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Aerosol absorption is a key property to assess the radiative impacts of aerosols on climate at both global and regional scales. The aerosol physico-chemical and optical properties remain not sufficiently constrained in climate models, with difficulties to properly represent both the aerosol load and their absorption properties in clear and cloudy scenes, especially for absorbing biomass burning aerosols (BBA). In this study we focus on biomass burning (BB) particle plumes transported above clouds over the southeast Atlantic (SEA) region off the southwest coast of Africa, in order to improve the representation of their physico-chemical and absorption properties. The methodology is based on aerosol regional numerical simulations from the WRF-Chem coupled meteorology–chemistry model combined with a detailed inventory of BB emissions and various sets of innovative aerosol remote sensing observations, both in clear and cloudy skies from the POLDER-3/PARASOL space sensor. Current literature indicates that some organic aerosol compounds (OC), called brown carbon (BrOC), primarily emitted by biomass combustion absorb the ultraviolet-blue radiation more efficiently than pure black carbon (BC). We exploit this specificity by comparing the spectral dependence of the aerosol single scattering albedo (SSA) derived from the POLDER-3 satellite observations in the 443–1020 nm wavelength range with the SSA simulated for different proportions of BC, OC and BrOC at the source level, considering the homogeneous internal mixing state of particles. These numerical simulation experiments are based on two main constraints: maintaining a realistic aerosol optical depth both in clear and above cloudy scenes and a realistic BC/OC mass ratio. Modelling experiments are presented and discussed to link the chemical composition with the absorption properties of BBA and to provide estimates of the relative proportions of black, organic and brown carbon in the African BBA plumes transported over the SEA region for July 2008. The absorbing fraction of organic aerosols in the BBA plumes, i.e. BrOC, is estimated at 2 % to 3 %. The simulated mean SSA are 0.81 (565 nm) and 0.84 (550 nm) in clear and above cloudy scenes respectively, in good agreement with those retrieved by POLDER-3 (0.85±0.05 at 565 nm in clear sky and at 550 nm above clouds) for the studied period.

The 2014–2015 Holuhraun lava-flood eruption of Bárðarbunga volcano (Iceland) emitted prodigious amounts of sulfur dioxide into the atmosphere. This eruption caused a large-scale episode of air pollution throughout Western Europe in September 2014, the first event of this magnitude recorded in the modern era. We gathered chemistry-transport simulations and a wealth of complementary observations from satellite sensors (OMI, IASI), ground-based remote sensing (lidar, sunphotometry, differential optical absorption spectroscopy) and ground-level air quality monitoring networks to characterize both the spatial-temporal distributions of volcanic SO2 and sulfate aerosols as well as the dynamics of the planetary boundary layer. Time variations of dynamical and microphysical properties of sulfate aerosols in the aged low-tropospheric volcanic cloud, including loading, vertical distribution, size distribution and single scattering albedo, are provided. Retrospective chemistry-transport simulations at low horizontal resolution (25 km × 25 km) capture the correct temporal dynamics of this far-range air pollution event but fail to reproduce the correct magnitude of SO2 concentration at ground-level. Simulations at higher spatial resolution, relying on two nested domains with finest resolution of 7.3 km × 7.3 km, improve substantially the far-range vertical distribution of the volcanic cloud and subsequently the description of ground-level SO2 concentrations. However, remaining discrepancies between model and observations are shown to result from an inaccurate representation of the planetary boundary layer (PBL) dynamics. Comparison with lidar observations points out a systematic under-estimation of the PBL height by the model, whichever the PBL parameterization scheme. Such a shortcoming impedes the capture of the overlying Bárðarbunga cloud into the PBL at the right time and in sufficient quantities. This study therefore demonstrates the key role played by the PBL dynamics in accurately modelling large-scale volcanogenic air pollution.

Sulfur-rich degassing, which is mostly composed of sulfur dioxide (SO2), plays a major role in the overall impact of volcanism on the atmosphere and climate. The accurate assessment of this impact is currently hampered by the poor knowledge of volcanic SO2 emissions. Here, using an inversion procedure, we show how assimilating snapshots of the volcanic SO2 load derived from the Infrared Atmospheric Sounding Interferometer (IASI) allows for reconstructing both the flux and altitude of the SO2 emissions with an hourly resolution. For this purpose, the regional chemistry-transport model CHIMERE is used to describe the dispersion of SO2 when released in the atmosphere. As proof of concept, we study the 10 April 2011 eruption of the Etna volcano (Italy), which represents one of the few volcanoes instrumented on the ground for the continuous monitoring of SO2 degassing. We find that the SO2 flux time-series retrieved from satellite imagery using the inverse scheme is in agreement with ground observations during ash-poor phases of the eruption. However, large discrepancies are observed during the ash-rich paroxysmal phase as a result of enhanced plume opacity affecting ground-based ultraviolet (UV) spectroscopic retrievals. As a consequence, the SO2 emission rate derived from the ground is underestimated by almost one order of magnitude. Altitudes of the SO2 emissions predicted by the inverse scheme are validated against an RGB image of the Moderate Resolution Imaging Spectroradiometer (MODIS) capturing the near-source atmospheric pathways followed by Etna plumes, in combination with forward trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. At a large distance from the source, modelled SO2 altitudes are compared with independent information on the volcanic cloud height. We find that the altitude predicted by the inverse scheme is in agreement with snapshots of the SO2 height retrieved from recent algorithms exploiting the high spectral resolution of IASI. The validity of the modelled SO2 altitude is further confirmed by the detection of a layer of particles at the same altitude by the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). Analysis of CALIOP colour and depolarization ratios suggests that these particles consist of sulfate aerosols formed from precursory volcanic SO2. The reconstruction of emission altitude, through inversion procedures which assimilate volcanic SO2 column amounts, requires specific meteorological conditions, especially sufficient wind shear so that gas parcels emitted at different altitudes follow distinct trajectories. We consequently explore the possibility and limits of assimilating in inverse schemes infrared (IR) imagery of the volcanic SO2 cloud altitude which will render the inversion procedure independent of the wind shear prerequisite.

We present an adaptable tool, the OPTSIM (OPTical properties SIMulation) software, for the simulation of optical properties and lidar attenuated backscattered profiles (β') from aerosol concentrations calculated by chemistry transport models (CTM). It was developed to model both Level 1 observations and Level 2 aerosol lidar retrievals in order to compare model results to measurements: the level 2 enables to estimate the main properties of aerosols plume structures, but may be limited due to specific assumptions. The level 1, originally developed for this tool, gives access to more information about aerosols properties (β') requiring, at the same time, less hypothesis on aerosols types. In addition to an evaluation of the aerosol loading and optical properties, active remote sensing allows the analysis of aerosols' vertical structures. An academic case study for two different species (black carbon and dust) is presented and shows the consistency of the simulator. Illustrations are then given through the analysis of dust events in the Mediterranean region during the summer 2007. These are based on simulations by the CHIMERE regional CTM and observations from the CALIOP space-based lidar, and highlight the potential of this approach to evaluate the concentration, size and vertical structure of the aerosol plumes.

In this study, we investigate the shortwave aerosol direct radiative forcing (ADRF) and its feedback on air temperature and atmospheric dynamics during a major fire event that occurred in Russia during August 2010. The methodology is based on an offline coupling between the CHIMERE chemistry-transport and the Weather Research and Forecasting (WRF) models. First, simulations for the period 5–12 August 2010 have been evaluated by using AERONET (AErosol RObotic NETwork) and satellite measurements of the POLarization and Directionality of the Earth's Reflectance (POLDER) and the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) sensors. During this period, elevated POLDER aerosol optical thickness (AOT) is found over a large part of eastern Europe, with values above 2 (at 550 nm) in the aerosol plume. According to CALIOP observations, particles remain confined to the first five kilometres of the atmospheric layer. Comparisons with satellite measurements show the ability of CHIMERE to reproduce the regional and vertical distribution of aerosols during their transport from the source region. Over Moscow, AERONET measurements indicate an important increase of AOT (340 nm) from 0.7 on 5 August to 2–4 between 6 and 10 August when the aerosol plume was advected over the city. Particles are mainly observed in the fine size mode (radius in the range 0.2–0.4 μm) and are characterized by elevated single-scattering albedo (SSA) (0.95–0.96 between 440 and 1020 nm). Comparisons of simulations with AERONET measurements show that aerosol physical–optical properties (size distribution, AOT, SSA) have been well simulated over Moscow in terms of intensity and/or spectral dependence. Secondly, modelled aerosol optical properties have been used as input in the radiative transfer code of WRF to evaluate their direct radiative impact. Simulations indicate a significant reduction of solar radiation at the ground (up to 80–150 W m−2 in diurnal averages over a large part of eastern Europe due to the presence of the aerosol plume. This ADRF causes an important reduction of the near-surface air temperature between 0.2 and 2.6° on a regional scale. Moscow has been affected by the aerosol plume, especially between 6 and 10 August. During this period, aerosol causes a significant reduction of surface shortwave radiation (up to 70–84 W m−2 in diurnal averages) with a moderate part (20–30%) due to solar absorption within the aerosol layer. The resulting feedbacks lead to a cooling of the air up to 1.6° at the surface and 0.1° at an altitude of 1500–2000 m (in diurnal averages), that contribute to stabilize the atmospheric boundary layer (ABL). Indeed, a reduction of the ABL height of 13 to 65% has been simulated during daytime in presence of aerosols. This decrease is the result of a lower air entrainment as the vertical wind speed in the ABL is shown to be reduced by 5 to 80% (at midday) when the feedback of the ADRF is taken into account. However, the ADRF is shown to have a lower impact on the horizontal wind speed, suggesting that the dilution of particles would be mainly affected by the weakening of the ABL development and associated vertical entrainment. Indeed, CHIMERE simulations driven by the WRF meteorological fields including this ADRF feedback result in a large increase in the modelled near-surface PM10 concentrations (up to 99%). This is due to their lower vertical dilution in the ABL, which tend to reduce model biases with the ground PM10 values observed over Moscow during this specific period.