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In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2009–2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes.

The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model–measurement evaluation of the particle light scattering enhancement factor f(RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f(RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f(RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f(RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH = 0 % and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RH = 0 % is assumed as the model dry RH and 1.16 when RH = 40 % is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model–measurement evaluation and model improvements are provided.

A reference dataset of multi-wavelength particle light scattering and hemispheric backscattering coefficients for different relative humidities (RH) between RH = 30 and 95% and wavelengths between λ = 450 nm and 700 nm is described in this work. Tandem-humidified nephelometer measurements from 26 ground-based sites around the globe, covering multiple aerosol types, have been re-analysed and harmonized into a single dataset. The dataset includes multi-annual measurements from long-term monitoring sites as well as short-term field campaign data. The result is a unique collection of RH-dependent aerosol light scattering properties, presented as a function of size cut. This dataset is important for climate and atmospheric model-measurement inter-comparisons, as a means to improve model performance, and may be useful for satellite and remote sensing evaluation using surface-based, in-situ measurements.Design Type(s)spectral data collection and processing objective • data integration objective • time series designMeasurement Type(s)light scatteringTechnology Type(s)NephelometryFactor Type(s)geographic location • instrument • Environment • temporal_intervalSample Characteristic(s)United States of America • climate system • Canada • The Netherlands • Greece • Germany • Portuguese Republic • South Korea • China • United Kingdom • Finland • Switzerland • Maldives Archipelago • Brazil • Republic of Ireland • Niger • India • Kingdom of Spain • Kingdom of NorwayMachine-accessible metadata file describing the reported data (ISA-Tab format)

This investigation focuses on the characterisation of the aerosol particle hygroscopicity. Aerosol particle optical properties were measured at Granada, Spain, during winter and spring seasons in 2013. Measured optical properties included particle light-absorption coefficient (σ ap ) and particle light-scattering coefficient (σ sp ) at dry conditions and at relative humidity (RH) of 85±10%. The scattering enhancement factor, f(RH=85%), had a mean value of 1.5±0.2 and 1.6±0.3 for winter and spring campaigns, respectively. Cases of high scattering enhancement were more frequent during the spring campaign with 27% of the f(RH=85%) values above 1.8, while during the winter campaign only 8% of the data were above 1.8. A Saharan dust event (SDE), which occurred during the spring campaign, was characterised by a predominance of large particles with low hygroscopicity. For the day when the SDE was more intense, a mean daily value of f(RH=85%)=1.3±0.2 was calculated. f(RH=85%) diurnal cycle showed two minima during the morning and afternoon traffic rush hours due to the increase in non-hygroscopic particles such as black carbon and road dust. This was confirmed by small values of the single-scattering albedo and the scattering Ångstrom exponent. A significant correlation between f(RH=85%) and the fraction of particulate organic matter and sulphate was obtained. Finally, the impact of ambient RH in the aerosol radiative forcing was found to be very small due to the low ambient RH. For high RH values, the hygroscopic effect should be taken into account since the aerosol forcing efficiency changed from −13 W/m 2 at dry conditions to −17 W/m 2 at RH=85%.

A harmonized data set of aerosol particle number size distributions and cloud condensation nuclei (CCN) concentrations at 10 US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) sites is presented. Additional complementary data including total particle number concentration, aerosol chemical composition and aerosol optical properties are included where available. Calculated parameters related to particle activation, (e.g., activated fraction, hygroscopicity parameter and critical diameter) are provided. DOE/ARM data are acquired and processed following DOE/ARM protocols which are based on international recommendations. Here, the data have undergone additional stages of quality assessment including various closure tests. This data set may be useful for studying aerosol processes and, with other data, assessing aerosol-cloud- interactions. High-resolution (5-min) data is provided along with 1-h averaged data, making the data set suitable for exploring the importance of new particle formation (NPF) events on CCN concentrations. Further applications include model and satellite evaluation of aerosol size distributions and CCN concentrations, and exploring relationships among different aerosol properties which may be useful for improving model parametrizations.

PM 10 was collected during an EMEP winter campaign of 2017–2018 in two urban background sites in Barcelona (BCN) and Granada (GRA), two Mediterranean cities in the coast and inland, respectively. The concentrations of PM 10 , organic carbon (OC), elemental carbon (EC), and organic molecular tracer compounds such as hopanes, anhydro-saccharides, polycyclic aromatic hydrocarbon, and several biogenic and anthropogenic markers of secondary organic aerosols (SOA) were two times higher in GRA compared to BCN and related to the atmospheric mixing heights in the areas. Multivariate curve resolution (MCR-ALS) source apportionment analysis identified primary emissions sources (traffic + biomass burning) that were responsible for the 50% and 20% of the organic aerosol contributions in Granada and Barcelona, respectively. The contribution of biomass burning was higher in the holidays than in the working days in GRA while all primary combustion emissions decreased in holidays in BCN. The MCR-ALS identified that oxidative species and SOA formation processes contributed to 40% and 80% in Granada and Barcelona, respectively. Aged SOA was dominant in Granada and Barcelona under stagnant atmospheric conditions and in presence of air pollution. On the other hand, fresh SOA contributions from α-pinene oxidation ( cis -pinonic acid) were three times higher in Barcelona than Granada and could be related to new particle formation, essentially due to overall cleaner air conditions and elevated air temperatures.

Short-range elastic backscatter lidar (SR-EBL) systems are remote sensing instruments for studying low atmospheric boundary layer processes. This work presents a field campaign oriented to filling the gap between the near-surface aerosol processes regarding aerosol radiative properties and connecting them with the atmospheric boundary layer (ABL), centering attention on the residual layer and the ABL transition periods. A Colibri Aerosol Lidar (CAL) instrument, based on the short-range lidar with high spatio-temporal resolution, was used for the first time in the ACTRIS AGORA facility (Andalusian Global Observatory of the Atmosphere) in Granada (Spain). This study showed the possibility of combining lidar and in situ measurements in the lowermost 150 m. The results address, on the one hand, the characterization of the short-range lidar for developing a method to find the calibration constant of the system and to correct the incomplete overlap to further data exploitation. On the other hand, relevant radiative properties such as the temporal series of the aerosol lidar ratio and extinction coefficient were quantified. The campaign was divided in three different periods based on the vehicular emission peak in the early mornings, namely, before, during, and after the emission peak. For before and after the emission peak data classification, aerosol properties presented closer values; however, large variability was obtained after the emission peak reaching the maximum values of extinction and a lidar ratio up to 51.5 ± 11.9 (Mm)−1 and 36.0 ± 10.5 sr, respectively. During the emission peaks, the values reached for extinction and lidar ratio were up to 136.8 ± 26.5 (Mm)−1 and 119.0 ± 22.7 sr, respectively.

Measurements on 27 June 2011 were performed over the Southern Iberian Peninsula at Granada EARLINET station, using active and passive remote sensing and airborne and surface in-situ data in order to study the entrainment processes between aerosols in the free troposphere and those in the planetary boundary layer (PBL). To this aim the temporal evolution of the lidar depolarisation, backscatter-related Angström exponent and potential temperature profiles were used in combination with the PBL contribution to the aerosol optical depth (AOD). Our results show that the mineral dust entrainment in the PBL was caused by the convective processes which 'trapped' the lofted mineral dust layer, distributing the mineral dust particles within the PBL. The temporal evolution of ground-based in-situ data evidenced the impact of this process at surface level. Finally, the amount of mineral dust in the atmospheric column available to be dispersed into the PBL was estimated by means of POLIPHON (Polarizing Lidar Photometer Networking). The dust mass concentration derived from POLIPHON was compared with the coarse-mode mass concentration retrieved with airborne in-situ measurements. Comparison shows differences below 50 µg/m 3 (30% relative difference) indicating a relative good agreement between both techniques.

In this work we present an analysis of aerosol microphysical properties during a mineral dust event taking advantage of the combination of different state-of-the-art retrieval techniques applied to active and passive remote sensing measurements and the evaluation of some of those techniques using independent data acquired from in situ aircraft measurements. Data were collected in a field campaign performed during a mineral dust outbreak at the Granada, Spain, experimental site (37.16° N, 3.61° W, 680 m a.s.l.) on 27 June 2011. Column-integrated properties are provided by sun- and star-photometry, which allows for a continuous evaluation of the mineral dust optical properties during both day and nighttime. Both the linear estimation and AERONET (Aerosol Robotic Network) inversion algorithms are applied for the retrieval of the column-integrated microphysical particle properties. In addition, vertically resolved microphysical properties are obtained from a multi-wavelength Raman lidar system included in EARLINET (European Aerosol Research Lidar Network), by using both LIRIC (Lidar Radiometer Inversion Code) algorithm during daytime and an algorithm applied to the Raman measurements based on the regularization technique during nighttime. LIRIC retrievals reveal the presence of dust layers between 3 and 5 km a.s.l. with volume concentrations of the coarse spheroid mode up to 60 µm3 cm−3. The combined use of the regularization and LIRIC methods reveals the night-to-day evolution of the vertical structure of the mineral dust microphysical properties and offers complementary information to that from column-integrated variables retrieved from passive remote sensing. Additionally, lidar depolarization profiles and LIRIC retrieved volume concentration are compared with aircraft in situ measurements. This study presents for the first time a comparison of the total volume concentration retrieved with LIRIC with independent in situ measurements, obtaining agreement within the estimated uncertainties for both methods and quite good agreement for the vertical distribution of the aerosol layers. Regarding the depolarization, the first published data set of the CAS-POL for polarization ratios is presented here and qualitatively compared with the lidar technique.

This study presents a comprehensive phenomenological analysis of cloud condensation nuclei (CCN) and aerosol properties – including activation properties, microphysical characteristics, chemical composition, and optical properties – across nine surface sites in different environments. Aerosol properties vary widely, reflecting the diverse environments, and controlling the CCN activation characteristics. Despite their critical role in aerosol–cloud interactions, CCN observations remain sparse and unevenly distributed, limiting global assessments of activation behavior. To address this gap, this study presents CCN predictive methods based on chemical composition combined with particle number size distribution (PNSD) data, and aerosol optical properties (AOPs). The chemical composition driven predictions are tested using three hygroscopicity schemes. All schemes overpredict the CCN concentrations (median relative bias; MRB = 13 %–15 %), although the two composition-derived CCN concentrations are markedly better predictors than the fixed-κchem assumption (MRB = 24 %). The AOPs-derived CCN prediction is based on two approaches: first, an extended empirical parameterization of Shen et al. (2019) (hereafter S2019) to 13 stations, which reduces bias from −27 % to −8 % and improves CCN agreement; and second, a random forest model that infers Twomey activation parameters (C and k) using both the S2019 variables and all the available AOPs. Including all AOPs reduces MRB from 19 % to 15 % and highlights the role of absorption in predicting CCN activation. These findings demonstrate that both chemical and optical measurements can provide a reasonable estimate of CCN concentrations when direct measurements are unavailable. These results will enable retrospective analyses of long-term aerosol time series to investigate aerosol–cloud interactions.