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Abstract. Aerosol particle optical, physical and chemical properties have been previously studied in the United Arab Emirates (UAE), but there is still a gap in the knowledge of particle sources, and in the horizontal and vertical transport of aerosol particles and their precursors in the area. To investigate how aerosol particle and SO2 concentrations at the surface responded to changes in horizontal and vertical transport, we used data from a one-year measurement campaign at a background site where local sources of SO2 where expected to be minimal. The measurement campaign provided a combination of in-situ measurements at the surface, and the boundary layer evolution from vertical and horizontal wind profiles measured by a Doppler lidar. The diurnal structure of the boundary layer in the UAE was very similar from day to day, with deep well-mixed boundary layer during the day transitioning to a shallow nocturnal layer, with the maximum boundary layer height usually being reached around 1400 local time. Both SO2 and nucleation mode aerosol particle concentrations were elevated for surface winds coming from the east or western sectors.We attribute this to oil refineries located on the eastern and western coasts of the UAE. The concentrations of larger cloud condensation nuclei (CCN) sized particles and their activation fraction did not show any clear dependence on wind direction, but the CCN number concentration showed some dependence on wind speed, with higher concentrations coinciding with the weakest surface winds. Peaks in SO2 concentrations were also observed despite low surface wind speeds and wind directions unfavourable for transport. However, winds aloft were much stronger, with wind speeds of 10 m s−1 at 1 km common at night, and with wind directions favourable for transport, and surface-measured concentrations increased rapidly once these particular layers started to be entrained into the growing boundary layer, even if the surface wind direction was from a clean sector. These conditions also displayed higher nucleation mode aerosol particle concentrations, i.e. new particle formation events occurring due to the increase in the gaseous precursor. [ABSTRACT FROM AUTHOR]

Optical properties of surface aerosols at Dome C, Antarctica in 2007-2013 and their potential source areas are presented. Scattering coefficients (ssp) were calculated from measured particle number size distributions with a Mie code and from filter samples using mass scattering efficiencies. Absorption coefficients (sap) were determined with a 3-wavelength Particle Soot Absorption Photometer (PSAP) and corrected for scattering by using two different algorithms. The scattering coefficients were also compared with ssp measured with a nephelometer at the South Pole Station (SPO). The minimum sap was observed in the austral autumn and the maximum in the austral spring, similar to other Antarctic sites. The darkest aerosol, i.e., the lowest single scattering albedo ?o ˜ 0.91 was observed in September and October and the highest ?o ˜ 0.99 in February and March. The uncertainty of the absorption Ångström exponent aap is high. The lowest aap monthly medians were observed in March and the highest in August – October. The equivalent black carbon (eBC) mass concentrations were compared with eBC measured at three other Antarctic sites: the SPO and two coastal sites, Neumayer and Syowa. The maximum monthly median eBC concentrations are almost the same (~3 ± 1 ng m-3 ) at all these sites in October-November. This suggests that there is no significant difference in eBC between the coastal and plateau sites. The seasonal cycle of the eBC mass fraction exhibits a minimum f(eBC) ˜ 0.1% in February-March and a maximum ~4-5% in August-October. Source areas were calculated using 50-day FLEXPART footprints. The highest eBC concentrations and the lowest ?o were associated with air masses coming from South America, Australia and Africa. Vertical simulations that take BC particle removal processes into account show that there would be essentially no BC particles arriving at Dome C from north of latitude 10°S at altitudes < 1600 m. The main biomass-burning regions Africa, Australia and Brazil are more to the south and their smoke plumes have been observed at higher altitudes than that so they can get transported to Antarctica. The seasonal cycle of BC emissions from wildfires and agricultural burning and other fires in South America, Africa and Australia were calculated from data downloaded from the Global Fire Emissions Database (GFED). The maximum total emissions were in August-September but the peak of monthly average eBC concentrations is observed 2 – 3 months later in November not only at Dome C but also at SPO and the coastal stations. The air mass residence-time-weighted BC emissions from South America are approximately an order of magnitude larger than from Africa and Oceania suggesting that South American BC emissions are the largest contributors to eBC at Dome C. At Dome C the maximum and minimum scattering coefficients were observed in austral summer and winter, respectively. At SPO ssp was similar to that observed at Dome C in the austral summer but there was a large difference in winter, suggesting that in winter SPO is more influenced by sea spray emissions than Dome C. The seasonal cycles of ssp at Dome C and at the SPO were compared with the seasonal cycles of secondary and primary marine aerosol emissions. The ssp measured at SPO correlated much better with the sea-spray aerosol emission fluxes in the Southern Ocean than ssp at Dome C. The seasonal cycles of biogenic secondary aerosols were estimated from monthly average phytoplankton biomass concentrations obtained from the CALIOP satellite sensor data. The analysis suggests that a large fraction of the biogenic scattering aerosol observed at Dome C has been formed in the polar zone but it may take a month for the aerosol to be formed, grown and get transported from the sea level to Dome C. [ABSTRACT FROM AUTHOR]

Aerosol particles play an important in role in the microphysics of clouds and hence on their likelihood to precipitate. In the changing climate already dry areas such as the United Arab Emirates (UAE) are predicted to become even drier. Comprehensive observations of the daily and seasonal variation in aerosol particle properties in such locations are required reducing the uncertainty in such predictions. We analyse observations from a one-year measurement campaign at a background location in the United Arab Emirates to investigate the properties of aerosol particles in this region, study the impact of boundary layer mixing on background aerosol particle properties measured at the surface and study the temporal evolution of the aerosol particle cloud formation potential in the region. We used in-situ aerosol particle measurements to characterise the aerosol particle composition, size, number and cloud condensation nuclei (CCN) properties, in-situ SO2 measurements as an anthropogenic signature and a long-range scanning Doppler lidar to provide vertical profiles of the horizontal wind and turbulent properties to monitor the evolution of the boundary layer. Anthropogenic sulphate dominated the aerosol particle mass composition in this location. There was a clear diurnal cycle in the surface wind direction, which had a strong impact on aerosol particle total number concentration, SO2 concentration and black carbon mass concentration. Local sources were the predominant source of black carbon, as concentrations clearly depended on the presence of turbulent mixing, with much higher values during calm nights. The measured concentrations of SO2, instead, were highly dependent on the surface wind direction as well as on the depth of the boundary layer when entrainment from the advected elevated layers occurred. The wind direction at the surface or of the elevated layer suggests that the cities of Dubai, Abu Dhabi and other coastal conurbations were the remote sources of SO2. We observed new aerosol particle formation events almost every day (on four days out of five on average). Calm nights had the highest CCN number concentrations and lowest κ values and activation fractions. We did not observe any clear dependence of CCN number concentration and κ parameter on the height of the daytime boundary layer, whereas the activation fraction did show a slight increase with increasing boundary layer height, due to the change in the shape of the aerosol particle size distribution where the relative portion of larger aerosol particles increased with increasing boundary layer height. We believe that this indicates that size is more important than chemistry for aerosol particle CCN activation at this site. The combination of instrumentation used in this campaign enabled us to identify periods when anthropogenic pollution from remote sources that had been transported in elevated layers was present, and had been mixed down to the surface in the growing boundary layer. [ABSTRACT FROM AUTHOR]

Long-term measurements of black carbon (BC) are warranted for investigating changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including multi-angle absorption photometers (MAAP), particle soot absorption photometers (PSAP), continuous light absorption photometer (CLAP), and Aethalometers. The measured babs can be converted to atmospheric mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC = babs/MBC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS- derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2) and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC, and long-term stability of the correlation slope, which represents the MAC. In general, babs - MBC (COSMOS) correlations were high (r² = 0.84-0.96 for hourly data) at Fukue in Japan, Barrow in Alaska, Ny-Ålesund in Svalbard, Pallastunturi in Finland, and Alert in Canada, and stable up to for 10 years. We successfully estimated MAC values (11.0-15.2 m² g-1 at a wavelength of 550 nm) for these instruments and these MAC values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC in these Arctic sites estimated by this method are consistent with each other, they are applicable to study spatial and temporal variation of MBC and to evaluate performance of numerical model calculations. [ABSTRACT FROM AUTHOR]

Following the emergence of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) responsible for COVID-19 in December 2019 in Wuhan (China) and its spread to the rest of the world, the World Health Organization declared a global pandemic in March 2020. Without effective treatment in the initial pandemic phase, social distancing and mandatory quarantines were introduced as the only available preventative measure. Despite the socioeconomic impacts, air quality improved due to lower pollutant emissions. Here we investigate the effects of the COVID-19 lockdowns on ambient black carbon (BC), which affects climate and damages health, using in-situ observations from 17 European stations in a Bayesian inversion framework. BC emissions declined by 11 % in Europe (20 % in Italy, 32 % in Germany, 20 % in Spain) during lockdown compared to the same period in the previous five years. BC temporal variation in the countries enduring the most drastic restrictions showed the most distinct lockdown impacts. Increased particle light absorption in at the beginning of the lockdown, confirmed by assimilated satellite and remote sensing data, suggests residential combustion was the dominant BC source. Accordingly, in Central and Eastern Europe, which experienced lower than average temperatures, BC was elevated compared to the previous five years. Except for the comparison of BC emissions in the lockdown with the previous five years, an immediate decrease was also seen, as compared with the period before the lockdown, which averaged about 10 % over Europe. Such a decrease was not seen in the previous years, which also confirms an impact on BC emissions from COVID-19. [ABSTRACT FROM AUTHOR]

One-year of ground-based night-time Raman lidar observations have been analysed under the Optimization of Aerosol Seeding In rain enhancement Strategies (OASIS) project, in order to characterize the aerosol particle properties over a rural site in the United Arab Emirates. In total, 1130 aerosol particle layers were detected during the one-year measurement campaign which took place between March 2018 and February 2019. Several subsequent aerosol layers could be observed simultaneously in the atmosphere up to 11 km. The observations indicate that the measurement site is a receptor of frequent dust events but predominantly the dust is mixed with aerosols of anthropogenic and/or marine origin. The mean aerosol optical depth over the measurement site ranged at 0.37 ± 0.12 and 0.21 ± 0.11 for the 355 and 532 nm, respectively. Moreover, a mean lidar ratio of 43 ± 11 sr at a wavelength of 355 nm and 39 ± 10 sr at 532 nm was found. The average linear particle depolarization ratio measured over the course of the campaign was 15 ± 6 % and 19 ± 7 % at 355 nm and 532 nm wavelengths, respectively. Since the region is both a source and a receptor of mineral dust, we have also explored the properties of Arabian mineral dust of the greater area of United Arab of Emirates and the Arabian Peninsula. The observed Arabian dust particle properties were 45 ± 5 (42 ± 5) sr at 355 (532) nm for the lidar ratio, 25 ± 2 % (31 ± 2 %) for the linear particle depolarization ratio at 355 (532) nm, and 0.3 ± 0.2 (0.2 ± 0.2) for the extinction-related Ångström exponent (backscatter-related Ångström exponent) between 355 and 532 nm. This study is the first to report comprehensive optical properties of the Arabian dust particles based on long term observations, using at the fullest the capabilities of a multi wavelength Raman lidar instrument. The results suggest that the mineral dust properties over the Middle East and western Asia, including the observation site, are comparable to those of African mineral dust with regard to the particle depolarization ratios but not for lidar ratios. The smaller lidar ratio values in this study compared to the reference studies are attributed to the difference in the geochemical characteristics of the soil originating in the study region compared to Northern Africa. [ABSTRACT FROM AUTHOR]

In order to assess the global evolution of aerosol parameters affecting climate change, a long-term trend analyses of aerosol optical properties were 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 prewhitening methods and with the Sen's slope were used as main trend analysis methods. 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 coefficients 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 coefficients 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 Arctic, 18 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 30 % 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 2010-2011 for all stations in the eastern and central US. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage enables a better global view of potential aerosol effects on climate changes. [ABSTRACT FROM AUTHOR]

Aerosol particles can contribute to the Arctic Amplification by direct and indirect radiative effects. Specifically, black carbon (BC) in the atmosphere, and when deposited on snow and sea ice, has a positive effect on the top of atmosphere radiation balance during polar day. Current climate models, however, are still struggling to reproduce Arctic aerosol conditions. We present an evaluation study with the global aerosol-climate model ECHAM6.3-HAM2.3 to examine emission-related uncertainties in the BC distribution and the direct radiative effect of BC. The model results are comprehensively compared against latest ground and air-borne aerosol observations for the period 2005–2017 with focus on BC. Four different setups of air pollution emissions are tested. The simulations in general match well with the observed amount and temporal variability of near-surface BC in the Arctic. Using actual daily instead of fixed biomass burning emissions is crucial to reproduce individual pollution events but has only a small influence on the seasonal cycle of BC. Compared to commonly used fixed anthropogenic emissions for the year 2000, an up-to-date inventory with transient air pollution emissions results in up to 30 % higher annual BC burden and an over 0.2 W m−2 higher annual mean all-sky net direct radiative effect of BC at top of the atmosphere over the Eastern Arctic Ocean. We estimate BC in the Arctic to lead to a net gain of up 0.8 W m−2 by the direct radiative effect of atmospheric BC plus the effect by an albedo reduction by BC-in-snow. Long-range transport is identified as one of the main sources of uncertainties for ECHAM6.3-HAM2.3, leading to an overestimation of BC in atmospheric layers above 500 hPa especially in summer. This is related to a misrepresentation in wet removal in one identified case at least, that was observed during the ARCTAS summer aircraft campaign. Over all, the current model version has significantly improved since previous intercomparison studies and performs now better than the AeroCom average in terms of the spatial and temporal distribution of Arctic BC. [ABSTRACT FROM AUTHOR]

The Amazon Basin is a unique region to study atmospheric aerosols, given their relevance for the regional hydrological cycle and large uncertainty of their sources. Multi-year datasets are crucial when contrasting periods of natural conditions and periods influenced by anthropogenic emissions. In the wet season, biogenic sources and processes prevail, and the Amazonian atmospheric composition resembles pre-industrial conditions. In the dry season, the Basin is influenced by widespread biomass burning emissions. This work reports multi-year observations of high time resolution submicrometer (10–600 nm) particle number size distributions at a rain forest site in Amazonia (TT34 tower, 60 km NW from Manaus city), between years 2008–2010 and 2012–2014. Median particle number concentration was 403 cm−3 in the wet season and 1254 cm−3 in the dry season. The Aitken mode (~ 30–100 nm in diameter) was prominent during the wet season, while accumulation mode (~ 100–600 nm in diameter) dominated the particle size spectra during the dry season. Cluster analysis identified groups of aerosol number size distribution influenced by convective downdrafts, nucleation events and fresh biomass burning emissions. New particle formation and subsequent growth was rarely observed during the 749 days of observations, similar to previous observations in the Amazon Basin. A stationary 1D column model (ADCHEM – Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer model) was used to assess importance of processes behind the observed diurnal particle size distribution trends. Three major particle source types are required in the model to reproduce the observations: (i) a surface source of particles in the evening, possibly related to primary biological emissions (ii) entrainment of accumulation mode aerosols in the morning, and (iii) convective downdrafts transporting Aitken mode particles into the boundary layer mostly during the afternoon. The latter process has the largest influence on the modelled particle number size distributions. However, convective downdrafts are often associated with rain and thus act both as a source of Aitken mode particles, and as a sink of accumulation mode particles, causing a net reduction in the median total particle number concentrations in the surface layer. Our study shows that the combination of the three mentioned particle sources are essential to sustain particle number concentrations in Amazonia. [ABSTRACT FROM AUTHOR]

Given the sensitivity of the Arctic climate to short-lived climate forcers, long-term in-situ surface measurements of aerosol parameters are useful in gaining insight into the magnitude and variability of these climate forcings. Seasonality of aerosol optical properties, including aerosol light scattering coefficient, absorption coefficient, single scattering albedo, scattering Ångström exponent, and asymmetry parameter are presented for six monitoring sites throughout the Arctic: Alert, Canada; Barrow, USA; Pallas, Finland; Summit, Greenland; Tiksi, Russia; and Zeppelin Mountain, Ny-Ålesund, Svalbard, Norway. Results show annual variability in all parameters, though the seasonality of each aerosol optical property varies from site to site. There is a large diversity in magnitude and variability of scattering coefficient at all sites, reflecting differences in aerosol source, transport and removal at different locations throughout the Arctic. Of the Arctic sites, the highest annual mean scattering coefficient is measured at Tiksi (12.47 Mm−1) and the lowest annual mean scattering coefficient is measured at Summit (1.74 Mm−1). At most sites, aerosol absorption peaks in the winter and spring, and has a minimum throughout the Arctic in the summer, indicative of the Arctic haze phenomenon; however, nuanced variations in seasonalities suggest that this phenomenon is not identically observed in all regions of the Arctic. The highest annual mean absorption coefficient is measured at Pallas (0.48 Mm−1) and Summit has the lowest annual mean absorption coefficient (0.12 Mm−1). At the Arctic monitoring stations analyzed here, mean annual single scattering albedo ranges from 0.909–0.960 (at Pallas and Barrow, respectively), mean annual scattering Ångström exponent ranges from 1.04–1.80 (at Barrow and Summit, respectively), and mean asymmetry parameter ranges from 0.57–0.75 (at Alert and Summit, respectively). Systematic variability of aerosol optical properties in the Arctic supports the notion that the sites presented here measure a variety of aerosol populations, which also experience different removal mechanisms. A robust conclusion from the climatologies presented is that the Arctic cannot be treated as one common and uniform environment, but rather is a region with ample spatio-temporal variability in aerosols. This notion is important in considering the design or aerosol monitoring networks in the region, and is important for informing climate models to better represent short-lived aerosol climate forcers in order to yield more accurate climate predictions for the Arctic. [ABSTRACT FROM AUTHOR]

This paper presents the light scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, located mainly in Europe. The data include particle light scattering (σ sp) and hemispheric backscattering (σbsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). A large range of ssp was observed across the network. Low ssp values were on average measured in Nordic and Baltic countries and in Western Europe whereas the highest σsp were measured at regional sites in eastern and central Europe. In these regional areas the SAE was also high indicating the predominance of fine-mode particles. On average, the SAE was lower in the Nordic and Baltic, western and southern countries suggesting a lower fraction of fine-mode particle compared to central and eastern Europe. An increasing gradient of ssp was observed when moving from mountain to regional and to urban sites. Conversely, the mass-independent SAE and g parameters did not show the same gradient. At all sites, both SAE and g varied greatly with aerosol particle loading. The lowest values of g were always observed under low ssp indicating a larger contribution from particles in the smaller accumulation mode. Then, g steeply increased with increasing ssp indicating a progressive shift of the particle size distribution toward the larger end of the accumulation mode. Under periods of high particle mass concentrations, the variation of g was less pronounced whereas the SAE increased or decreased suggesting changes mostly in the coarse aerosol particles mode rather than in the fine mode. The station placement seemed to be the main parameter affecting the intra-annual variability. At mountain sites, higher σsp was measured in summer mainly because of the enhanced boundary layer influence. Conversely, less horizontal and vertical dispersion in winter led to higher σsp at all low altitude sites in central and eastern Europe compared to summer. On average, these sites also showed SAE maxima in summer (and correspondingly g minima). Large intra-annual variability of SAE and g was observed also at Nordic and Baltic countries due to seasonal-dependent transport of different air masses to these remote sites. Statistically significant decreasing trends of σsp were observed at 5 out of 13 stations included in trend analyses. The total reductions of ssp were consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe. [ABSTRACT FROM AUTHOR]