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Particle water (liquid water content, LWC) and aerosol pH are important parameters of the aerosol phase, affecting heterogeneous chemistry and bioavailability of nutrients that profoundly impact cloud formation, atmospheric composition, and atmospheric fluxes of nutrients to ecosystems. Few measurements of in situ LWC and pH, however, exist in the published literature. Using concurrent measurements of aerosol chemical composition, cloud condensation nuclei activity, and tandem light scattering coefficients, the particle water mass concentrations associated with the aerosol inorganic (Winorg) and organic (Worg) components are determined for measurements conducted at the Finokalia atmospheric observation station in the eastern Mediterranean between June and November 2012. These data are interpreted using the ISORROPIA-II thermodynamic model to predict the pH of aerosols originating from the various sources that influence air quality in the region. On average, closure between predicted aerosol water and that determined by comparison of ambient with dry light scattering coefficients was achieved to within 8 % (slope  =  0.92, R2  =  0.8, n  =  5201 points). Based on the scattering measurements, a parameterization is also derived, capable of reproducing the hygroscopic growth factor (f(RH)) within 15 % of the measured values. The highest aerosol water concentrations are observed during nighttime, when relative humidity is highest and the collapse of the boundary layer increases the aerosol concentration. A significant diurnal variability is found for Worg with morning and afternoon average mass concentrations being 10–15 times lower than nighttime concentrations, thus rendering Winorg the main form of particle water during daytime. The average value of total aerosol water was 2.19 ± 1.75 µg m−3, contributing on average up to 33 % of the total submicron mass concentration. Average aerosol water associated with organics, Worg, was equal to 0.56 ± 0.37 µg m−3; thus, organics contributed about 27.5 % to the total aerosol water, mostly during early morning, late evening, and nighttime hours.The aerosol was found to be highly acidic with calculated aerosol pH varying from 0.5 to 2.8 throughout the study period. Biomass burning aerosol presented the highest values of pH in the submicron fraction and the lowest values in total water mass concentration. The low pH values observed in the submicron mode and independently of air mass origin could increase nutrient availability and especially P solubility, which is the nutrient limiting sea water productivity of the eastern Mediterranean.

Significance Atmospheric secondary organic aerosol has substantial impacts on climate, air quality, and human health. However, the formation mechanisms of secondary organic aerosol remain uncertain, especially on how anthropogenic pollutants (from human activities) control aerosol formation from biogenic volatile organic compounds (emitted by vegetation) and the magnitude of anthropogenic influences. Although possible mechanisms have been proposed based on laboratories studies, a coherent understanding of anthropogenic−biogenic interactions in ambient environments has not emerged. Here, we provide direct observational evidence that secondary organic aerosol formed from biogenic isoprene and monoterpenes is greatly mediated by anthropogenic SO ₂ and NO ₓ emissions based on integrated ambient measurements and laboratory studies. Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate and human health. The extent to which human activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence on the magnitude of anthropogenic influence on biogenic SOA formation based on comprehensive ambient measurements in the southeastern United States (US). Multiple high-time-resolution mass spectrometry organic aerosol measurements were made during different seasons at various locations, including urban and rural sites in the greater Atlanta area and Centreville in rural Alabama. Our results provide a quantitative understanding of the roles of anthropogenic SO ₂ and NO ₓ in ambient SOA formation. We show that isoprene-derived SOA is directly mediated by the abundance of sulfate, instead of the particle water content and/or particle acidity as suggested by prior laboratory studies. Anthropogenic NO ₓ is shown to enhance nighttime SOA formation via nitrate radical oxidation of monoterpenes, resulting in the formation of condensable organic nitrates. Together, anthropogenic sulfate and NO ₓ can mediate 43–70% of total measured organic aerosol (29–49% of submicron particulate matter, PM ₁) in the southeastern US during summer. These measurements imply that future reduction in SO ₂ and NO ₓ emissions can considerably reduce the SOA burden in the southeastern US. Updating current modeling frameworks with these observational constraints will also lead to more accurate treatment of aerosol formation for regions with substantial anthropogenic−biogenic interactions and consequently improve air quality and climate simulations.

This study investigates the concentration, cloud condensation nuclei (CCN) activity and hygroscopic properties of particles influenced by biomass burning in the eastern Mediterranean and their impacts on cloud droplet formation. Air masses sampled were subject to a range of atmospheric processing (several hours up to 3 days). Values of the hygroscopicity parameter, κ, were derived from CCN measurements and a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA). An Aerosol Chemical Speciation Monitor (ACSM) was also used to determine the chemical composition and mass concentration of non-refractory components of the submicron aerosol fraction. During fire events, the increased organic content (and lower inorganic fraction) of the aerosol decreases the values of κ, for all particle sizes. Particle sizes smaller than 80 nm exhibited considerable chemical dispersion (where hygroscopicity varied up to 100 % for particles of same size); larger particles, however, exhibited considerably less dispersion owing to the effects of condensational growth and cloud processing. ACSM measurements indicate that the bulk composition reflects the hygroscopicity and chemical nature of the largest particles (having a diameter of  ∼  100 nm at dry conditions) sampled. Based on positive matrix factorization (PMF) analysis of the organic ACSM spectra, CCN concentrations follow a similar trend as the biomass-burning organic aerosol (BBOA) component, with the former being enhanced between 65 and 150 % (for supersaturations ranging between 0.2 and 0.7 %) with the arrival of the smoke plumes. Using multilinear regression of the PMF factors (BBOA, OOA-BB and OOA) and the observed hygroscopicity parameter, the inferred hygroscopicity of the oxygenated organic aerosol components is determined. We find that the transformation of freshly emitted biomass burning (BBOA) to more oxidized organic aerosol (OOA-BB) can result in a 2-fold increase of the inferred organic hygroscopicity; about 10 % of the total aerosol hygroscopicity is related to the two biomass-burning components (BBOA and OOA-BB), which in turn contribute almost 35 % to the fine-particle organic water of the aerosol. Observation-derived calculations of the cloud droplet concentrations that develop for typical boundary layer cloud conditions suggest that biomass burning increases droplet number, on average by 8.5 %. The strongly sublinear response of clouds to biomass-burning (BB) influences is a result of strong competition of CCN for water vapor, which results in very low maximum supersaturation (0.08 % on average). Attributing droplet number variations to the total aerosol number and the chemical composition variations shows that the importance of chemical composition increases with distance, contributing up to 25 % of the total droplet variability. Therefore, although BB may strongly elevate CCN numbers, the impact on droplet number is limited by water vapor availability and depends on the aerosol particle concentration levels associated with the background.

Recent advances in particle sensor technologies have led to an increased development and utilization of low-cost, compact, particulate matter (PM) monitors. These devices can be deployed in dense monitoring networks, enabling an improved characterization of the spatiotemporal variability in ambient levels and exposure. However, the reliability of their measurements is an important prerequisite, necessitating rigorous performance evaluation and calibration in comparison to reference-grade instrumentation. In this study, field evaluation of Purple Air PA-II devices (low-cost PM sensors) is performed in two urban environments and across three seasons in Greece, in comparison to different types of reference instruments. Measurements were conducted in Athens (the largest city in Greece with nearly four-million inhabitants) for five months spanning over the summer of 2019 and winter/spring of 2020 and in Ioannina, a medium-sized city in northwestern Greece (100,000 inhabitants) during winter/spring 2019–2020. The PM2.5 sensor output correlates strongly with reference measurements (R2 = 0.87 against a beta attenuation monitor and R2 = 0.98 against an optical reference-grade monitor). Deviations in the sensor-reference agreement are identified as mainly related to elevated coarse particle concentrations and high ambient relative humidity. Simple and multiple regression models are tested to compensate for these biases, drastically improving the sensor’s response. Large decreases in sensor error are observed after implementation of models, leading to mean absolute percentage errors of 0.18 and 0.12 for the Athens and Ioannina datasets, respectively. Overall, a quality-controlled and robustly evaluated low-cost network can be an integral component for air quality monitoring in a smart city. Case studies are presented along this line, where a network of PA-II devices is used to monitor the air quality deterioration during a peri-urban forest fire event affecting the area of Athens and during extreme wintertime smog events in Ioannina, related to wood burning for residential heating.

A significant fraction of atmospheric particles that serve as cloud condensation nuclei (CCN) are thought to originate from the condensational growth of new particle formation (NPF) from the gas phase. Here, 7 years of continuous aerosol and meteorological measurements (June 2008 to May 2015) at a remote background site of the eastern Mediterranean were recorded and analyzed to assess the impact of NPF (of 162 episodes identified) on CCN and cloud droplet number concentration (CDNC) formation in the region. A new metric is introduced to quantitatively determine the initiation and duration of the influence of NPF on the CCN spectrum. NPF days were found to increase CCN concentrations (from 0.10 % to 1.00 % supersaturation) between 29 % and 77 %. Enhanced CCN concentrations from NPF are mostly observed, as expected, under low preexisting particle concentrations and occur in the afternoon, relatively later in the winter and autumn than in the summer. Potential impacts of NPF on cloud formation were quantified by introducing the observed aerosol size distributions and chemical composition into an established cloud droplet parameterization. We find that the supersaturations that develop are very low (ranging between 0.03 % and 0.27 %) for typical boundary layer dynamics (σw ∼0.3 m s−1) and NPF is found to enhance CDNC by a modest 13 %. This considerable contrast between CCN and CDNC response is in part from the different supersaturation levels considered, but also because supersaturation drops from increasing CCN because of water vapor competition effects during the process of droplet formation. The low cloud supersaturation further delays the appearance of NPF impacts on CDNC to clouds formed in the late evening and nighttime – which has important implications for the extent and types of indirect effects induced by NPF events. An analysis based on CCN concentrations using prescribed supersaturation can provide very different, even misleading, conclusions and should therefore be avoided. The proposed approach here offers a simple, yet highly effective way for a more realistic impact assessment of NPF events on cloud formation.

The Eastern Mediterranean, and even more the Middle East, is an area highly influenced by mineral dust emissions. Since the World Health Organization has a daily PM2.5 24-h guideline limit of 25 μg m−3, it is obvious that the monitoring of ambient particulate matter in such environments is crucial. The topography of the city of Amman—with downtown being the lowest point between seven hills, thus limiting ventilation, as well as enhanced emissions from traffic congestion, plenty of restaurants (grilling) and coffee shops offering water pipe smoking that requires coal burning—further exacerbates the air quality problem, and denotes that exposure is much higher than predicted based on ambient air quality monitoring at stationary sites. [...]in Jordan, a large part of the population, especially in cities, is exposed to poor air quality which exceeds WHO standards. Aerosol particles are both primarily emitted in the atmosphere and secondarily formed from atmospheric processing of organic and inorganic precursors, with the secondary organic aerosol (SOA) constituting a substantial fraction of the mass of submicron aerosol in populated areas around the world; this contributes to poor air quality and premature mortality [9].

The lockdown measures implemented worldwide to slow the spread of the COVID–19 pandemic have allowed for a unique real-world experiment, regarding the impacts of drastic emission cutbacks on urban air quality. In this study we assess the effects of a 7-week (23 March–10 May 2020) lockdown in the Greater Area of Athens, coupling in situ observations with estimations from a meteorology-atmospheric chemistry model. Measurements in central Athens during the lockdown were compared with levels during the pre- and post-lockdown 3-week periods and with respective levels in the four previous years. We examined regulatory pollutants as well as CO2, black carbon (BC) and source-specific BC components. Models were run for pre-lockdown and lockdown periods, under baseline and reduced-emissions scenarios. The in-situ results indicate mean concentration reductions of 30–35% for traffic-related pollutants in Athens (NO2, CO, BC from fossil fuel combustion), compared to the pre-lockdown period. A large reduction (53%) was observed also for the urban CO2 enhancement while the reduction for PM2.5 was subtler (18%). Significant reductions were also observed when comparing the 2020 lockdown period with past years. However, levels rebounded immediately following the lift of the general lockdown. The decrease in measured NO2 concentrations was reproduced by the implementation of the city scale model, under a realistic reduced-emissions scenario for the lockdown period, anchored at a 46% decline of road transport activity. The model permitted the assessment of air quality improvements on a spatial scale, indicating that NO2 mean concentration reductions in areas of the Athens basin reached up to 50%. The findings suggest a potential for local traffic management strategies to reduce ambient exposure and to minimize exceedances of air quality standards for primary pollutants.

Atmospheric new particle formation (NPF) events taking place over large distances between locations, featuring similar characteristics, have been the focus of studies during the last decade. The exact mechanism which triggers NPF still remains indefinable, so are the circumstances under which simultaneous occurrence of such events take place in different environments, let alone in environments which are parted by over 1200 km. In this study, concurrent number size distribution measurements were conducted in the urban environments of Athens (Greece) and Amman (Jordan) as well as the regional background site of Finokalia, Crete, all located within a distance of almost 1300 km for a 6-month period (February–July 2017). During the study period Athens and Finokalia had similar occurrence of NPF (around 20%), while the occurrence in Amman was double. When focusing on the dynamic characteristics at each site, it occurs that formation and growth rates at Amman are similar to those at Finokalia, while lower values in Athens can be ascribed to a higher pre-existing particle number at this urban site. By comparing common NPF events there are 5 concomitant days between all three sites, highly related to air masses origin. Additionally, for another 19 days NPF takes place simultaneously between Finokalia and Amman, which also share common meteorological characteristics, adding to a total of 60% out of 41 NPF events observed at Finokalia, also simultaneously occurring in Amman.

Port cities are affected by a wide array of emissions, including those from the shipping, road transport, and residential sectors; therefore, the characterization and apportionment of such sources in a high temporal resolution is crucial. This study presents measurements of fine aerosol chemical composition in Piraeus, one of the largest European ports, during two monthly periods (winter vs. summer) in 2018–2019, using online instrumentation (Aerosol Chemical Speciation Monitor—ACSM, 7-λ aethalometer). PMF source apportionment was performed on the ACSM mass spectra to quantify organic aerosol (OA) components, while equivalent black carbon (BC) was decomposed to its fossil fuel combustion and biomass burning (BB) fractions. The combined traffic, shipping and, especially, residential emissions led to considerably elevated submicron aerosol levels (22.8 μg m−3) in winter, which frequently became episodic late at night under stagnant conditions. Carbonaceous compounds comprised the major portion of this submicron aerosol in winter, with mean OA and BC contributions of 61% (13.9 μg m−3) and 16% (3.7 μg m−3), respectively. The contribution of BB to BC concentrations was considerable and spatially uniform. OA related to BB emissions (fresh and processed) and hydrocarbon-like OA (from vehicular traffic and port-related fossil fuel emissions including shipping) accounted for 37% and 30% of OA, respectively. In summer, the average PM1 concentration was significantly lower (14.8 μg m−3) and less variable, especially for the components associated with secondary aerosols (such as OA and sulfate). The effect of the port sector was evident in summer and maintained BC concentrations at high levels (2.8 μg m−3), despite the absence of BB and improved atmospheric dispersion. Oxygenated components yielded over 70% of OA in summer, with the more oxidized secondary component of regional origin being dominant (41%) despite the intensity of local sources, in the Piraeus environment. In general, with respect to local sources that can be the target of mitigation policies, this work highlights the importance of port-related activities but also reveals the extensive wintertime impact of residential wood burning. While a separation of the BB source is feasible, more research is needed on how to disentangle the short-term effects of different fossil-fuel combustion sources.

This study provides an overview of the atmospheric drivers of climate change over Greece (Eastern Mediterranean), focusing on greenhouse gases (GHG: carbon dioxide, CO2; methane, CH4; etc.). CO2 in Greece is mostly produced by energy production, followed by transport, construction, and industry. Waste management is the largest anthropogenic source of methane, accounting for 47% of total CH4 emissions, surpassing emissions from the agricultural sector in 2017, while the energy sector accounts for the remaining 10.5%. In situ simultaneous observations of GHG concentrations in Greece conducted at three sites with different topologies (urban background; Athens, regional background; Finokalia and free troposphere; and Helmos) during the last 5 years (2019–2023) showed increasing trends of the order of 2.2 ppm·yr−1 and ~15 ppb·yr−1 for CO2 and CH4, respectively, in line with the global trends. These increasing trends were found from both ground-based and satellite-based remote-sensing observations. Finally, during the lockdown period due to the COVID-19 global pandemic, a 58% reduction in CO2 levels was observed in the urban background site of Athens after subtracting the regional background levels from Finokalia, while the respective reduction in CH4 was of only the order of 15%, highlighting differences in emission sources.