ALBERT

Description: Intense anthropogenic emissions over the Indian sub-continent lead to the formation of layers of particulate pollution that can be transported to the high altitude regions of the Himalaya-Hindu-Kush (HKH). Aerosol particles contain a substantial fraction of strongly absorbing material, including black carbon (BC), organic compounds (OC), and dust all of which can contribute to atmospheric warming, in addition to greenhouse gases. Using a 3-year record of continuous measurements of aerosol optical properties, we present a time series of key climate relevant aerosol properties including the aerosol absorption (σap) and scattering (σsp) coefficients as well as the single-scattering albedo (w0). Results of this investigation show substantial seasonal variability of these properties, with long range transport during the pre- and post-monsoon seasons and efficient precipitation scavenging of aerosol particles during the monsoon season. The monthly averaged scattering coefficients range from 0.1 Mm−1 (monsoon) to 20 Mm−1 while the average absorption coefficients range from 0.5 Mm−1 to 3.5 Mm−1. Both have their maximum values during the pre-monsoon period (April) and reach a minimum during Monsoon (July–August). This leads to dry w0 values from 0.86 (pre-monsoon) to 0.79 (monsoon) seasons. Significant diurnal variability due to valley wind circulation is also reported. Using aerosol optical depth (AOD) measurements, we calculated the resulting direct local radiative forcing due to aerosols for selected air mass cases. We found that the presence of absorbing particulate material can locally induce an additional top of the atmosphere (TOA) forcing of 10 to 20 W m−2 for the first atmospheric layer (500 m above surface). The TOA positive forcing depends on the presence of snow at the surface, and takes place preferentially during episodes of regional pollution occurring on a very regular basis in the Himalayan valleys. Warming of the first atmospheric layer is paralleled by a substantial decrease of the amount of radiation reaching the surface. The surface forcing is estimated to range from −4 to −20 W m−2 for small-scale regional pollution events and large-scale pollution events, respectively. The calculated surface forcing is also very dependent on surface albedo, with maximum values occurring over a snow-covered surface. Overall, this work presents the first estimates of aerosol direct radiative forcing over the high Himalaya based on in-situ aerosol measurements, and results suggest a TOA forcing significantly greater than the IPCC reported values for green house gases.

Description: The shortwave radiative forcing (ΔF) and the radiative forcing efficiency (ΔFeff) of natural and anthropogenic aerosols have been analyzed using estimates of radiation both at the Top (TOA) and at the Bottom Of Atmosphere (BOA) modeled based on AERONET aerosol retrievals. Six main types of atmospheric aerosols have been compared (desert mineral dust, biomass burning, urban-industrial, continental background, oceanic and free troposphere) in similar observational conditions (i.e., for solar zenith angles between 55° and 65°) in order to compare the nearly same solar geometry. The instantaneous ΔF averages obtained vary from −122 ± 37 Wm−2 (aerosol optical depth, AOD, at 0.55 μm, 0.85 ± 0.45) at the BOA for the mixture of desert mineral dust and biomass burning aerosols in West Africa and −42 ± 22 Wm−2 (AOD = 0.9 ± 0.5) at the TOA for the pure mineral dust also in this region up to −6 ± 3 Wm−2 and −4 ± 2 Wm−2 (AOD = 0.03 ± 0.02) at the BOA and the TOA, respectively, for free troposphere conditions. This last result may be taken as reference on a global scale. Furthermore, we observe that the more absorbing aerosols are overall more efficient at the BOA in contrast to at the TOA, where they backscatter less solar energy into the space. The analysis of the radiative balance at the TOA shows that, together with the amount of aerosols and their absorptive capacity, it is essential to consider the surface albedo of the region on which they are. Thus, we document that in regions with high surface reflectivity (deserts and snow conditions) atmospheric aerosols lead to a warming of the Earth-atmosphere system.

Description: Within the frame of the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) project, the Météo-France aircraft ATR-42 performed 22 research flights over central Europe and the North Sea during the intensive observation period in May 2008. For the campaign, the ATR-42 was equipped to study the aerosol physical, chemical, hygroscopic and optical properties, as well as cloud microphysics. For the 22 research flights, retroplume analyses along the flight tracks were performed with FLEXPART in order to classify air masses into five sectors of origin, allowing for a qualitative evaluation of emission influence on the respective air parcel. This study shows that the extensive aerosol parameters (aerosol mass and number concentrations) show vertical decreasing gradients and in some air masses maximum mass concentrations (mainly organics) in an intermediate layer (1–3 km). The observed mass concentrations (in the boundary layer (BL): between 10 and 30 μg m−3; lower free troposphere (LFT): 0.8 and 14 μg m−3) are high especially in comparison with the 2015 European norms for PM2.5 (25 μg m−3) and with previous airborne studies performed over England (Morgan et al., 2009; McMeeking et al., 2012). Particle number size distributions show a larger fraction of particles in the accumulation size range in the LFT compared to BL. The chemical composition of submicron aerosol particles is dominated by organics in the BL, while ammonium sulphate dominates the submicron aerosols in the LFT, especially in the aerosol particles originated from north-eastern Europe (~ 80%), also experiencing nucleation events along the transport. As a consequence, first the particle CCN acting ability, shown by the CCN/CN ratio, and second the average values of the scattering cross sections of optically active particles (i.e. scattering coefficient divided by the optical active particle concentration) are increased in the LFT compared to BL.

Description: During the Eyjafjallajökull eruption (14 April to 24 May 2010), the volcanic aerosol cloud was observed across Europe by several airborne in situ and ground-based remote-sensing instruments. On 18 and 19 May, layers of depolarizing particles (i.e. non-spherical particles) were detected in the free troposphere above the Puy de Dôme station, (PdD, France) with a Rayleigh-Mie LIDAR emitting at a wavelength of 355 nm, with parallel and crossed polarization channels. These layers in the free troposphere (FT) were also well captured by simulations with the Lagrangian particle dispersion model FLEXPART, which furthermore showed that the ash was eventually entrained into the planetary boundary layer (PBL). Indeed, the ash cloud was then detected and characterized with a comprehensive set of in situ instruments at the Puy de Dôme station (PdD). In agreement with the FLEXPART simulation, up to 65 μg m−3 of particle mass and 2.2 ppb of SO2 were measured at PdD, corresponding to concentrations higher than the 95 percentile of 2 yr of measurements at PdD. Moreover, the number concentration of particles increased to 24 000 cm−3, mainly in the submicronic mode, but a supermicronic mode was also detected with a modal diameter of 2 μm. The resulting optical properties of the ash aerosol were characterized by a low scattering Ångström exponent (0.98), showing the presence of supermicronic particles. For the first time to our knowledge, the combination of in situ optical and physical characterization of the volcanic ash allowed the calculation of the mass-to-extinction ratio (η) with no assumptions on the aerosol density. The mass-to-extinction ratio was found to be significantly different from the background boundary layer aerosol (max: 1.57 g m−2 as opposed to 0.33 ± 0.03 g m−2). Using this ratio, ash mass concentration in the volcanic plume derived from LIDAR measurements was found to be 655 ± 23 μg m−3 when the plume was located in the FT (3000 m above the sea level – a.s.l.). This ratio could also be used to retrieve an aerosol mass concentration of 579 ± 60 μg m−3 on 19 April, when LIDAR observations detected the ash cloud at 3000 m a.s.l. in correspondence with model simulations (FLEXPART). On 22 April, another ash plume entered the BL, and although it was more diluted than during the May episode, the French research aircraft ATR42 that passed over Clermont-Ferrand in the PBL confirmed the presence of particles with a supermicronic mode, again with a modal diameter at 2 μm. This data set combining airborne, ground-based and remote sensing observations with dispersion model simulations shows an overall very good coherence during the volcanic eruption period, which allows a good confidence in the characteristics of the ash particles that can be derived from this unique data set.

Description: Intense anthropogenic emissions over the Indian sub-continent lead to the formation of layers of particulate pollution that can be transported to the high altitude regions of the Himalaya-Hindu-Kush (HKH). Aerosol particles contain a substantial fraction of strongly absorbing material, including black carbon (BC), organic compounds (OC), and dust all of which can contribute to atmospheric warming, in addition to greenhouse gases. Using a 3-year record of continuous measurements of aerosol optical properties, we present a time series of key climate relevant aerosol properties including the aerosol absorption (σap) and scattering (σsp) coefficients as well as the single-scattering albedo (w). Results of this investigation show substantial seasonal variability of these properties, with long range transport during the pre- and post-monsoon seasons and efficient precipitation scavenging of aerosol particles during the monsoon season. The monthly averaged scattering coefficients range from 0.1 Mm−1 (monsoon) to 20 Mm−1 while the average absorption coefficients range from 0.5 Mm−1 to 3.5 Mm−1. Both have their maximum values during the pre-monsoon period (April) and reach a minimum during Monsoon (July–August). This leads to w values from 0.86 (pre-monsoon) to 0.79 (monsoon) seasons. Significant diurnal variability due to valley wind circulation is also reported. Using typical air mass trajectories encountered at the station, and aerosol optical depth (aod) measurements, we calculated the resulting direct local radiative forcing due to aerosols. We found that the presence of absorbing particulate material can locally induce an additional top of the atmosphere (TOA) forcing of 10 to 20 W m−2 for the first atmospheric layer (500 m above surface). The TOA positive forcing depends on the presence of snow at the surface, and takes place preferentially during episodes of regional pollution occurring on a very regular basis in the Himalayan valleys. Warming of the first atmospheric layer is paralleled by a substantial decrease of the amount of radiation reaching the surface. The surface forcing is estimated to range from −4 to −20 W m−2 for small-scale regional pollution events and large-scale pollution events, respectively. The calculated surface forcing is also very dependent on surface albedo, with maximum values occurring over a snow-covered surface. Overall, this work presents the first estimates of aerosol direct radiative forcing over the high Himalaya based on in-situ aerosol measurements, and results suggest a TOA forcing significantly greater than the IPCC reported values for green house gases.

Description: Within the frame of the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) project the Météo-France aircraft ATR-42 performed 22 research flights, over central Europe and the North Sea during the intensive observation period in May 2008. For the campaign, the ATR-42 was equipped in order to study aerosol physical, chemical and optical properties, as well as cloud microphysics. During the campaign, continental air masses from Eastern and Western Europe were encountered, along with polar and Scandinavian air masses. For the 22 research flights, retroplume analyses along the flight tracks were performed with FLEXPART in order to classify air masses into five sectors of origin which allows for a qualitative evaluation of emission influence on the respective air parcel. In the polluted boundary layer (BL), typical concentrations of particles with diameters larger than 10 nm (N10) are of the order of 5000–6000 cm−3, whereas N10 concentrations of clean air masses were lower than 1300 cm−3. The detection of the largest particle number concentrations occurred in air masses coming from Polar and Scandinavian regions for which an elevated number of nucleation mode (25–28 nm) particles was observed and attributed to new particle formation over open sea. In the free troposphere (FT), typical observed N10 are of the order of 900 cm−3 in polluted air masses and 400–600 cm−3 in clean air masses, respectively. In both layers, the chemical composition of submicron aerosol particles is dominated by organic matter and nitrate in polluted air masses, while, sulphate and ammonium followed by organics dominate the submicron aerosols in clean air masses. The highest CCN/CN ratios were observed within the polar air masses while the CCN concentration values are the highest within the polluted air masses. Within the five air mass sectors defined and the two layers (BL and FT), observations have been distinguished into anticyclonic (first half of May 2008) and cyclonic conditions (second half of May 2008). Strong relationships between meteorological conditions and physical, chemical as well as optical properties are found.

Description: Optical properties of aerosols were measured from the GAW Puy de Dôme station (1465 m) over a seven year period (2006–2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010–2011). The analysis of the spatial and temporal variability of the optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the PBL height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type. At 90% humidity, the scattering factor enhancement (fσsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH = 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type.

Description: The shortwave radiative forcing (ΔF) and the radiative forcing efficiency (ΔFeff) of natural and anthropogenic aerosols have been analyzed using estimates of radiation both at the top (TOA) and at the bottom of atmosphere (BOA) modeled based on AERONET aerosol retrievals. In this study we have considered six main types of atmospheric aerosols: desert mineral dust, biomass burning, urban-industrial, continental background, oceanic and free troposphere. The ΔF averages obtained vary from −148 ± 44 Wm−2 (aerosol optical depth, AOD, at 0.55 μm, 0.85 ± 0.45) at the BOA for the mixture of desert mineral dust and biomass burning aerosols in Central Africa and −42 ± 22 Wm−2 (AOD = 0.86 ± 0.51) at the TOA for the pure mineral dust also in this region up to −6 ± 3 Wm−2 and −4 ± 2 Wm−2 (AOD = 0.03 ± 0.02) at the BOA and the TOA, respectively, for free troposphere conditions. This last result may be taken as reference on a global scale. Furthermore, we observe that the more absorbing aerosols are overall more efficient at the BOA in contrast to at the TOA, where they backscatter less solar energy into the space. The analysis of the radiative balance at the TOA shows that, together with the amount of aerosols and their absorptive capacity, it is essential to consider the surface albedo of the region on which they are. Thus, we document that in regions with high surface reflectivity (deserts and snow conditions) atmospheric aerosols lead to a warming of the Earth-atmosphere system, contributing to the greenhouse gas effect.