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Opis: Submicron aerosol chemical composition was studied during a year-long period (26 July 2016–31 July 2017) and two wintertime intensive campaigns (18 December 2013–21 February 2014 and 23 December 2015–17 February 2016), at a central site in Athens, Greece, using an Aerosol Chemical Speciation Monitor (ACSM). Concurrent measurements included a particle-into-liquid sampler (PILS-IC), a scanning mobility particle sizer (SMPS), an AE-33 Aethalometer, and ion chromatography analysis on 24 or 12 h filter samples. The aim of the study was to characterize the seasonal variability of the main submicron aerosol constituents and decipher the sources of organic aerosol (OA). Organics were found to contribute almost half of the submicron mass, with 30 min resolution concentrations during wintertime reaching up to 200 µg m−3. During winter (all three campaigns combined), primary sources contributed about 33 % of the organic fraction, and comprised biomass burning (10 %), fossil fuel combustion (13 %), and cooking (10 %), while the remaining 67 % was attributed to secondary aerosol. The semi-volatile component of the oxidized organic aerosol (SV-OOA; 22 %) was found to be clearly linked to combustion sources, in particular biomass burning; part of the very oxidized, low-volatility component (LV-OOA; 44 %) could also be attributed to the oxidation of emissions from these primary combustion sources. These results, based on the combined contribution of biomass burning organic aerosol (BBOA) and SV-OOA, indicate the importance of increased biomass burning in the urban environment of Athens as a result of the economic recession. During summer, when concentrations of fine aerosols are considerably lower, more than 80 % of the organic fraction is attributed to secondary aerosol (SV-OOA 31 % and LV-OOA 53 %). In contrast to winter, SV-OOA appears to result from a well-mixed type of aerosol that is linked to fast photochemical processes and the oxidation of primary traffic and biogenic emissions. Finally, LV-OOA presents a more regional character in summer, owing to the oxidation of OA over the period of a few days.
Ključne besede: ACSM, organic aerosol, PMF, source apportionment
Objavljeno v RUNG: 13.05.2024; Ogledov: 11; Prenosov: 0
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Opis: 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.
Ključne besede: regional NPF, CCN, cloud droplets, Eastern Mediterranean, regional background
Objavljeno v RUNG: 13.05.2024; Ogledov: 11; Prenosov: 0
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Opis: One-year measurements (October 2016–September 2017) of aerosol optical properties in the Athens urban environment were analyzed; for closure purposes, the results were supported by data of chemical composition of the non-refractory submicron aerosol fraction acquired with an Aerosol Chemical Speciation Monitor (ACSM). Both the spectral scattering (bsca) and absorption (babs) coefficients exhibit a pronounced annual variability with higher values (63.6 Mm–1 at 550 nm and 41.0 Mm–1 at 520 nm, respectively) in winter, due to domestic heating releasing increased carbonaceous emissions and the shallow mixing layer trapping aerosols near the surface. Much lower values (33.5 Mm–1 and 22.9 Mm–1 for bsca and babs, respectively) are found during summer, indicating rather aged aerosols from regional sources. The estimations of the dry spectral single scattering albedo (SSA), scattering (SAE) and absorption (AAE) Ångström exponents focus on the seasonality of the urban aerosols. The high SAE (~2.0) and low SSA (0.62 ± 0.11) values throughout the year indicate the dominance of fine-absorbing aerosols from fossil-fuel combustion, while the high AAE (~1.5) in winter suggests enhanced presence of biomass-burning aerosols. Pronounced morning and late evening/night peaks are found in both bsca and babs during winter, coinciding with the morning traffic rush hour and increased residential wood burning in the evening, while in the other seasons, the diurnal patterns flatten out. The wind speed strongly affects the aerosol loading and properties in winter, since for winds below 3 m s–1, a high increase in bsca and babs is observed, consistent with low dilution processes and hazy/smoggy conditions. Our closure experiments indicate a good agreement (R2 = 0.91, slope = 1.08) between the reconstructed and measured bsca values and reveal that organic matter contributes about half of the sub-micron mass in winter, followed by sulfate (~40%) and nitrate (10%, only in winter) aerosols.
Ključne besede: urban aerosols, light scattering, absorption, chemical species, wood burning, Athens
Objavljeno v RUNG: 10.05.2024; Ogledov: 68; Prenosov: 0
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Opis: A first assessment of the spatial variability of ambient black carbon (BC) concentrations in the Greater Area of Athens (GAA) was carried out during an intensive wintertime campaign, when ambient levels are exacerbated by increased biomass burning for residential heating. Short-term daytime BC measurements were conducted at 50 sites (traffic and urban/suburban/regional background) and on-road along 12 routes. Daytime measurements were adjusted based on BC concentrations continuously monitored at a reference site. Indicative nighttime BC ambient concentrations were also measured at several residences across the area. Daytime BC concentrations recorded an average of 2.3 μg m-3 with considerable between-site variability. Concentrations at traffic sites were significantly higher (43% on average), compared with the rest of the sites. Varying levels were observed between background site subtypes, with concentrations at urban background sites (located near the center of Athens and the port of Piraeus) being 34% and 114% higher, on average, than at suburban and regional background sites, respectively. The traffic intensity at the nearest road and the population and built density in the surrounding area of sites were recognized as important factors controlling BC levels. On-road concentration measurements (5.4 μg m-3 on average) enabled the identification of hot-spots in the road network, with peak levels encountered along motorways (13.5 μg m-3 on average). Nighttime measurements demonstrated that wintertime BC pollution, enhanced by residential biomass burning for heating, affects the entire Athens basin. The reference site in central Athens was found to be representative of the temporal variability for daytime and nighttime BC concentrations at background locations.
Ključne besede: mobile measurements, microaethalometer, Athens, mapping, traffic, biomass burning
Objavljeno v RUNG: 10.05.2024; Ogledov: 84; Prenosov: 0
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Opis: Atmospheric new particle formation (NPF) is a common phenomenon all over the world. In this study we present the longest time series of NPF records in the eastern Mediterranean region by analyzing 10 years of aerosol number size distribution data obtained with a mobility particle sizer. The measurements were performed at the Finokalia environmental research station on Crete, Greece, during the period June 2008–June 2018. We found that NPF took place on 27 % of the available days, undefined days were 23 % and non-event days 50 %. NPF is more frequent in April and May probably due to the terrestrial biogenic activity and is less frequent in August. Throughout the period under study, nucleation was observed also during the night. Nucleation mode particles had the highest concentration in winter and early spring, mainly because of the minimum sinks, and their average contribution to the total particle number concentration was 8 %. Nucleation mode particle concentrations were low outside periods of active NPF and growth, so there are hardly any other local sources of sub-25 nm particles. Additional atmospheric ion size distribution data simultaneously collected for more than 2 years were also analyzed. Classification of NPF events based on ion spectrometer measurements differed from the corresponding classification based on a mobility spectrometer, possibly indicating a different representation of local and regional NPF events between these two measurement data sets. We used the MALTE-Box model for simulating a case study of NPF in the eastern Mediterranean region. Monoterpenes contributing to NPF can explain a large fraction of the observed NPF events according to our model simulations. However the adjusted parameterization resulting from our sensitivity tests was significantly different from the initial one that had been determined for the boreal environment.
Ključne besede: particles, number size distributions, new particle formation, regional background, SMPS, Eastern Mediterannean
Objavljeno v RUNG: 10.05.2024; Ogledov: 74; Prenosov: 0
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