Reunion island (tropical Indian Ocean). The instrument was shown capable of wind measurements between 5 and 50 km with accuracy better than 1 m/s up to 30 km. The system consists of a monomode Nd:Yag laser operating at 532 nm, three telescopes and a double-edge Fabry-Perot interferometer. The laser light is sent alternatively in the vertical as well as zonal and meridional directions at 40° from the zenith using a rotating mirror. The two components of the horizontal wind are obtained from the measurement of the Doppler shift of the return signal spectrally filtered by the Fabry-Perot etalon. After demonstration of the method in 1989 the measurements were used for studying stratospheric dynamics as well as for constructing wind climatology up to 50 km altitude. A new system, featuring a more compact design was installed at Maïdo observatory at Reunion Island (21° S). The design of the instrument, results of observations and comparison against GPS radiosondes are presented. Application of Doppler lidar for validation of the future ADM-Aeolus satellite mission is discussed as well.

A new lidar system devoted to tropospheric and lower stratospheric water vapor measurements has been installed at the Maïdo altitude station facility of Réunion island, in the southern subtropics. To evaluate the performances and the capabilities of the new system with a particular focus on UTLS (Upper Troposphere Lower Stratosphere) measurements, the Maïdo Lidar Calibration Campaign (MALICCA) was performed in April 2013. Varying the characteristics of the transmitter and the receiver components, different system configuration scenarios were tested and possible parasite signals (fluorescent contamination, rejection) were investigated. A hybrid calibration methodology has been set up and validated to insure optimal lidar calibration stability with time. In particular, the receiver transmittance is monitored through the calibration lamp method that, at the moment, can detect transmittance variations greater than 10-15 %. Calibration coefficients are then calculated through the hourly values of IWV (Integrated Water Vapor) provided by the co-located GPS. The comparison between the constants derived by GPS and Vaisala RS92 radiosondes launched at Maïdo during MALICCA, points out an acceptable agreement in terms of accuracy of the mean calibration value (with a difference of approximately 2-3 %), but a significant difference in terms of variability (14% vs. 7-9 %, for GPS and RS92 calibration procedures, respectively). We obtained a relatively good agreement between the lidar measurements and 15 co-located and simultaneous RS92 radiosondes. A relative difference below 10% is measured in the low and middle troposphere (2-10 km). The upper troposphere (up to 15 km) is characterized by a larger spread (approximately 20 %), because of the increasing distance between the two sensors. To measure water vapor in the UTLS region, nighttime and monthly water vapor profiles are presented and compared. The good agreement between the lidar monthly profile and the mean WVMR profile measured by satellite MLS (Microwave Limb Sounder) has been used as a quality control procedure of the lidar product, attesting the absence of significant wet biases and validating the calibration procedure. Due to its performance and location, the MAIDO H2O lidar will become a reference instrument in the southern subtropics, insuring the long-term survey of the vertical distribution of water vapor. Furthermore, this system allows the investigation of several scientific themes, such as stratosphere- troposphere exchange, tropospheric dynamics in the subtropics, and links between cirrus clouds and water vapor. [ABSTRACT FROM AUTHOR]

A new lidar system devoted to tropospheric and lower stratospheric water vapor measurements has been installed at the MaÏdo altitude station facility of La Reunion Island, in the southern subtropics. The main objectives of the MAÏdo LIdar Calibration Campaign (MALICCA), performed in April 2013, were to validate the system, to set up a calibration methodology, to compare the acquired water profiles with radiosonde measurements and to evaluate its performances and capabilities with a particular focus on the UTLS measurements. Varying the characteristics of the transmitter and the receiver components, different system configuration scenarios were tested and possible parasite signals (fluorescent contamination, rejection) were investigated. A hybrid calibration methodology has been set up and validated to insure optimal lidar calibration stability with time. In particular, the receiver transmittance is monitored through the calibration lamp method that, at the moment, can detect transmittance variations greater than 1-15 %. Calibration coefficients are then calculated through the hourly values of IWV provided by the co-located GPS. The comparison between the constants derived by GPS and Vaisala RS92 radiosondes launched at MaÏdo during MALICCA, points out an acceptable agreement in terms of accuracy of the mean calibration value (with a difference of approximately 2-3 %), but a significant difference in terms of variability (14 vs. 7-9 %, for GPS and RS92 calibration procedures, respectively). We obtained a relatively good agreement between the lidar measurements and co-located and simultaneous RS92 radiosondes. A relative difference below 10% is measured in low and middle troposphere (2-10 km). The upper troposphere (up to 15 km) is characterized by a larger spread (approximately 20 %), because of the in creasing distance between the two sensors. To measure water vapor in the UTLS region, nighttime and monthly water vapor profiles are presented and compared. The good agreement between the lidar monthly profile and the mean WVMR profile measured by satellite MLS has been used as a quality control procedure of the lidar product, attesting the absence of significant wet biases and validating the calibration procedure. Thanks to its performance and location, the MAIDO H2O lidar is devoted to become a reference instrument in the southern subtropics, allowing to insure the long-term survey of the vertical distribution of water vapor, and to document scientific themes such as stratosphere-troposphere exchange, tropospheric dynamics in the subtropics, links between cirrus clouds and water vapor. [ABSTRACT FROM AUTHOR]

The objective of this paper is to deliver the most accurate ozone (O3) and carbon monoxide (CO) climatology for the pure troposphere only, i.e. exclusively from the ground to the dynamical tropopause on an individual profile basis. The results (profiles and columns) are derived solely from the Measurements of OZone and water vapour by in-service AIrbus airCraft programme (MOZAIC) over 15 years (1994-2009). The study, focused on the northern midlatitudes [24-50° N] and [119°W-140° E], includes more than 40 000 profiles over 11 sites to give a quasi-global zonal picture. Considering all the sites, the pure tropospheric column peak-to-peak seasonal cycle ranges are 23.7-43.2DU for O3 and 1.7-6.9×1018 moleculescm-2 for CO. The maxima of the seasonal cycles are not in phase, occurring in February-April for CO and May-July for O3. The phase shift is related to the photochemistry and OH removal efficiencies. The purely tropospheric seasonal profiles are characterized by a typical autumn-winter/spring-summer O3 dichotomy (except in Los Angeles, Eastmed - a cluster of Cairo and Tel Aviv - and the regions impacted by the summer monsoon) and a summer-autumn/winter-spring CO dichotomy. We revisit the boundary-layer, mid-tropospheric (MT) and uppertropospheric (UT) partial columns using a new monthly varying MT ceiling. Interestingly, the seasonal cycle maximum of the UT partial columns is shifted from summer to spring for O3 and to very early spring for CO. Conversely, the MT maximum is shifted from spring to summer and is associated with a summer (winter) MT thickening (thinning). Lastly, the pure tropospheric seasonal cycles derived from our analysis are consistent with the cycles derived from spaceborne measurements, the correlation coefficients being r = 0.6-0.9 for O3 and r > 0.9 for CO. The cycles observed from space are nevertheless greater than MOZAIC for O3 (by 9-18 DU) and smaller for CO (up to 1×1018 moleculescm-2). The larger winter O3 difference between the two data sets suggests probable stratospheric contamination in satellite data due to the tropopause position. The study underlines the importance of rigorously discriminating between the stratospheric and tropospheric reservoirs and avoiding use of a monthly averaged tropopause position without this strict discrimination in order to assess the pure O3 and CO tropospheric trends. [ABSTRACT FROM AUTHOR]

In order to evaluate the observed high rural ozone levels in the eastern Mediterranean area during summertime, vertical profiles of ozone measured in the period 1994-2008 in the framework of the MOZAIC project (Measurement of Ozone and Water Vapor by Airbus in Service Aircraft) over the eastern Mediterranean basin (Cairo, Tel Aviv, Heraklion, Rhodes, Antalya) were analyzed, focusing in the lower troposphere (1.5-5 km). At first, vertical profiles collected during extreme days with very high or very low tropospheric ozone mixing ratios have been examined together with the corresponding back-trajectories. Also, the average profiles of ozone, relative humidity, carbon monoxide, temperature gradient and wind speed corresponding to the 7% highest and the 7% lowest ozone mixing ratios for the 1500-5000m height layer for Cairo and Tel Aviv have been examined and the corresponding composite maps of geopotential heights at 850 hPa have been plotted. Based on the above analysis, it turns out that the lower-tropospheric ozone variability over the eastern Mediterranean area is controlled mainly by the synoptic meteorological conditions, combined with local topographical and meteorological features. In particular, the highest ozone concentrations in the lower troposphere and subsequently in the boundary layer are associated with largescale subsidence of ozone-rich air masses from the upper troposphere under anticyclonic conditions while the lowest ozone concentrations are associated with low pressure conditions inducing uplifting of boundary-layer air, poor in ozone and rich in relative humidity, to the lower troposphere. [ABSTRACT FROM AUTHOR]

Since the nineties, atmospheric measurement systems have been deployed at Reunion Island, mainly for monitoring the atmospheric composition in the framework of NDSC/NDACC (Network for the Detection of Stratospheric Change/Network for the Detection of Atmospheric Composition Change). The location of Reunion Island presents a great interest because there are very few multi-instrumented stations in the tropics and particularly in the southern hemisphere. In 2012, a new observatory was commissioned in Maïdo at 2200m above sea level: it hosts various instruments for atmospheric measurements, including lidar systems, spectro-radiometers and in situ gas and aerosol measurements. This new high-altitude Maïdo station provides an opportunity: 1. to improve the performance of the optical instruments above the marine boundary layer, and to open new perspectives on upper troposphere and lower stratosphere studies; 2. to develop in situ measurements of the atmospheric composition for climate change surveys, in a reference site in the tropical/subtropical region of the southern hemisphere; 3. to offer trans-national access to host experiments or measurement campaigns for focused process studies. [ABSTRACT FROM AUTHOR]

Since the nineties, atmospheric measurement systems have been deployed at Reunion Island, mainly for monitoring the atmospheric composition in the framework of NDSC/NDACC (Network for the Detection of Stratospheric Change/Network for the Detection of Atmospheric Composition Change). The location of Reunion Island presents a great interest because there are very few multi-instrumented stations in the tropics and particularly in the Southern Hemisphere. In 2012, a new observatory was commissioned in Maïdo at 2200ma.s.l.: it hosts various instruments for atmospheric measurements, including LiDAR systems, spectro-radiometers and in situ gases and aerosols measurements. This new high-altitude Maïdo station allows: 1. To improve the performance of the optical instruments above the marine boundary layer, and to open new perspectives on upper troposphere and lower stratosphere studies. 2. To develop in-situ measurements of the atmospheric composition for climate change survey, in a reference site in the tropical/subtropical region of the Southern Hemisphere. 3. To offer trans-national access to host experiments or measurement campaigns for focused process studies. [ABSTRACT FROM AUTHOR]

The article discusses a study that presents a quality assessment of the Infrared Atmospheric Sounding Interferometer (IASI) carbon monoxide (CO) profiles retrieved by the two different retrieval algorithms SOFRID and FORLI. It indicates that SOFRID and FORLI showed biases no higher than 13%compared to the MOZAIC reference set. It found discrepancies between the two IASI products and MOZAIC.

This work evaluates the IASI CO product against independent in-situ aircraft data from the MOZAIC program and the POLARCAT aircraft campaign. The validation is carried out by analysing the impact of assimilation of eight months of IASI CO columns retrieved for the period of May to December 2008 into the global chemistry transport model LMDz-INCA. A modelling system based on a sub-optimal Kalman filter was developed and a specific treatment that takes into account the representativeness of observations at the scale of the model grid is applied to the IASI CO columns and associated errors before their assimilation in the model. Comparisons of the assimilated CO profiles with in situ CO measurements indicate that the assimilation leads to a considerable improvement of the model simulations in the middle troposphere as compared with a control run with no assimilation. Model biases in the simulation of background values are reduced and improvement in the simulation of very high concentrations is observed. The improvement is due to the transport by the model of the information present in the IASI CO retrievals. Our analysis also shows the impact of assimilation of CO on the representation of transport into the Arctic region during the POLARCAT summer campaign. A considerable increase in CO mixing ratios over the Asian source region was observed when assimilation was used leading to much higher values of CO during the cross-pole transport episode. These higher values are in good agreement with data from the POLARCAT flights that sampled this plume. [ABSTRACT FROM AUTHOR]

A detailed 3-D evaluation of an ensemble of five regional Chemistry Transport Models (RCTM) and one global CTM with focus on free tropospheric ozone over Europe is presented. It is performed over a summer period (June to August 2008) in the context of the GEMS-RAQ project. A data set of about 400 vertical ozone profiles from balloon soundings and commercial aircraft at 11 different locations is used for model evaluation, in addition to satellite measurements with the infrared nadir sounder (IASI) showing largest sensitivity to free tropospheric ozone. In the middle troposphere, the four regional models using the same top and boundary conditions from IFS-MOZART exhibit a systematic negative bias with respect to observed profiles of about -20 %. Root Mean Square Error (RMSE) values are constantly growing with altitude, from 22% to 32% to 53 %, respectively for 0-2 km, 2-8 km and 8-10 km height ranges. Lowest correlation is found in the middle troposphere, with minimum coefficients (R) between 0.2 to 0.45 near 8 km, as compared to 0.7 near the surface and similar values around 10 km. A sensitivity test made with the CHIMERE mode also shows that using hourly instead of monthly chemical boundary conditions generally improves the model skill (i.e. improve RMSE and correlation). Lower tropospheric 0-6 km partial ozone columns derived from IASI show a clear North- South gradient over Europe, which is qualitatively reproduced by the models. Also the temporal variability showing decreasing ozone concentrations in the lower troposphere (0-6 km columns) during summer is well reproduced by models even if systematic bias remains (the value of the bias being also controlled by the type of used boundary conditions). A multi-day case study of a trough with low tropopause was conducted and showed that both IASI and models were able to resolve strong horizontal gradients of middle and upper tropospheric ozone occurring in the vicinity of an upper tropospheric frontal zone. [ABSTRACT FROM AUTHOR]

A global chemistry-climate model LMDz_INCA is used to investigate the contribution of African and Asian emissions to tropospheric ozone over Central and West Africa during the summer monsoon. The model results show that ozone in this region is most sensitive to lightning NOx and to Central African biomass burning emissions. However, other emission categories also contribute significantly to regional ozone. The maximum ozone changes due to lightning NOx occur in the upper troposphere between 400 hPa and 200 hPa over West Africa and downwind over the Atlantic Ocean. Biomass burning emissions mainly influence ozone in the lower and middle troposphere over Central Africa, and downwind due to westward transport. Biogenic emissions of volatile organic compounds, which can be uplifted from the lower troposphere to higher altitudes by the deep convection that occurs over West Africa during the monsoon season, lead to maximum ozone changes in the lower stratosphere region. Soil NOx emissions over the Sahel region make a significant contribution to ozone in the lower troposphere. In addition, convective uplift of these emissions and subsequent ozone production are also an important source of ozone in the upper troposphere over West Africa. Concerning African anthropogenic emissions, they only make a small contribution to ozone compared to the other emission categories. The model results indicate that most ozone changes due to African emissions occur downwind, especially over the Atlantic Ocean, far from the emission regions. The import of Asian emissions also makes a considerable contribution to ozone concentrations above 150 hPa and has to be taken into account in studies of the ozone budget over Africa. Using IPCC AR5 (Intergovernmental Panel on Climate Change: Fifth Assessment Report) estimates of anthropogenic emissions for 2030 over Africa and Asia. model calculations show larger changes in ozone over Africa due to growth in Asian emissions compared to African emissions over the next 20 yr. [ABSTRACT FROM AUTHOR]

A modelling system for assimilation of CO total columns measured by the IASI/MetOp was developed. The system, based on a sub-optimal Kalman filter coupled with the LMDz-INCA chemistry transport model, allows both assimilating long periods of historical data and making rapid forecasts of the CO concentrations in the middle troposphere based on latest available measurements. Tests of the forecast system were conducted during the international POLARCAT campaigns. A specific treatment that takes into account the representativeness of observations at the scale of the model grid is applied to the IASI CO columns and associated errors before their assimilation in the model. This paper presents the results of assimilation of eight months of historical satellite data measured in 2008. Comparisons of the assimilated CO profiles with independent in situ CO measurements from the MOZAIC program and the POLARCAT aircraft campaigns indicate that the assimilation leads to a considerable improvement of the model simulations in the middle troposphere as compared with a control run with no assimilation. Model biases in the simulation of background values are reduced and improvement in the simulation of very high concentrations is observed. The improvement is due to the transport by the model of the information present in the IASI CO retrievals. The consistency of the improvement contributes to the validation of the IASI CO data. [ABSTRACT FROM AUTHOR]

A detailed 3-D evaluation of an ensemble of five regional CTM's and one global CTM with focus on free tropospheric ozone over Europe is presented. It is performed over a summer period (June to August 2008) in the context of the GEMS-RAQ project. A data set of about 400 vertical ozone profiles from balloon soundings and commercial aircraft at 11 different locations is used for model evaluation, in addition to satellite measurements with the infrared nadir IASI sounder showing largest sensitivity to free tropospheric ozone. In the free troposphere, models using the same top and boundary conditions from MOZART-IFS exhibit a systematic negative bias with respect to observed profiles of about -20%. RMSE values are constantly growing with altitude, from 22% to 32% to 53%, respectively for 0-2 km, 2-8 km and 8-10 km height ranges. Lowest correlation is found in the free troposphere, with minimum coefficients (R) between 0.2 to 0.45 near 8 km, as compared to 0.7 near the surface and similar values around 10 km. Use of hourly instead of monthly chemical boundary conditions generally improves the model skill. Lower tropospheric 0-6 km partial ozone columns derived from IASI show a clear North-South gradient over Europe, which is qualitatively reproduced by the models. Also the temporal variability showing decreasing ozone concentrations in the lower troposphere (0-6 km columns) during summer is well catched by models even if systematic bias remains (the value of the bias being also controlled by the type of BC used). A multi-day case study of a through with low tropopause was conducted and showed that both IASI and models were able to resolve strong horizontal gradients of middle and upper tropospheric ozone occurring in the vicinity of an upper tropospheric frontal zone. [ABSTRACT FROM AUTHOR]

The ozone (O3) variability over south Asia during the 2008 post-monsoon season has been assessed using measurements from the MetOP-A/IASI instrument and O3 profiles retrieved with the SOftware for a Fast Retrieval of IASI Data (SOFRID). The information content study and error analyses carried out in this paper show that IASI Level 1 data can be used to retrieve tropospheric O3 columns (TOC, surface-225 hPa) and UTLS columns (225--70 hPa) with errors smaller than 20%. Validation with global radiosonde O3 profiles obtained during a period of 6 months show the excellent agreement between IASI and radiosonde for the UTLS with correlation coefficient R >0.91 and good agreement in the troposphere with correlation coefficient R > 0.74. For both the UTLS and the troposphere Relative Standard Deviations (RSD) are lower than 23%. Comparison with in-situ measurements from the MOZAIC program around Hyderabad demonstrates that IASI is able to capture the TOC inter and intra-seasonal variability in central India. Nevertheless, the agreement is mitigated by the fact that the smoothing of the true O3 profiles by the retrieval results in a reduction of the TOC variability detected by IASI relative to the variability observed by in situ instruments. The post-monsoon temporal variability of the vertical profile of O3 around Hyderabad has been investigated with MOZAIC observations. These observations from airborne instruments show that tropospheric O3 is steadily elevated during most of the studied period with the exception of two sharp drops following the crossing of tropical storms over India. Lagrangian simulations with the FLEXPART model indicate that elevated O3 concentrations in the middle troposphere near Hyderabad are associated with the transport of UTLS air-masses that have followed the Subtropical Westerly Jet (SWJ) and subsided over northern India together with boundary layer polluted air-masses transported from the Indo-gangetic plain by the north-easterly trades. Low O3 concentrations result from the uplift and westward transport of pristine air-masses from the marine boundary layer of the Bay of Bengal by tropical storms. In order to extend the analysis of tropospheric O3 variability to the whole of south Asia, we have used IASI-SOFRID O3 data. We show that IASI O3 data around Hyderabad were able to capture the fast variability revealed by MOZAIC. Furthermore, their spatio-temporal coverage demonstrates that the behaviour of tropospheric O3 observed near Hyderabad extended over most of central and south India and part of the Bay of Bengal. This result highlights the ability of the IASI sensor to capture fast changes in chemical composition related to dramatic tropical weather conditions. [ABSTRACT FROM AUTHOR]

The article presents a study which seeks to determine the performance of the GEMS/MACC models to reproduce the tropospheric vertical distribution of carbon monoxide (CO). It compares the performance of three offline chemistry transport models (CTMs) namely MOZART-3, MOCAGE and TM5. It presents a global analysis of observed CO seasonal averages and interannual variability from 2002 to 2007, and present a validation of CO estimates produced by the MACC models for 2004.

This paper presents an evaluation of a new linear parameterization valid for the troposphere and the stratosphere, based on a first order approximation of the carbon monoxide (CO) continuity equation. This linear scheme (hereinafter noted LINCO) has been implemented in the 3-D Chemical Transport Model (CTM) MOCAGE (MOdèle de Chimie Atmospherique Grande Echelle). First, a one and a half years of LINCO simulation has been compared to output obtained from a detailed chemical scheme output. The mean differences between both schemes are about ±25 ppbv (part per billion by volume) or 15% in the troposphere and ±10 ppbv or 100% in the stratosphere. Second, LINCO has been compared to diverse observations from satellite instruments covering the troposphere (Measurements Of Pollution In The Troposphere: MOPITT) and the stratosphere (Microwave Limb Sounder: MLS) and also from aircraft (Measurements of ozone and water vapour by Airbus in-service aircraft: MOZAIC programme) mostly flying in the upper troposphere and lower stratosphere (UTLS). In the troposphere, the LINCO seasonal variations as well as the vertical and horizontal distributions are quite close to MOPITT CO observations. However, a bias of ~-40 ppbv is observed at 700 hPa between LINCO and MOPITT. In the stratosphere, MLS and LINCO present similar large-scale patterns, except over the poles where the CO concentration is underestimated by the model. In the UTLS, LINCO presents small biases less than 2% compared to independent MOZAIC profiles. Third, we assimilated MOPITT CO using a variational 3DFGAT (First Guess at Appropriate Time) method in conjunction with MOCAGE for a long run of one and a half years. The data assimilation greatly improves the vertical CO distribution in the troposphere from 700 to 350 hPa compared to independent MOZAIC profiles. At 146 hPa, the assimilated CO distribution is also improved compared to MLS observations by reducing the bias up to a factor of 2 in the tropics. This study confirms that the linear scheme is able to simulate reasonably well the CO distribution in the troposphere and in the lower stratosphere. Therefore, the low computing cost of the linear scheme opens new perspectives to make free runs and CO data assimilation runs at high resolution and over periods of several years. [ABSTRACT FROM AUTHOR]

Within the African Monsoon Multidisciplinary Analysis (AMMA), we investigate the impact of nitrogen oxides produced by lightning (LiNOx) and convective transport during the West African Monsoon (WAM) upon the composition of the upper troposphere (UT) in the tropics. For this purpose, we have performed simulations with 4 state-of-the-art chemistry transport models involved within AMMA, namely MOCAGE, TM4, LMDz-INCA and p-TOMCAT. The model intercomparison is complemented with an evaluation of the simulations based on both spaceborne and airborne observations. The baseline simulations show important differences between the UT CO and O3 distributions simulated by each of the 4 models when compared to measurements from the MOZAIC program and fom the Aura/MLS spaceborne sensor. We show that such model discrepancies can be explained by differences in the convective transport parameterizations and, more particularly, the altitude reached by convective updrafts (ranging between ∼200-125 hPa). Concerning UT O3, the models exhibit a good agreement with the main observed features. Nevertheless the majority of models simulate low O3 concentrations compared to both MOZAIC and Aura/MLS observations south of the equator, and rather high concentrations in the Northern Hemisphere. Sensitivity studies are performed to quantify the effect of deep convective transport and the influence of LiNOx production on the UT composition. These clearly indicate that the CO maxima and the elevated O3 concentrations south of the equator are due to convective uplift of air masses impacted by Southern African biomass burning, in agreement with previous studies. Moreover, during the WAM, LiNOx from Africa are responsible for the highest UT O3 enhancements (10-20 ppbv) over the tropical Atlantic between 10° S-20° N. Differences between models are primarily due to the performance of the parameterizations used to simulate lightning activity which are evaluated using spaceborne observations of flash frequency. Combined with comparisons of in-situ NO measurements we show that the models producing the highest amounts of LiNOx over Africa during theWAM (INCA and p-TOMCAT) capture observed NO profiles with the best accuracy, although they both overestimate lightning activity over the Sahel. [ABSTRACT FROM AUTHOR]

We have performed simulations using a 3-D global chemistry-transport model (TM4 AMMA) to investigate the effect that continental transport of biomass burning plumes have on regional air quality over Equatorial Africa during the West African Monsoon (WAM) period in 2006. By performing a number of sensitivity studies we show that biomass burning emissions from southern Africa (0-40° S) have a strong influence on the composition of the tropical troposphere around Equatorial Africa and the outflow regions towards the west, especially between 10° S-10° N. By altering both the temporal distribution and the injection heights used for introducing the biomass burning emissions we show that changes in temporal distribution are much more important in determining the daily variability of trace gas species over the southern Atlantic than boundary layer processes. When adopting the GFEDv2 emission inventory the maximum concentrations in CO and O3 occur between 0-5° S, which coincides with the position of the southern African Easterly Jet. By comparing co-located model output with in-situ measurements made during the AMMA measurement campaign we show that the model fails to capture the tropospheric profile of CO in the burning region, as well as the "extreme" concentrations of both CO and O3 seen around 600-700 hPa above Equatorial Africa. Trajectory analysis show that the 6-hourly ECMWF meteorological fields do not allow transport of biomass burning plumes from southern Africa directly into the mid-troposphere around ∼6° N. Similar trajectory simulations repeated using an updated meteorological dataset, which assimilates additional measurement data for the African region, shows markedly different origins for pollution events and reveals that the performance of the CTM is heavily constrained by the ECMWF operational analysis data which drives the model. [ABSTRACT FROM AUTHOR]

This paper presents a comprehensive characterization of a very deep stratospheric intrusion which occurred over the British Isles on 15 August 2007. The signature of this event is diagnosed using ozonesonde measurements over Lerwick, UK (60.14° N, 1.19° W) and is also well characterized using meteorological analyses from the global operational weather prediction model of Météo-France, ARPEGE. Modelled as well as assimilated fields of both ozone (O3) and carbon monoxide (CO) have been used in order to better document this event. O3 and CO from Aura/MLS and Terra/MOPITT instruments, respectively, are assimilated into the three-dimensional chemical transport model MOCAGE of Météo-France using a variational 3-DFGAT (First Guess at Appropriate Time) method. The validation of O3 and CO assimilated fields is done using selfconsistency diagnostics and by comparison with independent observations such as MOZAIC (O3 and CO), AIRS (CO) and OMI (O3). It particularly shows in the upper troposphere and lower stratosphere region that the assimilated fields are closer to MOZAIC than the free model run. The O3 bias between MOZAIC and the analyses is -11.5 ppbv with a RMS of 22.4 ppbv and a correlation coefficient of 0.93, whereas between MOZAIC and the free model run, the corresponding values are 33 ppbv, 38.5 ppbv and 0.83, respectively. In the same way, for CO, the bias, RMS and correlation coefficient between MOZAIC and the analyses are -3.16 ppbv, 13 ppbv and 0.79, respectively, whereas between MOZAIC and the free model they are 6.3 ppbv, 16.6 ppbv and 0.71, respectively. The paper also presents a demonstration of the capability of O3 and CO assimilated fields to better describe a stratosphere-troposphere exchange (STE) event in comparison with the free run modelled O3 and CO fields. Although the assimilation of MLS data improves the distribution of O3 above the tropopause compared to the free model run, it is not sufficient to reproduce the STE event well. Assimilated MOPITT CO allows a better qualitative description of the stratospheric intrusion event. The MOPITT CO analyses appear more promising than the MLS O3 analyses in terms of their ability to capture a deep STE event. Therefore, the results of this study open the perspectives for using MOPITT CO in the STE studies. [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]

This paper presents a complete characterization of a very deep stratospheric intrusion which occurred over the British Isles on 15 August 2007. The signature of this event is diagnosed using ozonesonde measurements over Lerwick, UK (60.14° N, 1.19° W) and is also well characterized using meteorological analyses from the global operational weather prediction model of Météo-France, ARPEGE. Modelled as well as assimilated fields of both ozone (O3) and carbon monoxide (CO) have been used in order to better document this event. The paper also presents a demonstration of the capability of O3 and CO assimilated fields to better describe a stratosphere-troposphere exchange (STE) event in comparison with the free run modelled O3 and CO fields. O3 and CO from Aura/MLS and Terra/MOPITT instruments, respectively, are assimilated into the three-dimensional chemical transport model MOCAGE of Météo-France using a variational 3-D-FGAT (First Guess at Appropriate Time) method within the MOCAGE-PALM assimilation system. The usefulness of assimilated MOPITT CO data in a STE study is demonstrated in this novel result. The study shows that the use of the model MOCAGE gives consistent 3-D fields capable of describing the synoptic evolution of the event. However, modelled O3 and CO vertical distributions do not provide a quantitative evaluation of the intrusion. Although the assimilation of MLS data improves the distribution of O3 above the tropopause compared to the free model run, it is not sufficient to reproduce the stratospheric intrusion event well. Conversely, assimilated MOPITT CO allows a better description of the stratospheric intrusion event. Indeed, the horizontal distribution of the CO assimilated field is consistent with meteorological analyses. Moreover, the vertical distribution of the CO assimilated field is in accordance with the potential vorticity distribution and reveals a deeper intrusion from the lower stratosphere downward to the mid-troposphere compared to the O3 assimilated field. This study clearly demonstrates the capability of the assimilation of MOPITT CO to improve the CO distribution in the upper troposphere and lower stratosphere region. In addition, the behaviour of CO assimilated field is consistent with the synoptic evolution of the meteorological conditions. Therefore, the results of this study open the perspectives for using MOPITT CO in the STE studies. [ABSTRACT FROM AUTHOR]

This paper analyses a stratospheric injection by deep convection of biomass fire emissions over North America (Alaska, Yukon and Northwest Territories) on 24 June 2004 and its long-range transport over the eastern coast of the United States and the eastern Atlantic. The case study is based on airborne MOZAIC observations of ozone, carbon monoxide, nitrogen oxides and water vapour during the crossing of the southernmost tip of an upper level trough over the Eastern Atlantic on 30 June and on a vertical profile over Washington DC on 30 June, and on lidar observations of aerosol backscattering at Madison (University of Wisconsin) on 28 June. Attribution of the observed CO plumes to the boreal fires is achieved by backward simulations with a Lagrangian particle dispersion model (FLEXPART). A simulation with the Meso-NH model for the source region shows that a boundary layer tracer, mimicking the boreal forest fire smoke, is lofted into the lowermost stratosphere (2-5 pvu layer) during the diurnal convective cycle at isentropic levels (above 335 K) corresponding to those of the downstream MOZAIC observations. It is shown that the order of magnitude of the time needed by the parameterized convective detrainment flux to fill the volume of a model mesh (20 km horizontal, 500m vertical) above the tropopause with pure boundary layer air would be about 7.5 h, i.e. a time period compatible with the convective diurnal cycle. Over the area of interest, the maximum instantaneous detrainment fluxes deposited about 15 to 20% of the initial boundary layer tracer concentration at 335 K. According to the 275-ppbv carbon monoxide maximum mixing ratio observed by MOZAIC over Eastern Atlantic, such detrainment fluxes would be associated with a 1.4-1.8 ppmv carbon monoxide mixing ratio in the boundary layer over the source region. [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 Europe for summer 2003. The models reproduce the meteorological features and enhancement of pollution in the troposphere over Central and Western Europe 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% in the case of 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%. Results from sensitivity simulations indicate that an increase of the coarse resolution of the global models to around 1°x1° 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 global 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 those of other sensitivity runs where the horizontal resolution or European emissions are increased. 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 and CO found in most of the models during this extreme pollution event. [ABSTRACT FROM AUTHOR]

This paper presents a climatology and trends of tropospheric ozone in the Southwestern Indian Ocean (Reunion Island) and South Africa (Irene and Johannesburg). This study is based on a multi-instrumental dataset: PTU-O3 ozonesondes, DIAL LIDAR and MOZAIC airborne instrumentation. The seasonal profiles of tropospheric ozone at Reunion Island have been calculated from two different data sets: ozonesondes and LIDAR. The two climatological profiles are similar, except in austral summer when the LIDAR profiles show greater values in the free troposphere, and in the upper troposphere when the LIDAR profiles show lower values during all seasons. These results show that the climatological value of LIDAR profiles must be discussed with care since LIDAR measurements can be performed only under clear sky conditions, and the upper limit of the profile depends on the signal strength. In addition, linear trends have been calculated from ozonesonde data at Reunion and Irene. Considering the whole tropospheric column, the trend is slightly positive for Reunion, and more clearly positive for Irene. Trend calculations have also been made separating the troposphere into three layers, and separating the dataset into seasons. Results show that the positive trend for Irene is governed by the lower layer that is affected by industrial pollution and biomass burning. On the contrary, for Reunion Island, the strongest trends are observed in the upper troposphere, and in winter when stratosphere-troposphere exchange is more frequently expected. [ABSTRACT FROM AUTHOR]

Recently it was discovered that over the Middle East during summer ozone mixing ratios can reach a pronounced maximum in the middle troposphere. Here we extend the analysis to the surface and show that especially in the Persian Gulf region conditions are highly favorable for ozone air pollution. We apply the EMAC atmospheric chemistry-climate model to investigate long-distance transport and the regional formation of ozone. Further, we make use of available in situ and satellite measurements and compare these with model output. The results indicate that the region is a hot spot of photochemical smog where European Union air quality standards are violated throughout the year. Long-distance transports of air pollution from Europe and the Middle East, natural emissions and stratospheric ozone conspire to bring about relatively high background ozone mixing ratios. This provides a hotbed to strong and growing indigenous air pollution in the dry local climate, and these conditions are likely to get worse in the future. [ABSTRACT FROM AUTHOR]

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 theWAMregion 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. [ABSTRACT FROM AUTHOR]

This paper presents a climatology and trends of tropospheric ozone in the southwestern part of Indian Ocean (Reunion Island) and South Africa (Irene and Johannesburg). This study is based on a multi-instrumental dataset: PTU-O3 radiosoundings, DIAL LI-DAR, MOZAIC airborne instrumentation and Dasibi UV ground based measurements. The seasonal profiles of tropospheric ozone at Reunion Island have been calculated from two different data sets: radiosondes and LIDAR. The two climatological profiles are similar, except in austral summer when smaller values for the LIDAR profiles in the free troposphere, and in the upper troposphere for all seasons occur. These results show that the LIDAR profiles are at times not representative of the true ozone climatological value as measurements can be taken only under clear sky conditions, and the upper limit reached depends on the signal. In the lower troposphere, climatological ozone values from radiosondes have been compared to a one year campaign of ground based measurements from a Dasibi instrument located at high altitude site (2150 m) at Reunion Island. The seasonal cycle is comparable for the two datasets, with Dasibi UV values displaying slightly higher values. This suggests that if local dynamical and possibly physico-chemical effects may influence the ozone level, the seasonal cycle can be followed with ground level measurements. Average ground level concentrations measured on the summits of the island seem to be representative of the lower free troposphere ozone concentration at the same altitude (∼2000 m) whereas night time data would be representative of tropospheric concentration at a higher altitude (∼3000 m) due to the subsidence effect. Finally, linear trends have been calculated from radiosondes data at Reunion and Irene. Considering the whole tropospheric column, the trend is slightly positive for Reunion, and more clearly positive for Irene. Trend calculations have also been made separating the troposphere into three layers, and separating the dataset into seasons. Results shows that the positive trend for Irene is governed by the lower layer most probably by industrial pollution and biomass burning. On the contrary, for Reunion Island, the strongest trends are observed in the upper troposphere, and in winter when stratospheric-tropospheric exchange is more frequently expected. [ABSTRACT FROM AUTHOR]

The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric dynamics, is one of the key species provided by the primary instrument, the ACE-Fourier Transform Spectrometer (ACE-FTS). This instrument performs measurements in both the CO 1-0 and 2-0 ro-vibrational bands, from which vertically resolved CO concentration profiles are retrieved, from the mid-troposphere to the thermosphere. This paper presents an updated description of the ACE-FTS version 2.2 CO data product, along with a comprehensive validation of these profiles using available observations (February 2004 to December 2006). We have compared the CO partial columns with ground-based measurements using Fourier transform infrared spectroscopy and millimeter wave radiometry, and the volume mixing ratio profiles with airborne (both high-altitude balloon flight and airplane) observations. CO satellite observations provided by nadir-looking instruments (MOPITT and TES) as well as limb-viewing remote sensors (MIPAS, SMR and MLS) were also compared with the ACE-FTS CO products. We show that the ACE-FTS measurements provide CO profiles with small retrieval errors (better than 5% from the upper troposphere to 40 km, and better than 10% above). These observations agree well with the correlative measurements, considering the rather loose coincidence criteria in some cases. Based on the validation exercise we assess the following uncertainties to the ACE-FTS measurement data: better than 15% in the upper troposphere (8–12 km), than 30% in the lower stratosphere (12–30 km), and than 25% from 30 to 100 km. [ABSTRACT FROM AUTHOR]