The profound changes in global SO2 emissions over the last decades have affected atmospheric composition on a regional and global scale with large impact on air quality, atmospheric deposition and the radiative forcing of sulfate aerosols. Reproduction of historical atmospheric pollution levels based on global aerosol models and emission changes is crucial to prove that such models are able to predict future scenarios. Here, we analyze consistency of trends in observations of sulfur components in air and precipitation from major regional networks and estimates from six different global aerosol models from 1990 until 2015. There are large interregional differences in the sulfur trends consistently captured by the models and observations, especially for North America and Europe. Europe had the largest reductions in sulfur emissions in the first part of the period while the highest reduction came later in North America and East Asia. The uncertainties in both the emissions and the representativity of the observations are larger in Asia. However, emissions from East Asia clearly increased from 2000 to 2005 followed by a decrease, while in India a steady increase over the whole period has been observed and modelled. The agreement between a bottom-up approach, which uses emissions and process-based chemical transport models, with independent observations gives an improved confidence in the understanding of the atmospheric sulfur budget.

Abstract. Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. −15 %, however, with a considerably large interquartile range, suggesting a spread between −35 % and +10 %.

Abstract. In the present work, atmospheric mineral dust from a MACC-II short reanalysis run for 2 years (2007–2008) has been evaluated over northern Africa and the Middle East using satellite aerosol products (from MISR, MODIS and OMI satellite sensors), ground-based AERONET data, in situ PM10 concentrations from AMMA, and extinction vertical profiles from two ground-based lidars and CALIOP satellite-based lidar. The MACC-II aerosol optical depth (AOD) spatial and temporal (seasonal and interannual) variability shows good agreement with those provided by satellite sensors. The capability of the model to reproduce the AOD, Ångström exponent (AE) and dust optical depth (DOD) from daily to seasonal time-scale is quantified over 26 AERONET stations located in eight geographically distinct regions by using statistical parameters. Overall DOD seasonal variation is fairly well simulated by MACC-II in all regions, although the correlation is significantly higher in dust transport regions than in dust source regions. The ability of MACC-II in reproducing dust vertical profiles has been assessed by comparing seasonal averaged extinction vertical profiles simulated by MACC-II under dust conditions with corresponding extinction profiles obtained with lidar instruments at M'Bour and Santa Cruz de Tenerife, and with CALIOP. We find a good agreement in dust layers structures and averaged extinction vertical profiles between MACC-II, the lidars and CALIOP above the marine boundary layer from 1 to 6 km. Surface dust daily mean concentrations from MACC-II reanalysis has been evaluated with daily averaged PM10 at three monitoring stations of the Sahelian Dust Transect. MACC-II correctly reproduces daily to interannual surface dust concentration variability, although it underestimates daily and monthly means all year long, especially in winter and early spring (dry season). MACC-II reproduces well the dust variability recorded along the station transect which reflects the variability in dust emission by different Saharan sources, but fails in reproducing the sporadic and very strong dust events associated to mesoscale convective systems during the wet season.

Abstract. Aerosol particles are important and highly variable components of the terrestrial atmosphere, and they affect both air quality and climate. In order to evaluate their multiple impacts, the most important requirement is to precisely measure their characteristics. Remote sensing technologies such as lidar (light detection and ranging) and sun/sky photometers are powerful tools for determining aerosol optical and microphysical properties. In our work, we applied several methods to joint or separate lidar and sun/sky-photometer data to retrieve aerosol properties. The Raman technique and inversion with regularization use only lidar data. The LIRIC (LIdar-Radiometer Inversion Code) and recently developed GARRLiC (Generalized Aerosol Retrieval from Radiometer and Lidar Combined data) inversion methods use joint lidar and sun/sky-photometer data. This paper presents a comparison and discussion of aerosol optical properties (extinction coefficient profiles and lidar ratios) and microphysical properties (volume concentrations, complex refractive index values, and effective radius values) retrieved using the aforementioned methods. The comparison showed inconsistencies in the retrieved lidar ratios. However, other aerosol properties were found to be generally in close agreement with the AERONET (AErosol RObotic NETwork) products. In future studies, more cases should be analysed in order to clearly define the peculiarities in our results.

[1] In this work we characterize optical properties and assess the direct radiative effect of an ash plume observed on April 17, 2010 by AERONET, lidar and broadband solar flux measurements collocated on the roof of the Laboratory of Atmospheric Optics in Lille, northern France. These measurements allowed experimental evaluation of ash radiative impact and validation of simulations. The derived aerosol model of ash is characterized by a bi-modal size distribution dominated by coarse mode centered at a radius of 1.5 mm and by relatively strong absorption at short wavelengths (single scattering albedo of 0.81 AE 0.02 at 440 nm as opposed to 0.92 AE 0.02 at 670, 870 and 1020 nm). Due to relatively low aerosol optical thickness during the ash plume transport ($0.26 at 440 nm), which is unfavorable for AERONET retrievals, the uncertainties in derived ash aerosol model were additionally evaluated. The complex refractive index of ash was derived assuming that effective refractive index retrieved by AERONET for externally mixed bi-component aerosol can be approximated as an average of refractive indices of two components weighted by their volume concentrations. Evaluation of the accuracy of this approximation showed acceptably small errors in simulations of single scattering albedo and aerosol phase function over the range of scattering angles observed by the AERONET almucantar. Daily average radiative forcing efficiency of ash calculated for a land surface reflectance representing Lille was about À93 AE 12 Wm À2 t 550 À1 and À31 AE 2 Wm À2 t 550 À1 at the bottom and top of the atmosphere; the values for an ocean surface reflectance are also provided.

Abstract. This study presents a multiparameter analysis of aerosol trends over the last 2 decades at regional and global scales. Regional time series have been computed for a set of nine optical, chemical-composition and mass aerosol properties by using the observations from several ground-based networks. From these regional time series the aerosol trends have been derived for the different regions of the world. Most of the properties related to aerosol loading exhibit negative trends, both at the surface and in the total atmospheric column. Significant decreases in aerosol optical depth (AOD) are found in Europe, North America, South America, North Africa and Asia, ranging from −1.2 % yr−1 to −3.1 % yr−1. An error and representativity analysis of the spatially and temporally limited observational data has been performed using model data subsets in order to investigate how much the observed trends represent the actual trends happening in the regions over the full study period from 2000 to 2014. This analysis reveals that significant uncertainty is associated with some of the regional trends due to time and space sampling deficiencies. The set of observed regional trends has then been used for the evaluation of 10 models (6 AeroCom phase III models and 4 CMIP6 models) and the CAMS reanalysis dataset and of their skills in reproducing the aerosol trends. Model performance is found to vary depending on the parameters and the regions of the world. The models tend to capture trends in AOD, the column Ångström exponent, sulfate and particulate matter well (except in North Africa), but they show larger discrepancies for coarse-mode AOD. The rather good agreement of the trends, across different aerosol parameters between models and observations, when co-locating them in time and space, implies that global model trends, including those in poorly monitored regions, are likely correct. The models can help to provide a global picture of the aerosol trends by filling the gaps in regions not covered by observations. The calculation of aerosol trends at a global scale reveals a different picture from that depicted by solely relying on ground-based observations. Using a model with complete diagnostics (NorESM2), we find a global increase in AOD of about 0.2 % yr−1 between 2000 and 2014, primarily caused by an increase in the loads of organic aerosols, sulfate and black carbon.

A 15-channel airborne sun-tracking photometer has been developed. The instrument provides aerosol optical depths over a wide spectral range (0.34–2.25 μm) with an accuracy (ΔAOD) of approximately 0.01. Taking measurements at different altitudes allow us to derive the aerosol extinction vertical profile. Thanks to the wide spectral range of the instrument, information on the aerosol size distribution along the vertical is also available

Routine sun-photometer and micro-lidar measurements were performed in Lille, northern France, in April and May 2010 during the Eyjafjallajökull volcanic eruption. The impact of such an eruption emphasized significance of hazards for human activities and importance of observations of the volcanic aerosol particles. This paper presents the main results of a joint micro-lidar/sun-photometer analysis performed in Lille, where volcanic ash plumes were observed during at least 22 days, whenever weather conditions permitted. Aerosol properties retrieved from automatic sun-photometer measurements (AERONET) were strongly changed during the volcanic aerosol plumes transport over Lille. In most cases, the aerosol optical depth (AOD) increased, whereas Ångström exponent decreased, thus indicating coarse-mode dominance in the volume size distribution. Moreover, the non-spherical fraction retrieved by AERONET significantly increased. The real part of the complex refractive index was up to 1.55 at 440 nm during the eruption, compared to background data of about 1.46 before the eruption. Collocated lidar data revealed that several aerosol layers were present between 2 and 5 km, all originating from the Iceland region as confirmed by backward trajectories. The volcanic ash AOD was derived from lidar extinction profiles and sun-photometer AOD, and its maximum was estimated around 0.37 at 532 nm on 18 April 2010. This value was observed at an altitude of 1700 m and corresponds to an ash mass concentration (AMC) slightly higher than 1000 μg m⁻³ (±50%). An effective lidar ratio of ash particles of 48 sr was retrieved at 532 nm for 17 April during the early stages of the eruption, a value which agrees with several other studies carried out on this topic. Even though the accuracy of the retrievals is not as high as that obtained from reference multiwavelength lidar systems, this study demonstrates the opportunity of micro-lidar and sun-photometer joint data processing for deriving volcanic AMC. It also outlines the fact that a network of combined micro-lidars and sun photometers can be a powerful tool for routine monitoring of aerosols, especially in the case of such hazardous volcanic events