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The intricacy of the chemical components of atmospheric aerosols causes distinct or even converse climate-forcing effects. Investigating the interannual trends and relative contributions (RCs) of component-segregated aerosol optical depth (AOD) regionally and over land enhances comprehension of the climatic and environmental implications of natural and anthropogenic aerosols. Here, we utilized multiyear (2007–2019) AOD data from the Copernicus Atmosphere Monitoring Service (CAMS) reanalysis to examine the trends in aerosol component loadings and identify the dominant components driving the total AOD (TAOD). Independent validations using ground-based Aerosol Robotic Network measurements revealed marked spatial consistency worldwide (Pearson correlation coefficient: 0.87, root mean square error: 0.08, mean fractional error: 34.04%, and index of agreement: 0.94), whereas the fractional gross error of 23.31% indicated widespread overestimation of CAMS AOD, particularly in the United States and Western Europe (WEU). Over the study period, the CAMS reanalysis featured notable reduction in sulfate (SO 4) in East China (EC), the Eastern United States (EUS), WEU, and Australia, together with considerable reduction in dust in EC, which played a substantial role in the trend of decline in TAOD globally. Conversely, positive trends in component-segregated AOD in South Asia (SA) (SO 4 , black carbon (BC), and organic matter (OM)) and Siberia (BC and OM) counteracted those reductions. Furthermore, we isolated the RCs of the components to regional trends in TAOD, which revealed that in EC (SA), anthropogenic aerosols, particularly SO 4 and OM, overwhelmingly contributed to the prevailing decrease (increase) in TAOD, with RCs of 31% and 45% (43.6% and 54.4%), respectively. We found that SO 4 was the predominant component controlling the decline in TAOD in EUS and WEU, although the rise in natural aerosols (sea salt) mitigated the impact of this reduction. These findings provide valuable insights into the roles of anthropogenic and natural aerosols in the interannual variation in AOD. • CAMS AOD has robust agreement with AERONET measurements. • Isolated aerosol components drive distinct dominance across dependent regions. • SO 4 and OM variations mainly account for the trend in TAOD in EC and SA. • Upward trends of SS counteract the TAOD reductions in EUS and WEU. [ABSTRACT FROM AUTHOR]

The Arctic is warming two to three times faster than the global average, and the role of aerosols is not well constrained. Aerosol number concentrations can be very low in remote environments, rendering local cloud radiative properties highly sensitive to available aerosol. The composition and sources of the climate-relevant aerosols, affecting Arctic cloud formation and altering their microphysics, remain largely elusive due to a lack of harmonized concurrent multi-component, multi-site, and multi-season observations. Here, we present a dataset on the overall chemical composition and seasonal variability of the Arctic total particulate matter (with a size cut at 10 μ m, PM _10 , or without any size cut) at eight observatories representing all Arctic sectors. Our holistic observational approach includes the Russian Arctic, a significant emission source area with less dedicated aerosol monitoring, and extends beyond the more traditionally studied summer period and black carbon/sulfate or fine-mode pollutants. The major airborne Arctic PM components in terms of dry mass are sea salt, secondary (non-sea-salt, nss) sulfate, and organic aerosol (OA), with minor contributions from elemental carbon (EC) and ammonium. We observe substantial spatiotemporal variability in component ratios, such as EC/OA, ammonium/nss-sulfate and OA/nss-sulfate, and fractional contributions to PM. When combined with component-specific back-trajectory analysis to identify marine or terrestrial origins, as well as the companion study by Moschos et al 2022 Nat. Geosci. focusing on OA, the composition analysis provides policy-guiding observational insights into sector-based differences in natural and anthropogenic Arctic aerosol sources. In this regard, we first reveal major source regions of inner-Arctic sea salt, biogenic sulfate, and natural organics, and highlight an underappreciated wintertime source of primary carbonaceous aerosols (EC and OA) in West Siberia, potentially associated with the oil and gas sector. The presented dataset can assist in reducing uncertainties in modelling pan-Arctic aerosol-climate interactions, as the major contributors to yearly aerosol mass can be constrained. These models can then be used to predict the future evolution of individual inner-Arctic atmospheric PM components in light of current and emerging pollution mitigation measures and improved region-specific emission inventories.

We carried out simulations with predefined and simulated aerosol distributions in order to investigate the improvement in the forecasting capabilities of an operational weather forecast model by the use of an improved aerosol representation. This study focuses on convective cumulus clouds developing after the passage of a cold front on 25 April 2008 over Germany. The northerly flow after the cold front leads to increased sea salt aerosol concentrations compared to prefrontal conditions. High aerosol number concentrations are simulated in the interactive scenario representing typically polluted conditions. Nevertheless, due to the presence of sea salt particles, effective radii of cloud droplets reach values typical of pristine clouds (between 7 µm and 13 µm) at the same time. Compared to the predefined continental and maritime aerosol scenarios, the simulated aerosol distribution leads to a significant change in cloud properties such as cloud droplet radii and number concentrations. Averaged over the domain covered by the convective cumuli clouds, we found a systematic decrease in precipitation with increasing aerosol number concentrations. Differences in cloud cover, short wave radiation and cloud top heights are buffered by systematic differences in precipitation and the related diabatic effects. Comparisons with measured precipitation show good agreement for the interactive aerosol scenario as well as for the extreme maritime aerosol scenario.

Long distance dispersal (LDD) of airborne aerosol of foot-and-mouth disease (FMD) virus was extensively modeled in the literature. Most studies modeled this aerosol in simplistic approach as a passive tracer, neglecting physical and biological mechanisms that affect bio-aerosols such as the FMD aerosol. This approach was justified either because under persistent wind these mechanisms lower the extant of downwind hazard or on the grounds that the effect of some of the physical mechanisms on particles as small as the FMD particles (0.015–20 μm) is supposed to be negligible compared to the effect of atmospheric turbulence. Even when the FMD aerosol was treated as aerosol, it was assumed that it is monodisperse, i.e., all its particles are of the same size. The aim of the study is to examine whether these simplistic approaches are indeed justified when dealing with LDD of a bio-aerosol under actual atmospheric conditions. In order to do so, the influence of a more realistic modeling of the FMD aerosol as a polydisperse aerosol was compared to passive tracer and to monodisperse aerosol. The comparison refers to a case of a widespread FMD outbreak that occurred in 2012 in Egypt. This outbreak involved the emergence of a new serotype in Egypt, SAT2 and concern was raised that this serotype will advance further to Asia and Europe. Israel is located on the land bridge between Africa, Asia and Europe, and shares a long desert border with Egypt as well as a long Mediterranean shore adjacent to Egypt's shore. This unique location as well as the fact that Israel does not have any cattle trade with its neighboring countries make Israel an interesting test case for the examination of the necessary conditions for the long distance dispersal (LDD) of a new FMD strains from Africa to Europe. The analysis in this study shows that under quasi-stationary wind conditions modeling FMD dispersal as a passive tracer results in a significantly longer hazard distance. Under non-stationary conditions this modeling assumption results in an under-estimation of the hazard distance in comparison to the results of polydisperse aerosol. In these conditions modeling the FMD dispersal as a monodisperse aerosol results in similar under-estimation. The implications of such under-estimation may be severe because it may lead authorities in a threatened area to refrain from taking the necessary protective measures. Therefore, the modeling of the FMD aerosol as a polydisperse aerosol is preferable, leading to realistic estimation both under non-stationary and stationary wind conditions. [ABSTRACT FROM AUTHOR]

Natural aerosols define a preindustrial baseline state from which the magnitude of anthropogenic aerosol effects on climate are calculated and are a major component of the large uncertainty in anthropogenic aerosol-cloud radiative forcing. This uncertainty would be reduced if aerosol environments unperturbed by air pollution could be studied in the present-day atmosphere, but the pervasiveness of air pollution makes identification of unperturbed regions difficult. Here, we use global model simulations to define unperturbed aerosol regions in terms of two measures that compare 1750 and 2000 conditions-the number of days with similar aerosol concentrations and the similarity of the aerosol response to perturbations in model processes and emissions. The analysis shows that the aerosol system in many present-day environments looks and behaves like it did in the preindustrial era. On a global annual mean, unperturbed aerosol regions cover 12% of the Earth (16% of the ocean surface and 2% of the land surface). There is a strong seasonal variation in unperturbed regions of between 4% in August and 27% in January, with the most persistent conditions occurring over the equatorial Pacific. About 90% of unperturbed regions occur in the Southern Hemisphere, but in the Northern Hemisphere, unperturbed conditions are transient and spatially patchy. In cloudy regions with a radiative forcing relative to 1750, model results suggest that unperturbed aerosol conditions could still occur on a small number of days per month. However, these environments are mostly in the Southern Hemisphere, potentially limiting the usefulness in reducing Northern Hemisphere forcing uncertainty. [ABSTRACT FROM AUTHOR]

We carried out simulations with predefined and simulated aerosol distributions in order to investigate the improvement in the forecasting capabilities of an operational weather forecast model by the use of an improved aerosol representation. This study focuses on convective cumulus clouds developing after the passage of a cold front on 25 April 2008 over Germany. The northerly flow after the cold front leads to increased sea salt aerosol concentrations compared to prefrontal conditions. High aerosol number concentrations are simulated in the interactive scenario representing typically polluted conditions. Nevertheless, due to the presence of sea salt particles, effective radii of cloud droplets reach values typical of pristine clouds (between 7 µm and 13 µm) at the same time. Compared to the predefined continental and maritime aerosol scenarios, the simulated aerosol distribution leads to a significant change in cloud properties such as cloud droplet radii and number concentrations. Averaged over the domain covered by the convective cumuli clouds, we found a systematic decrease in precipitation with increasing aerosol number concentrations. Differences in cloud cover, short wave radiation and cloud top heights are buffered by systematic differences in precipitation and the related diabatic effects. Comparisons with measured precipitation show good agreement for the interactive aerosol scenario as well as for the extreme maritime aerosol scenario. [ABSTRACT FROM AUTHOR]

Abstract: A ten-month field study aimed to determine the contribution of natural events (i.e. sea-salt and mineral dust events) to urban PM concentration was carried out at six sampling sites in Central Italy (Lazio region). Four indicators have been used to identify natural events during the period of the study. The first one is constituted by the ratio between number of particles in the coarse to the accumulation mode. It is simple, cheap, and the information are given in quasi-real time, but the nature of the event (sea-salt or mineral dust) is not detectable. The second indicator relies on the chemical analysis of the collected PM by X-ray fluorescence (XRF) and allows a robust identification of sea-salt and crustal components. The third one is based on diagnostic ratios of elemental fractions: Mgextractable/Tiresidue for sea-salt and Tiresidue/Sbresidue for mineral dust. It requires skilled staff but it is most accurate and sensible. The last indicator, constructed on the basis of natural radioactivity data, is not diagnostic for the nature of the event but it is able to estimate the increase in PM concentration with respect to the expected concentration in the absence of natural events. The relevance of natural events and the variations in PM concentration and composition during the study are discussed. The joined use of the four indicators allowed the identification of about 20 natural PM episodes. In general, sea-salt aerosol events did not cause exceedance of the daily EU limit value for PM10. Saharan dust events, instead, were in most cases responsible for the exceedance of the limit value at all stations. [Copyright &y& Elsevier]

Natural aerosols define a pre-industrial baseline state from which the magnitude of anthropogenic aerosol effects on climate are calculated and are a major component of the large uncertainty in anthropogenic aerosol-cloud radiative forcing. This uncertainty would be reduced if aerosol environments unperturbed by air pollution could be studied in the present-day atmosphere, but the pervasiveness of air pollution makes identification of unperturbed regions difficult. This study uses global model simulations to show where aerosol concentrations have remained similar between 1750 and 2000. Four suitable measurement stations are then identified in regions with a pristine-like aerosol state. [ABSTRACT FROM AUTHOR]