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  • Open Access English
    Authors: 
    Blechschmidt, Anne-Marlene; Arteta, Joaquim; Coman, Adriana; Curier, Lyana; Eskes, Henk; Foret, Gilles; Gielen, Clio; Hendrick, Francois; Marécal, Virginie; Meleux, Frédérik; +13 more
    Project: EC | MACC-III (633080), EC | MACC II (283576), EC | NORS (284421)

    Multi-axis differential optical absorption spectroscopy (MAX-DOAS) tropospheric NO2 column retrievals from four European measurement stations are compared to simulations from five regional air quality models which contribute to the European regional ensemble forecasts and reanalyses of the operational Copernicus Atmosphere Monitoring Service (CAMS). Compared to other observational data usually applied for regional model evaluation, MAX-DOAS data are closer to the regional model data in terms of horizontal and vertical resolution, and multiple measurements are available during daylight, so that, for example, diurnal cycles of trace gases can be investigated. In general, there is good agreement between simulated and retrieved NO2 column values for individual MAX-DOAS measurements with correlations between 35 % and 70 % for individual models and 45 % to 75 % for the ensemble median for tropospheric NO2 vertical column densities (VCDs), indicating that emissions, transport and tropospheric chemistry of NOx are on average well simulated. However, large differences are found for individual pollution plumes observed by MAX-DOAS. Most of the models overestimate seasonal cycles for the majority of MAX-DOAS sites investigated. At the urban stations, weekly cycles are reproduced well, but the decrease towards the weekend is underestimated and diurnal cycles are overall not well represented. In particular, simulated morning rush hour peaks are not confirmed by MAX-DOAS retrievals, and models fail to reproduce observed changes in diurnal cycles for weekdays versus weekends. The results of this study show that future model development needs to concentrate on improving representation of diurnal cycles and associated temporal scalings.

  • Open Access English
    Authors: 
    Sourdeval, Odran; Gryspeerdt, Edward; Krämer, Martina; Goren, Tom; Delanoë, Julien; Afchine, Armin; Hemmer, Friederike; Quaas, Johannes;
    Project: EC | QUAERERE (306284), EC | MSCCC (703880)

    The number concentration of cloud particles is a key quantity for understanding aerosol–cloud interactions and describing clouds in climate and numerical weather prediction models. In contrast with recent advances for liquid clouds, few observational constraints exist regarding the ice crystal number concentration (Ni). This study investigates how combined lidar–radar measurements can be used to provide satellite estimates of Ni, using a methodology that constrains moments of a parameterized particle size distribution (PSD). The operational liDAR–raDAR (DARDAR) product serves as an existing base for this method, which focuses on ice clouds with temperatures Tc<-30 ∘C. Theoretical considerations demonstrate the capability for accurate retrievals of Ni, apart from a possible bias in the concentration in small crystals when Tc≳−50 ∘C, due to the assumption of a monomodal PSD shape in the current method. This is verified via a comparison of satellite estimates to coincident in situ measurements, which additionally demonstrates the sufficient sensitivity of lidar–radar observations to Ni. Following these results, satellite estimates of Ni are evaluated in the context of a case study and a preliminary climatological analysis based on 10 years of global data. Despite a lack of other large-scale references, this evaluation shows a reasonable physical consistency in Ni spatial distribution patterns. Notably, increases in Ni are found towards cold temperatures and, more significantly, in the presence of strong updrafts, such as those related to convective or orographic uplifts. Further evaluation and improvement of this method are necessary, although these results already constitute a first encouraging step towards large-scale observational constraints for Ni. Part 2 of this series uses this new dataset to examine the controls on Ni.

  • Open Access English
    Authors: 
    Gryspeerdt, Edward; Goren, Tom; Sourdeval, Odran; Quaas, Johannes; Mülmenstädt, Johannes; Dipu, Sudhakar; Unglaub, Claudia; Gettelman, Andrew; Christensen, Matthew;
    Project: EC | QUAERERE (306284), EC | MSCCC (703880)

    The impact of aerosols on cloud properties is one of the largest uncertainties in the anthropogenic radiative forcing of the climate. Significant progress has been made in constraining this forcing using observations, but uncertainty remains, particularly in the magnitude of cloud rapid adjustments to aerosol perturbations. Cloud liquid water path (LWP) is the leading control on liquid-cloud albedo, making it important to observationally constrain the aerosol impact on LWP. Previous modelling and observational studies have shown that multiple processes play a role in determining the LWP response to aerosol perturbations, but that the aerosol effect can be difficult to isolate. Following previous studies using mediating variables, this work investigates use of the relationship between cloud droplet number concentration (Nd) and LWP for constraining the role of aerosols. Using joint-probability histograms to account for the non-linear relationship, this work finds a relationship that is broadly consistent with previous studies. There is significant geographical variation in the relationship, partly due to role of meteorological factors (particularly relative humidity). The Nd–LWP relationship is negative in the majority of regions, suggesting that aerosol-induced LWP reductions could offset a significant fraction of the instantaneous radiative forcing from aerosol–cloud interactions (RFaci). However, variations in the Nd–LWP relationship in response to volcanic and shipping aerosol perturbations indicate that the Nd–LWP relationship overestimates the causal Nd impact on LWP due to the role of confounding factors. The weaker LWP reduction implied by these “natural experiments” means that this work provides an upper bound to the radiative forcing from aerosol-induced changes in the LWP.

  • Open Access English
    Authors: 
    Calmer, Radiance; Roberts, Gregory C.; Sanchez, Kevin J.; Sciare, Jean; Sellegri, Karine; Picard, David; Vrekoussis, Mihalis; Pikridas, Michael;
    Project: EC | BACCHUS (603445)

    In the framework of the EU-FP7 BACCHUS (impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) project, an intensive field campaign was performed in Cyprus (March 2015). Remotely piloted aircraft system (RPAS), ground-based instruments, and remote-sensing observations were operating in parallel to provide an integrated characterization of aerosol–cloud interactions. Remotely piloted aircraft (RPA) were equipped with a five-hole probe, pyranometers, pressure, temperature and humidity sensors, and measured vertical wind at cloud base and cloud optical properties of a stratocumulus layer. Ground-based measurements of dry aerosol size distributions and cloud condensation nuclei spectra, and RPA observations of updraft and meteorological state parameters are used here to initialize an aerosol–cloud parcel model (ACPM) and compare the in situ observations of cloud optical properties measured by the RPA to those simulated in the ACPM. Two different cases are studied with the ACPM, including an adiabatic case and an entrainment case, in which the in-cloud temperature profile from RPA is taken into account. Adiabatic ACPM simulation yields cloud droplet number concentrations at cloud base (approximately 400 cm−3) that are similar to those derived from a Hoppel minimum analysis. Cloud optical properties have been inferred using the transmitted fraction of shortwave radiation profile measured by downwelling and upwelling pyranometers mounted on a RPA, and the observed transmitted fraction of solar radiation is then compared to simulations from the ACPM. ACPM simulations and RPA observations shows better agreement when associated with entrainment compared to that of an adiabatic case. The mean difference between observed and adiabatic profiles of transmitted fraction of solar radiation is 0.12, while this difference is only 0.03 between observed and entrainment profiles. A sensitivity calculation is then conducted to quantify the relative impacts of 2-fold changes in aerosol concentration, and updraft to highlight the importance of accounting for the impact of entrainment in deriving cloud optical properties, as well as the ability of RPAs to leverage ground-based observations for studying aerosol–cloud interactions.

  • Open Access English
    Authors: 
    Heikenfeld, Max; White, Bethan; Labbouz, Laurent; Stier, Philip;
    Project: EC | RECAP (724602), EC | ACCLAIM (280025), EC | BACCHUS (603445)

    The impact of aerosols on ice- and mixed-phase processes in deep convective clouds remains highly uncertain, and the wide range of interacting microphysical processes is still poorly understood. To understand these processes, we analyse diagnostic output of all individual microphysical process rates for two bulk microphysics schemes in the Weather and Research Forecasting model (WRF). We investigate the response of individual processes to changes in aerosol conditions and the propagation of perturbations through the microphysics all the way to the macrophysical development of the convective clouds. We perform simulations for two different cases of idealised supercells using two double-moment bulk microphysics schemes and a bin microphysics scheme. The simulations cover a comprehensive range of values for cloud droplet number concentration (CDNC) and cloud condensation nuclei (CCN) concentration as a proxy for aerosol effects on convective clouds. We have developed a new cloud tracking algorithm to analyse the morphology and time evolution of individually tracked convective cells in the simulations and their response to the aerosol perturbations. This analysis confirms an expected decrease in warm rain formation processes due to autoconversion and accretion for more polluted conditions. There is no evidence of a significant increase in the total amount of latent heat, as changes to the individual components of the integrated latent heating in the cloud compensate each other. The latent heating from freezing and riming processes is shifted to a higher altitude in the cloud, but there is no significant change to the integrated latent heat from freezing. Different choices in the treatment of deposition and sublimation processes between the microphysics schemes lead to strong differences including feedbacks onto condensation and evaporation. These changes in the microphysical processes explain some of the response in cloud mass and the altitude of the cloud centre of gravity. However, there remain some contrasts in the development of the bulk cloud parameters between the microphysics schemes and the two simulated cases.

  • Open Access English
    Authors: 
    Haslett, Sophie L.; Taylor, Jonathan W.; Evans, Mathew; Morris, Eleanor; Vogel, Bernhard; Dajuma, Alima; Brito, Joel; Batenburg, Anneke M.; Borrmann, Stephan; Schneider, Johannes; +11 more
    Project: EC | DACCIWA (603502), UKRI | Training the next generat... (NE/L002469/1)

    Vast stretches of agricultural land in southern and central Africa are burnt between June and September each year, which releases large quantities of aerosol into the atmosphere. The resulting smoke plumes are carried west over the Atlantic Ocean at altitudes between 2 and 4 km. As only limited observational data in West Africa have existed until now, whether this pollution has an impact at lower altitudes has remained unclear. The Dynamics-aerosol-chemistry-cloud interactions in West Africa (DACCIWA) aircraft campaign took place in southern West Africa during June and July 2016, with the aim of observing gas and aerosol properties in the region in order to assess anthropogenic and other influences on the atmosphere. Results presented here show that a significant mass of aged accumulation mode aerosol was present in the southern West African monsoon layer, over both the ocean and the continent. A median dry aerosol concentration of 6.2 µg m−3 (standard temperature and pressure, STP) was observed over the Atlantic Ocean upwind of the major cities, with an interquartile range from 5.3 to 8.0 µg m−3. This concentration increased to a median of 11.1 µg m−3 (8.6 to 15.7 µg m−3) in the immediate outflow from cities. In the continental air mass away from the cities, the median aerosol loading was 7.5 µg m−3 (5.9 to 10.5 µg m−3). The accumulation mode aerosol population over land displayed similar chemical properties to the upstream population, which implies that upstream aerosol is a significant source of aerosol pollution over the continent. The upstream aerosol is found to have most likely originated from central and southern African biomass burning. This demonstrates that biomass burning plumes are being advected northwards, after being entrained into the monsoon layer over the eastern tropical Atlantic Ocean. It is shown observationally for the first time that they contribute up to 80 % to the regional aerosol loading in the monsoon layer over southern West Africa. Results from the COSMO-ART (Consortium for Small-scale Modeling – Aerosol and Reactive Trace gases) and GEOS-Chem models support this conclusion, showing that observed aerosol concentrations over the northern Atlantic Ocean can only be reproduced when the contribution of transported biomass burning aerosol is taken into account. As a result, the large and growing emissions from the coastal cities are overlaid on an already substantial aerosol background. Simulations using COSMO-ART show that cloud droplet number concentrations can increase by up to 27 % as a result of transported biomass burning aerosol. On a regional scale this renders cloud properties and precipitation less sensitive to future increases in anthropogenic emissions. In addition, such high background loadings will lead to greater pollution exposure for the large and growing population in southern West Africa. These results emphasise the importance of including aerosol from across country borders in the development of air pollution policies and interventions in regions such as West Africa.

  • Open Access English
    Authors: 
    Benedetti, Angela; Giuseppe, Francesca; Jones, Luke; Peuch, Vincent-Henri; Rémy, Samuel; Zhang, Xiaoye;
    Project: EC | PANDA (606719)

    Asian dust is a seasonal meteorological phenomenon which affects east Asia, and has severe consequences on the air quality of China, North and South Korea and Japan. Despite the continental extent, the prediction of severe episodes and the anticipation of their consequences is challenging. Three 1-year experiments were run to assess the skill of the model of the European Centre for Medium-Range Weather Forecasts (ECMWF) in monitoring Asian dust and understand its relative contribution to the aerosol load over China. Data used were the Moderate Resolution Imaging Spectroradiometer (MODIS) Dark Target and the Deep Blue aerosol optical depth (AOD). In particular the experiments aimed at understanding the added value of data assimilation runs over a model run without any aerosol data. The year 2013 was chosen as representative of the availability of independent AOD data from two established ground-based networks (AERONET, Aerosol Robotic Network, and CARSNET, China Aerosol Remote Sensing Network), which could be used to evaluate experiments. Particulate matter (PM) data from the China Environmental Protection Agency were also used in the evaluation. Results show that the assimilation of satellite AOD data is beneficial to predict the extent and magnitude of desert dust events and to improve the short-range forecast of such events. The availability of observations from the MODIS Deep Blue algorithm over bright surfaces is an asset, allowing for a better localization of the sources and definition of the dust events. In general both experiments constrained by data assimilation perform better than the unconstrained experiment, generally showing smaller normalized mean bias and fractional gross error with respect to the independent verification datasets. The impact of the assimilated satellite observations is larger at analysis time, but lasts into the forecast up to 48 h. The performance of the global model in terms of particulate matter does not show the same degree of skill as the performance in terms of optical depth. Despite this, the global model is able to capture some regional pollution patterns. This indicates that the global model analyses may be used as boundary conditions for regional air quality models at higher resolution, enhancing their performance in situations in which part of the pollution may have originated from large-scale mechanisms. While assimilation is not a substitute for model development and characterization of the emission sources, results indicate that it can play a role in delivering improved monitoring of Asian dust optical depth.

  • Open Access English
    Authors: 
    Babić, Karmen; Adler, Bianca; Kalthoff, Norbert; Andersen, Hendrik; Dione, Cheikh; Lohou, Fabienne; Lothon, Marie; Pedruzo-Bagazgoitia, Xabier;
    Project: EC | DACCIWA (603502)

    This study presents the first detailed observational analysis of the complete diurnal cycle of stratiform low-level clouds (LLC) and involved atmospheric processes over southern West Africa (SWA). The data used here were collected during the comprehensive DACCIWA (Dynamics-Aerosol-Chemistry-Cloud-Interactions in West Africa) ground-based campaign, which aimed at monitoring LLC characteristics and capturing the wide range of atmospheric conditions related to the West African monsoon flow. In this study, in situ and remote sensing measurements from the supersite near Savè (Benin) collected during a typical day, which is characterized by the onset of a nocturnal low-level jet (NLLJ) and the formation of LLC, are analyzed. The associated dynamic and thermodynamic conditions allow the identification of five different phases related to the LLC diurnal cycle: the stable, jet, stratus I, stratus II, and convective phases. The analysis of relative humidity tendency shows that cooling is a dominant process for LLC formation, which leads to a continuous increase in relative humidity at a maximum rate of 6 % h−1, until finally saturation is reached and LLC form with a cloud-base height near the height of NLLJ maximum. Results of heat budget analysis illustrate that horizontal cold-air advection, related to the maritime inflow, which brings the cool maritime air mass and a prominent NLLJ wind profile, has the dominant role in the observed strong cooling of −1.2 K h−1 during the jet phase. The contribution from horizontal cold advection is quantified to be up to 68 %, while radiative cooling and sensible heat flux divergence both contribute 16 % to the observed heat budget below the NLLJ maximum. After the LLC form (stratus phases I and II), turbulent mixing is an important factor leading to the cooling below the cloud base, while strong radiative cooling at the cloud top helps to maintain thick stratus.

  • Open Access English
    Authors: 
    Taylor, Jonathan W.; Haslett, Sophie L.; Bower, Keith; Flynn, Michael; Crawford, Ian; Dorsey, James; Choularton, Tom; Connolly, Paul J.; Hahn, Valerian; Voigt, Christiane; +15 more
    Project: EC | DACCIWA (603502), EC | BACCHUS (603445)

    Low-level clouds (LLC) cover a wide area of southern West Africa (SWA) during the summer monsoon months, and have an important cooling effect on the regional climate. Previous studies of these clouds have focused on modelling and remote sensing via satellite. We present the first comprehensive set of regional, in situ measurements of cloud microphysics, taken during June – July 2016, as part of the DACCIWA (Dynamics-Aerosol-Chemistry-Clouds Interactions in West Africa) campaign, assessing spatial and temporal variation in the properties of these clouds. LLC developed overnight and mean cloud cover peaked a few hundred kilometres inland around 10:00 local solar time (LST), before clouds began to dissipate and convection intensified in the afternoon. Additional sea breeze clouds developed near the coast in the late morning, reaching a maximum extent around 12:00 LST. Regional variation in LLC cover was largely determined by the modulation of the cool maritime inflow by the local orography, with peaks on the upwind side of hills and minima on the leeward sides. In the broad-scale cloud field, no lasting impacts related to anthropogenic aerosol were observed downwind of major population centres. The boundary layer cloud drop number concentration (CDNC) was locally variable inland, ranging from 200 to 840 cm−3 (10th and 90th percentiles at standard temperature and pressure), but showed no systematic regional variations. Enhancements were seen in pollution plumes from the coastal cities, but were not statistically significant across the region. The majority of accumulation mode aerosols, and therefore cloud condensation nuclei, were from ubiquitous biomass burning smoke transported from the southern hemisphere. Consequently, all clouds measured (inland and offshore) had significantly higher CDNC and lower effective radius than clouds over the remote south Atlantic from literature. A parcel model sensitivity analysis showed that doubling or halving local emissions only changed the calculated CDNC by 13–22 %, as the high background meant local emissions were a small fraction of total aerosol. As the population of SWA grows, local emissions are expected to rise. Biomass burning smoke transported from the southern hemisphere is likely to dampen any effect of these increased local emissions on cloud-aerosol interactions. An integrative analysis between local pollution and Central African biomass burning emissions must be considered when predicting anthropogenic impacts on the regional cloud field during the West African monsoon.

  • Open Access English
    Authors: 
    Flamant, Cyrille; Deroubaix, Adrien; Chazette, Patrick; Brito, Joel; Gaetani, Marco; Knippertz, Peter; Fink, Andreas H.; Coetlogon, Gaëlle; Menut, Laurent; Colomb, Aurélie; +10 more
    Project: EC | DACCIWA (603502)

    The complex vertical distribution of aerosols over coastal southern West Africa (SWA) is investigated using airborne observations and numerical simulations. Observations were gathered on 2 July 2016 offshore of Ghana and Togo, during the field phase of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa project. This was the only flight conducted over the ocean during which a downward-looking lidar was operational. The aerosol loading in the lower troposphere includes emissions from coastal cities (Accra, Lomé, Cotonou, and Lagos) as well as biomass burning aerosol and dust associated with long-range transport from central Africa and the Sahara, respectively. Our results indicate that the aerosol distribution on this day is impacted by subsidence associated with zonal and meridional regional-scale overturning circulations associated with the land–sea surface temperature contrast and orography over Ghana and Togo, as typically observed on hot, cloud-free summer days such as 2 July 2016. Furthermore, we show that the zonal circulation evidenced on 2 July is a persistent feature over the Gulf of Guinea during July 2016. Numerical tracer release experiments highlight the dominance of aged emissions from Accra on the observed pollution plume loadings over the ocean, in the area of aircraft operation. The contribution of aged emission from Lomé and Cotonou is also evident above the marine boundary layer. Given the general direction of the monsoon flow, the tracer experiments indicate no contribution from Lagos emissions to the atmospheric composition of the area west of Cotonou, where our airborne observations were gathered. The tracer plume does not extend very far south over the ocean (i.e. less than 100 km from Accra), mostly because emissions are transported northeastward near the surface over land and westward above the marine atmospheric boundary layer. The latter is possible due to interactions between the monsoon flow, complex terrain, and land–sea breeze systems, which support the vertical mixing of the urban pollution. This work sheds light on the complex – and to date undocumented – mechanisms by which coastal shallow circulations can distribute atmospheric pollutants over the densely populated SWA region.

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23 Research products, page 1 of 3
  • Open Access English
    Authors: 
    Blechschmidt, Anne-Marlene; Arteta, Joaquim; Coman, Adriana; Curier, Lyana; Eskes, Henk; Foret, Gilles; Gielen, Clio; Hendrick, Francois; Marécal, Virginie; Meleux, Frédérik; +13 more
    Project: EC | MACC-III (633080), EC | MACC II (283576), EC | NORS (284421)

    Multi-axis differential optical absorption spectroscopy (MAX-DOAS) tropospheric NO2 column retrievals from four European measurement stations are compared to simulations from five regional air quality models which contribute to the European regional ensemble forecasts and reanalyses of the operational Copernicus Atmosphere Monitoring Service (CAMS). Compared to other observational data usually applied for regional model evaluation, MAX-DOAS data are closer to the regional model data in terms of horizontal and vertical resolution, and multiple measurements are available during daylight, so that, for example, diurnal cycles of trace gases can be investigated. In general, there is good agreement between simulated and retrieved NO2 column values for individual MAX-DOAS measurements with correlations between 35 % and 70 % for individual models and 45 % to 75 % for the ensemble median for tropospheric NO2 vertical column densities (VCDs), indicating that emissions, transport and tropospheric chemistry of NOx are on average well simulated. However, large differences are found for individual pollution plumes observed by MAX-DOAS. Most of the models overestimate seasonal cycles for the majority of MAX-DOAS sites investigated. At the urban stations, weekly cycles are reproduced well, but the decrease towards the weekend is underestimated and diurnal cycles are overall not well represented. In particular, simulated morning rush hour peaks are not confirmed by MAX-DOAS retrievals, and models fail to reproduce observed changes in diurnal cycles for weekdays versus weekends. The results of this study show that future model development needs to concentrate on improving representation of diurnal cycles and associated temporal scalings.

  • Open Access English
    Authors: 
    Sourdeval, Odran; Gryspeerdt, Edward; Krämer, Martina; Goren, Tom; Delanoë, Julien; Afchine, Armin; Hemmer, Friederike; Quaas, Johannes;
    Project: EC | QUAERERE (306284), EC | MSCCC (703880)

    The number concentration of cloud particles is a key quantity for understanding aerosol–cloud interactions and describing clouds in climate and numerical weather prediction models. In contrast with recent advances for liquid clouds, few observational constraints exist regarding the ice crystal number concentration (Ni). This study investigates how combined lidar–radar measurements can be used to provide satellite estimates of Ni, using a methodology that constrains moments of a parameterized particle size distribution (PSD). The operational liDAR–raDAR (DARDAR) product serves as an existing base for this method, which focuses on ice clouds with temperatures Tc<-30 ∘C. Theoretical considerations demonstrate the capability for accurate retrievals of Ni, apart from a possible bias in the concentration in small crystals when Tc≳−50 ∘C, due to the assumption of a monomodal PSD shape in the current method. This is verified via a comparison of satellite estimates to coincident in situ measurements, which additionally demonstrates the sufficient sensitivity of lidar–radar observations to Ni. Following these results, satellite estimates of Ni are evaluated in the context of a case study and a preliminary climatological analysis based on 10 years of global data. Despite a lack of other large-scale references, this evaluation shows a reasonable physical consistency in Ni spatial distribution patterns. Notably, increases in Ni are found towards cold temperatures and, more significantly, in the presence of strong updrafts, such as those related to convective or orographic uplifts. Further evaluation and improvement of this method are necessary, although these results already constitute a first encouraging step towards large-scale observational constraints for Ni. Part 2 of this series uses this new dataset to examine the controls on Ni.

  • Open Access English
    Authors: 
    Gryspeerdt, Edward; Goren, Tom; Sourdeval, Odran; Quaas, Johannes; Mülmenstädt, Johannes; Dipu, Sudhakar; Unglaub, Claudia; Gettelman, Andrew; Christensen, Matthew;
    Project: EC | QUAERERE (306284), EC | MSCCC (703880)

    The impact of aerosols on cloud properties is one of the largest uncertainties in the anthropogenic radiative forcing of the climate. Significant progress has been made in constraining this forcing using observations, but uncertainty remains, particularly in the magnitude of cloud rapid adjustments to aerosol perturbations. Cloud liquid water path (LWP) is the leading control on liquid-cloud albedo, making it important to observationally constrain the aerosol impact on LWP. Previous modelling and observational studies have shown that multiple processes play a role in determining the LWP response to aerosol perturbations, but that the aerosol effect can be difficult to isolate. Following previous studies using mediating variables, this work investigates use of the relationship between cloud droplet number concentration (Nd) and LWP for constraining the role of aerosols. Using joint-probability histograms to account for the non-linear relationship, this work finds a relationship that is broadly consistent with previous studies. There is significant geographical variation in the relationship, partly due to role of meteorological factors (particularly relative humidity). The Nd–LWP relationship is negative in the majority of regions, suggesting that aerosol-induced LWP reductions could offset a significant fraction of the instantaneous radiative forcing from aerosol–cloud interactions (RFaci). However, variations in the Nd–LWP relationship in response to volcanic and shipping aerosol perturbations indicate that the Nd–LWP relationship overestimates the causal Nd impact on LWP due to the role of confounding factors. The weaker LWP reduction implied by these “natural experiments” means that this work provides an upper bound to the radiative forcing from aerosol-induced changes in the LWP.

  • Open Access English
    Authors: 
    Calmer, Radiance; Roberts, Gregory C.; Sanchez, Kevin J.; Sciare, Jean; Sellegri, Karine; Picard, David; Vrekoussis, Mihalis; Pikridas, Michael;
    Project: EC | BACCHUS (603445)

    In the framework of the EU-FP7 BACCHUS (impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) project, an intensive field campaign was performed in Cyprus (March 2015). Remotely piloted aircraft system (RPAS), ground-based instruments, and remote-sensing observations were operating in parallel to provide an integrated characterization of aerosol–cloud interactions. Remotely piloted aircraft (RPA) were equipped with a five-hole probe, pyranometers, pressure, temperature and humidity sensors, and measured vertical wind at cloud base and cloud optical properties of a stratocumulus layer. Ground-based measurements of dry aerosol size distributions and cloud condensation nuclei spectra, and RPA observations of updraft and meteorological state parameters are used here to initialize an aerosol–cloud parcel model (ACPM) and compare the in situ observations of cloud optical properties measured by the RPA to those simulated in the ACPM. Two different cases are studied with the ACPM, including an adiabatic case and an entrainment case, in which the in-cloud temperature profile from RPA is taken into account. Adiabatic ACPM simulation yields cloud droplet number concentrations at cloud base (approximately 400 cm−3) that are similar to those derived from a Hoppel minimum analysis. Cloud optical properties have been inferred using the transmitted fraction of shortwave radiation profile measured by downwelling and upwelling pyranometers mounted on a RPA, and the observed transmitted fraction of solar radiation is then compared to simulations from the ACPM. ACPM simulations and RPA observations shows better agreement when associated with entrainment compared to that of an adiabatic case. The mean difference between observed and adiabatic profiles of transmitted fraction of solar radiation is 0.12, while this difference is only 0.03 between observed and entrainment profiles. A sensitivity calculation is then conducted to quantify the relative impacts of 2-fold changes in aerosol concentration, and updraft to highlight the importance of accounting for the impact of entrainment in deriving cloud optical properties, as well as the ability of RPAs to leverage ground-based observations for studying aerosol–cloud interactions.

  • Open Access English
    Authors: 
    Heikenfeld, Max; White, Bethan; Labbouz, Laurent; Stier, Philip;
    Project: EC | RECAP (724602), EC | ACCLAIM (280025), EC | BACCHUS (603445)

    The impact of aerosols on ice- and mixed-phase processes in deep convective clouds remains highly uncertain, and the wide range of interacting microphysical processes is still poorly understood. To understand these processes, we analyse diagnostic output of all individual microphysical process rates for two bulk microphysics schemes in the Weather and Research Forecasting model (WRF). We investigate the response of individual processes to changes in aerosol conditions and the propagation of perturbations through the microphysics all the way to the macrophysical development of the convective clouds. We perform simulations for two different cases of idealised supercells using two double-moment bulk microphysics schemes and a bin microphysics scheme. The simulations cover a comprehensive range of values for cloud droplet number concentration (CDNC) and cloud condensation nuclei (CCN) concentration as a proxy for aerosol effects on convective clouds. We have developed a new cloud tracking algorithm to analyse the morphology and time evolution of individually tracked convective cells in the simulations and their response to the aerosol perturbations. This analysis confirms an expected decrease in warm rain formation processes due to autoconversion and accretion for more polluted conditions. There is no evidence of a significant increase in the total amount of latent heat, as changes to the individual components of the integrated latent heating in the cloud compensate each other. The latent heating from freezing and riming processes is shifted to a higher altitude in the cloud, but there is no significant change to the integrated latent heat from freezing. Different choices in the treatment of deposition and sublimation processes between the microphysics schemes lead to strong differences including feedbacks onto condensation and evaporation. These changes in the microphysical processes explain some of the response in cloud mass and the altitude of the cloud centre of gravity. However, there remain some contrasts in the development of the bulk cloud parameters between the microphysics schemes and the two simulated cases.

  • Open Access English
    Authors: 
    Haslett, Sophie L.; Taylor, Jonathan W.; Evans, Mathew; Morris, Eleanor; Vogel, Bernhard; Dajuma, Alima; Brito, Joel; Batenburg, Anneke M.; Borrmann, Stephan; Schneider, Johannes; +11 more
    Project: EC | DACCIWA (603502), UKRI | Training the next generat... (NE/L002469/1)

    Vast stretches of agricultural land in southern and central Africa are burnt between June and September each year, which releases large quantities of aerosol into the atmosphere. The resulting smoke plumes are carried west over the Atlantic Ocean at altitudes between 2 and 4 km. As only limited observational data in West Africa have existed until now, whether this pollution has an impact at lower altitudes has remained unclear. The Dynamics-aerosol-chemistry-cloud interactions in West Africa (DACCIWA) aircraft campaign took place in southern West Africa during June and July 2016, with the aim of observing gas and aerosol properties in the region in order to assess anthropogenic and other influences on the atmosphere. Results presented here show that a significant mass of aged accumulation mode aerosol was present in the southern West African monsoon layer, over both the ocean and the continent. A median dry aerosol concentration of 6.2 µg m−3 (standard temperature and pressure, STP) was observed over the Atlantic Ocean upwind of the major cities, with an interquartile range from 5.3 to 8.0 µg m−3. This concentration increased to a median of 11.1 µg m−3 (8.6 to 15.7 µg m−3) in the immediate outflow from cities. In the continental air mass away from the cities, the median aerosol loading was 7.5 µg m−3 (5.9 to 10.5 µg m−3). The accumulation mode aerosol population over land displayed similar chemical properties to the upstream population, which implies that upstream aerosol is a significant source of aerosol pollution over the continent. The upstream aerosol is found to have most likely originated from central and southern African biomass burning. This demonstrates that biomass burning plumes are being advected northwards, after being entrained into the monsoon layer over the eastern tropical Atlantic Ocean. It is shown observationally for the first time that they contribute up to 80 % to the regional aerosol loading in the monsoon layer over southern West Africa. Results from the COSMO-ART (Consortium for Small-scale Modeling – Aerosol and Reactive Trace gases) and GEOS-Chem models support this conclusion, showing that observed aerosol concentrations over the northern Atlantic Ocean can only be reproduced when the contribution of transported biomass burning aerosol is taken into account. As a result, the large and growing emissions from the coastal cities are overlaid on an already substantial aerosol background. Simulations using COSMO-ART show that cloud droplet number concentrations can increase by up to 27 % as a result of transported biomass burning aerosol. On a regional scale this renders cloud properties and precipitation less sensitive to future increases in anthropogenic emissions. In addition, such high background loadings will lead to greater pollution exposure for the large and growing population in southern West Africa. These results emphasise the importance of including aerosol from across country borders in the development of air pollution policies and interventions in regions such as West Africa.

  • Open Access English
    Authors: 
    Benedetti, Angela; Giuseppe, Francesca; Jones, Luke; Peuch, Vincent-Henri; Rémy, Samuel; Zhang, Xiaoye;
    Project: EC | PANDA (606719)

    Asian dust is a seasonal meteorological phenomenon which affects east Asia, and has severe consequences on the air quality of China, North and South Korea and Japan. Despite the continental extent, the prediction of severe episodes and the anticipation of their consequences is challenging. Three 1-year experiments were run to assess the skill of the model of the European Centre for Medium-Range Weather Forecasts (ECMWF) in monitoring Asian dust and understand its relative contribution to the aerosol load over China. Data used were the Moderate Resolution Imaging Spectroradiometer (MODIS) Dark Target and the Deep Blue aerosol optical depth (AOD). In particular the experiments aimed at understanding the added value of data assimilation runs over a model run without any aerosol data. The year 2013 was chosen as representative of the availability of independent AOD data from two established ground-based networks (AERONET, Aerosol Robotic Network, and CARSNET, China Aerosol Remote Sensing Network), which could be used to evaluate experiments. Particulate matter (PM) data from the China Environmental Protection Agency were also used in the evaluation. Results show that the assimilation of satellite AOD data is beneficial to predict the extent and magnitude of desert dust events and to improve the short-range forecast of such events. The availability of observations from the MODIS Deep Blue algorithm over bright surfaces is an asset, allowing for a better localization of the sources and definition of the dust events. In general both experiments constrained by data assimilation perform better than the unconstrained experiment, generally showing smaller normalized mean bias and fractional gross error with respect to the independent verification datasets. The impact of the assimilated satellite observations is larger at analysis time, but lasts into the forecast up to 48 h. The performance of the global model in terms of particulate matter does not show the same degree of skill as the performance in terms of optical depth. Despite this, the global model is able to capture some regional pollution patterns. This indicates that the global model analyses may be used as boundary conditions for regional air quality models at higher resolution, enhancing their performance in situations in which part of the pollution may have originated from large-scale mechanisms. While assimilation is not a substitute for model development and characterization of the emission sources, results indicate that it can play a role in delivering improved monitoring of Asian dust optical depth.

  • Open Access English
    Authors: 
    Babić, Karmen; Adler, Bianca; Kalthoff, Norbert; Andersen, Hendrik; Dione, Cheikh; Lohou, Fabienne; Lothon, Marie; Pedruzo-Bagazgoitia, Xabier;
    Project: EC | DACCIWA (603502)

    This study presents the first detailed observational analysis of the complete diurnal cycle of stratiform low-level clouds (LLC) and involved atmospheric processes over southern West Africa (SWA). The data used here were collected during the comprehensive DACCIWA (Dynamics-Aerosol-Chemistry-Cloud-Interactions in West Africa) ground-based campaign, which aimed at monitoring LLC characteristics and capturing the wide range of atmospheric conditions related to the West African monsoon flow. In this study, in situ and remote sensing measurements from the supersite near Savè (Benin) collected during a typical day, which is characterized by the onset of a nocturnal low-level jet (NLLJ) and the formation of LLC, are analyzed. The associated dynamic and thermodynamic conditions allow the identification of five different phases related to the LLC diurnal cycle: the stable, jet, stratus I, stratus II, and convective phases. The analysis of relative humidity tendency shows that cooling is a dominant process for LLC formation, which leads to a continuous increase in relative humidity at a maximum rate of 6 % h−1, until finally saturation is reached and LLC form with a cloud-base height near the height of NLLJ maximum. Results of heat budget analysis illustrate that horizontal cold-air advection, related to the maritime inflow, which brings the cool maritime air mass and a prominent NLLJ wind profile, has the dominant role in the observed strong cooling of −1.2 K h−1 during the jet phase. The contribution from horizontal cold advection is quantified to be up to 68 %, while radiative cooling and sensible heat flux divergence both contribute 16 % to the observed heat budget below the NLLJ maximum. After the LLC form (stratus phases I and II), turbulent mixing is an important factor leading to the cooling below the cloud base, while strong radiative cooling at the cloud top helps to maintain thick stratus.

  • Open Access English
    Authors: 
    Taylor, Jonathan W.; Haslett, Sophie L.; Bower, Keith; Flynn, Michael; Crawford, Ian; Dorsey, James; Choularton, Tom; Connolly, Paul J.; Hahn, Valerian; Voigt, Christiane; +15 more
    Project: EC | DACCIWA (603502), EC | BACCHUS (603445)

    Low-level clouds (LLC) cover a wide area of southern West Africa (SWA) during the summer monsoon months, and have an important cooling effect on the regional climate. Previous studies of these clouds have focused on modelling and remote sensing via satellite. We present the first comprehensive set of regional, in situ measurements of cloud microphysics, taken during June – July 2016, as part of the DACCIWA (Dynamics-Aerosol-Chemistry-Clouds Interactions in West Africa) campaign, assessing spatial and temporal variation in the properties of these clouds. LLC developed overnight and mean cloud cover peaked a few hundred kilometres inland around 10:00 local solar time (LST), before clouds began to dissipate and convection intensified in the afternoon. Additional sea breeze clouds developed near the coast in the late morning, reaching a maximum extent around 12:00 LST. Regional variation in LLC cover was largely determined by the modulation of the cool maritime inflow by the local orography, with peaks on the upwind side of hills and minima on the leeward sides. In the broad-scale cloud field, no lasting impacts related to anthropogenic aerosol were observed downwind of major population centres. The boundary layer cloud drop number concentration (CDNC) was locally variable inland, ranging from 200 to 840 cm−3 (10th and 90th percentiles at standard temperature and pressure), but showed no systematic regional variations. Enhancements were seen in pollution plumes from the coastal cities, but were not statistically significant across the region. The majority of accumulation mode aerosols, and therefore cloud condensation nuclei, were from ubiquitous biomass burning smoke transported from the southern hemisphere. Consequently, all clouds measured (inland and offshore) had significantly higher CDNC and lower effective radius than clouds over the remote south Atlantic from literature. A parcel model sensitivity analysis showed that doubling or halving local emissions only changed the calculated CDNC by 13–22 %, as the high background meant local emissions were a small fraction of total aerosol. As the population of SWA grows, local emissions are expected to rise. Biomass burning smoke transported from the southern hemisphere is likely to dampen any effect of these increased local emissions on cloud-aerosol interactions. An integrative analysis between local pollution and Central African biomass burning emissions must be considered when predicting anthropogenic impacts on the regional cloud field during the West African monsoon.

  • Open Access English
    Authors: 
    Flamant, Cyrille; Deroubaix, Adrien; Chazette, Patrick; Brito, Joel; Gaetani, Marco; Knippertz, Peter; Fink, Andreas H.; Coetlogon, Gaëlle; Menut, Laurent; Colomb, Aurélie; +10 more
    Project: EC | DACCIWA (603502)

    The complex vertical distribution of aerosols over coastal southern West Africa (SWA) is investigated using airborne observations and numerical simulations. Observations were gathered on 2 July 2016 offshore of Ghana and Togo, during the field phase of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa project. This was the only flight conducted over the ocean during which a downward-looking lidar was operational. The aerosol loading in the lower troposphere includes emissions from coastal cities (Accra, Lomé, Cotonou, and Lagos) as well as biomass burning aerosol and dust associated with long-range transport from central Africa and the Sahara, respectively. Our results indicate that the aerosol distribution on this day is impacted by subsidence associated with zonal and meridional regional-scale overturning circulations associated with the land–sea surface temperature contrast and orography over Ghana and Togo, as typically observed on hot, cloud-free summer days such as 2 July 2016. Furthermore, we show that the zonal circulation evidenced on 2 July is a persistent feature over the Gulf of Guinea during July 2016. Numerical tracer release experiments highlight the dominance of aged emissions from Accra on the observed pollution plume loadings over the ocean, in the area of aircraft operation. The contribution of aged emission from Lomé and Cotonou is also evident above the marine boundary layer. Given the general direction of the monsoon flow, the tracer experiments indicate no contribution from Lagos emissions to the atmospheric composition of the area west of Cotonou, where our airborne observations were gathered. The tracer plume does not extend very far south over the ocean (i.e. less than 100 km from Accra), mostly because emissions are transported northeastward near the surface over land and westward above the marine atmospheric boundary layer. The latter is possible due to interactions between the monsoon flow, complex terrain, and land–sea breeze systems, which support the vertical mixing of the urban pollution. This work sheds light on the complex – and to date undocumented – mechanisms by which coastal shallow circulations can distribute atmospheric pollutants over the densely populated SWA region.

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