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The Aerosol, Radiation and Clouds in southern Africa (AEROCLO-sA) project investigates the role of aerosols on the regional climate of southern Africa. This is a unique environment where natural and anthropogenic aerosols and a semipermanent and widespread stratocumulus (Sc) cloud deck are found. The project aims to understand the dynamical, chemical, and radiative processes involved in aerosol–cloud–radiation interactions over land and ocean and under various meteorological conditions. The AEROCLO-sA field campaign was conducted in August and September of 2017 over Namibia. An aircraft equipped with active and passive remote sensors and aerosol in situ probes performed a total of 30 research flight hours. In parallel, a ground-based mobile station with state-of-the-art in situ aerosol probes and remote sensing instrumentation was implemented over coastal Namibia, and complemented by ground-based and balloonborne observations of the dynamical, thermodynamical, and physical properties of the lower troposphere. The focus laid on mineral dust emitted from salty pans and ephemeral riverbeds in northern Namibia, the advection of biomass-burning aerosol plumes from Angola subsequently transported over the Atlantic Ocean, and aerosols in the marine boundary layer at the ocean–atmosphere interface. This article presents an overview of the AEROCLO-sA field campaign with results from the airborne and surface measurements. These observations provide new knowledge of the interactions of aerosols and radiation in cloudy and clear skies in connection with the atmospheric dynamics over southern Africa. They will foster new advanced climate simulations and enhance the capability of spaceborne sensors, ultimately allowing a better prediction of future climate and weather in southern Africa

This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240 m a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz–El Alto, located approximately 20 km away and 1.5 km below the sampling site. The extended multi-year record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96 Mm−1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68 Mm−1 respectively) and higher values during the dry season (0.80, 11.23, and 14.51 Mm−1 respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz–El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28 % to 80 % increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere.

We analyse the airborne measurements of above-cloud aerosols from the AErosol, RadiatiOn, and CLOuds in southern Africa (AEROCLO-sA) field campaign performed in Namibia during August and September 2017. The study aims to retrieve the aerosol above-cloud direct radiative effect (DRE) with well-defined uncertainties. To improve the retrieval of the aerosol and cloud properties, the airborne demonstrator of the Multi-Viewing, Multi-Channel, Multi-Polarization (3MI) satellite instrument, called the Observing System Including PolaRisation in the Solar Infrared Spectrum (OSIRIS), was deployed on-board the SAFIRE (Service des Avions Français Instrumentés pour la Rechercheen Environnement) Falcon 20 aircraft during 10 flights performed over land, over the ocean, and along the Namibian coast. The airborne instrument OSIRIS provides observations at high temporal and spatial resolutions for aerosol above clouds (AACs) and cloud properties. OSIRIS was supplemented with the Photomètre Léger Aéroporté pour la surveillance des Masses d'Air version 2 (PLASMA2). The combined airborne measurements allow, for the first time, the validation of AAC algorithms previously developed for satellite measurements. The variations in the aerosol properties are consistent with the different atmospheric circulation regimes observed during the deployment. Airborne observations typically show strong aerosol optical depth (AOD; up to 1.2 at 550 nm) of fine-mode particles from biomass burning (extinction Ångström exponent varying between 1.6 and 2.2), transported above bright stratocumulus decks (mean cloud top around 1 km above mean sea level), with cloud optical thickness (COT) up to 35 at 550 nm. The above-cloud visible AOD retrieved with OSIRIS agrees within 10 % of the PLASMA2 sun photometer measurements in the same environment. The single scattering albedo (SSA) is one of the most influential parameters on the AAC DRE calculation that remains largely uncertain in models. During the AEROCLO-sA campaign, the average SSA obtained by OSIRIS at 550 nm is 0.87, which is in agreement within 3 %, on average, with previous polarimetric-based satellite and airborne retrievals. The strong absorption of the biomass burning plumes in the visible range is generally consistent with the observations from the Aerosol Robotic Network (AERONET) ground-based sun photometers. This, however, shows a significant increase in the particles' absorption at 440 nm in northern Namibia and Angola, which indicates more absorbing organic species within the observed smoke plumes. Biomass burning aerosols are also vertically collocated, with significant amounts of water content up to the top of the plume at around 6 km height in our measurements. The detailed characterization of aerosol and cloud properties, water vapour, and their uncertainties obtained from OSIRIS and PLASMA2 measurements allows us to study their impacts on the AAC DRE. The high-absorbing load of AAC, combined with high cloud albedo, leads to unprecedented DRE estimates, which are higher than previous satellite-based estimates. The average AAC DRE calculated from the airborne measurements in the visible range is +85 W m−2 (standard deviation of 26 W m−2), with instantaneous values up to +190 W m−2 during intense events. These high DRE values, associated with their uncertainties, have to be considered as new upper cases in order to evaluate the ability of models to reproduce the radiative impact of the aerosols over the southeastern Atlantic region.

Air traffic affects cloudiness, and thus climate, by emitting exhaust gases and particles. The study of the evolution of contrail properties is very challenging due to the complex interplay of vortex dynamics and the atmospheric environment (e.g. temperature, supersaturation). Despite substantial progress in recent years, the optical, microphysical, and macrophysical properties of contrails and ambient cirrus during contrail formation and subsequent ageing are still subject to large uncertainties due to instrumental and observational limitations and the large number of variables influencing the contrail life cycle. In this study, various contrail cases corresponding to different aircraft types and atmospheric conditions are investigated using a statistical method based on the in situ optical measurements performed during the Contrail and Cirrus Experiments (CONCERT) campaigns 2008 and 2011. The two aircraft campaigns encompass more than 17 aircraft contrail cases. A principal component analysis (PCA) of the angular scattering coefficients measured by the polar nephelometer is implemented. The goal is to classify the sampled ice cloud measurements in several clusters representative of different contrail development stages (primary wake, young contrail, aged contrail, and cirrus). Extinction and asymmetry coefficients, nitrogen oxide concentrations, and relative humidity with respect to ice and particle size distributions are analysed for each cluster to characterize the evolution of ice cloud properties during the contrail to cirrus evolution. The PCA demonstrates that contrail optical properties are well suited to identify and discriminate between the different contrail growth stages and to characterize the evolution of contrail properties.

Aerosol particles are important due to their direct and indirect impacts on climate. Within the planetary boundary layer (BL), these particles have a relatively short lifetime due to their frequent removal process by wet deposition. When aerosols are transported into the free troposphere (FT), their atmospheric lifetime increases significantly, making them representative of large spatial areas. In this work, we use a combination of in situ measurements performed at the high altitude PUY (Puy de Dôme, 45°46′ N, 2°57′ E, 1465 m a.s.l) station, together with LIDAR profiles at Clermont-Ferrand for characterizing FT conditions, and further characterize the physical properties of aerosol in this poorly documented area of the atmosphere. First, a combination of four criteria was used to identify whether the PUY station lies within the FT or within the BL. Results show that the PUY station is located in BL with frequencies ranging from 50% during the winter, up to 97% during the summer. Then, the classification is applied to a year-long dataset (2015) of particle size distribution data to study the differences in particle physical characteristics (size distribution) and black carbon (BC) concentrations between the FT and the BL. Although BC, Aitken, and the accumulation mode particles concentrations were higher in the BL than in the FT in winter and autumn, they were measured to be higher in the FT compared to BL in spring. No significant difference between the BL and the FT concentrations was observed for the nucleation mode particles for all seasons, suggesting a continuous additional source of nucleation mode particles in the FT during winter and autumn. Coarse mode particle concentrations were found higher in the FT than in the BL for all seasons and especially during summer. This indicates an efficient long-range transport of large particles in the FT from distant sources (marine and desert) due to higher wind speeds in the FT compared to BL. For FT air masses, we used 204-h air mass back-trajectories combined with boundary layer height estimations from ECMWF ERA-Interim to assess the time they spent in the FT since their last contact with the BL and to evaluate the impact of this parameter on the aerosol properties. We observed that even after 75 h without any contact with the BL, FT aerosols preserve specific properties of their air mass type.

We present a Rayleigh-Mie-Raman LIDAR system in operation at Clermont-Ferrand (France) since 2008. The system provides continuous vertical tropospheric profiles of aerosols, cirrus optical properties and water vapour mixing ratio. Located in proximity to the high altitude Puy de Dôme station, labelled as the GAW global station PUY since August 2014, it is a useful tool to describe the boundary layer dynamics and hence interpret in situ measurements. This LIDAR has been upgraded with specific hardware/software developments and laboratory calibrations in order to improve the quality of the profiles, calibrate the depolarization ratio, and increase the automation of operation. As a result, we provide a climatological water vapour profile analysis for the 2009–2013 period, showing an annual cycle with a winter minimum and a summer maximum, consistent with in-situ observations at the PUY station. An overview of a preliminary climatology of cirrus clouds frequency shows that in 2014, more than 30% of days present cirrus events. Finally, the backscatter coefficient profile observed on 27 September 2014 shows the capacity of the system to detect cirrus clouds at 13 km altitude, in presence of aerosols below the 5 km altitude.

Aerosols of the volcanic degassing plumes from Mt. Etna and Mt. Stromboli were probed with in situ instruments on board the Deutsches Zentrum für Luft- und Raumfahrt research aircraft Falcon during the contrail, volcano, and cirrus experiment CONCERT in September 2011. Aerosol properties were analyzed using angular-scattering intensities and particle size distributions measured simultaneously with the Polar Nephelometer and the Forward Scattering Spectrometer probes (FSSP series 100 and 300), respectively. Aerosols of degassing plumes are characterized by low values of the asymmetry parameter (between 0.6 and 0.75); the effective diameter was within the range of 1.5–2.8 µm and the maximal diameter was lower than 20 µm. A principal component analysis applied to the Polar Nephelometer data indicates that scattering features of volcanic aerosols of different crater origins are clearly distinctive from angular-scattering intensities of cirrus and contrails. Retrievals of aerosol properties revealed that the particles were \"optically spherical\" and the estimated values of the real part of the refractive index are within the interval from 1.35 to 1.38. The interpretation of these results leads to the conclusion that the degassing plume aerosols were porous with air voids. Our estimates suggest that aerosol particles contained about 18 to 35 % of air voids in terms of the total volume.

Aerosols influence the Earth radiative budget through scattering and absorption of solar radiation. Several methods are used to investigate aerosol properties and thus quantify their direct and indirect impacts on climate. At the Puy de Dôme station, continuous high-altitude near-surface in situ measurements and low-altitude ground-based remote sensing atmospheric column measurements give the opportunity to compare the aerosol extinction measured with both methods over a 1-year period. To our knowledge, it is the first time that such a comparison is realised with continuous measurements of a high-altitude site during a long-term period. This comparison addresses to which extent near-surface in situ measurements are representative of the whole atmospheric column, the aerosol mixing layer (ML) or the free troposphere (FT). In particular, the impact of multi-aerosol layers events detected using lidar backscatter profiles is analysed. A good correlation between in situ aerosol extinction coefficient and aerosol optical depth (AOD) measured by the Aerosol Robotic Network (AERONET) sun photometer is observed with a correlation coefficient around 0.80, indicating that the in situ measurements station is representative of the overall atmospheric column. After filtering for multilayer cases and correcting for each layer optical contribution (ML and FT), the atmospheric structure seems to be the main factor influencing the comparison between the two measurement techniques. When the site lies in the ML, the in situ extinction represents 45 % of the sun photometer ML extinction while when the site lies within the FT, the in situ extinction is more than 2 times higher than the FT sun photometer extinction. Moreover, the assumption of a decreasing linear vertical aerosol profile in the whole atmosphere has been tested, significantly improving the instrumental agreement. Remote sensing retrievals of the aerosol particle size distributions (PSDs) from the sun photometer observations are then compared to the near-surface in situ measurements, at dry and at ambient relative humidities. When in situ measurements are considered at dry state, the in situ fine mode diameters are 44 % higher than the sun-photometer-retrieved diameters and in situ volume concentrations are 20 % lower than those of the sun-photometer-retrieved fine mode concentration. Using a parameterised hygroscopic growth factor applied to aerosol diameters, the difference between in situ and retrieved diameters grows larger. Coarse mode in situ diameters and concentrations show a good correlation with retrieved PSDs from remote sensing.

The Aerosol, Radiation and Clouds in southern Africa (AEROCLO-sA) project investigates the role of aerosols on the regional climate of southern Africa. This is a unique environment where natural and anthropogenic aerosols and a semipermanent and widespread stratocumulus (Sc) cloud deck are found. The project aims to understand the dynamical, chemical, and radiative processes involved in aerosol–cloud–radiation interactions over land and ocean and under various meteorological conditions. The AEROCLO-sA field campaign was conducted in August and September of 2017 over Namibia. An aircraft equipped with active and passive remote sensors and aerosol in situ probes performed a total of 30 research flight hours. In parallel, a ground-based mobile station with state-of-the-art in situ aerosol probes and remote sensing instrumentation was implemented over coastal Namibia, and complemented by ground-based and balloonborne observations of the dynamical, thermodynamical, and physical properties of the lower troposphere. The focus laid on mineral dust emitted from salty pans and ephemeral riverbeds in northern Namibia, the advection of biomass-burning aerosol plumes from Angola subsequently transported over the Atlantic Ocean, and aerosols in the marine boundary layer at the ocean–atmosphere interface. This article presents an overview of the AEROCLO-sA field campaign with results from the airborne and surface measurements. These observations provide new knowledge of the interactions of aerosols and radiation in cloudy and clear skies in connection with the atmospheric dynamics over southern Africa. They will foster new advanced climate simulations and enhance the capability of spaceborne sensors, ultimately allowing a better prediction of future climate and weather in southern Africa.

Brown carbon (BrC) is a fraction of organic aerosol (OA) that absorbs radiation in the ultraviolet and short visible wavelengths. Its contribution to radiative forcing is uncertain due to limited knowledge of its imaginary refractive index (k). This study investigates the variability of k for OA from wildfires, residential, shipping, and traffic emission sources over Europe. The Multiscale Online Nonhydrostatic Atmosphere Chemistry (MONARCH) model simulated OA concentrations and source contributions, feeding an offline optical tool to constrain k values at 370 nm. The model was evaluated against OA mass concentrations from aerosol chemical speciation monitors (ACSMs) and filter sample measurements, as well as aerosol light absorption measurements at 370 nm derived from an Aethalometer™ from 12 sites across Europe. Results show that MONARCH captures the OA temporal variability across environments (regional, suburban, and urban background). Residential emissions are a major OA source in colder months, while secondary organic aerosol (SOA) dominates in warmer periods. Traffic is a minor primary OA contributor. Biomass and coal combustion significantly influence OA absorption, with shipping emissions also notable near harbors. Optimizing k values at 370 nm revealed significant variability in OA light absorption, influenced by emission sources and environmental conditions. Derived k values for biomass burning (0.03 to 0.13), residential (0.008 to 0.13), shipping (0.005 to 0.08), and traffic (0.005 to 0.07) sources improved model representation of OA absorption compared to a constant k. Introducing such emission source-specific constraints is an innovative approach to enhance OA absorption in atmospheric models.