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1.
Summertime particulate matter and its composition in Greece
M. A. Tsiflikiotou, E. Kostenidou, D. K. Papanastasiou, D. Patoulias, Pavlos Zarmpas, D. Paraskevopoulou, E. Diapouli, Christos Kaltsonoudis, Kalliopi Florou, Iasonas Stavroulas, 2019, original scientific article

Abstract: During the summer of 2012 a coordinated field campaign was conducted in multiple locations in Greece in order to characterize the ambient particulate matter (PM) levels, its chemical composition and the contribution of the regional and local sources. PM1, PM2.5 and PM10 samples were collected simultaneously at seven different sites in Greece: an urban and a suburban station in Patras, a suburban station in Thessaloniki, a suburban and an urban background station in Athens, a rural background station at the Navarino Environmental Observatory (NEO) in southwestern Peloponnese and a remote background site at Finokalia in the northeastern part of Crete. The sites were selected to facilitate the estimation of the contribution of the local emission sources and long range transport. Sulfate and organics were the major PM1 components in all sites suggesting that high sulfate levels still remain in parts of Europe. The photochemistry of the Eastern Mediterranean can convert rapidly the emitted sulphur dioxide to sulfate. Our analysis indicated significant sulfate production over the area, with high sulfate levels, especially in the remote site of Finokalia, associated with air masses that had passed over Turkey. There was high regional secondary organic aerosol production dominating organic aerosol levels even in a major city like Athens. High organic aerosol levels were associated with air masses that had crossed the Balkans with a significant biogenic component. The average PM2.5 concentration ranged from 13 to 18 μg m−3 in the different sites. There were unexpected significant gradients in the concentrations of secondary aerosol components in length scales of a few hundred kilometers. The low concentrations of measured PM2.5 nitrate are mostly organic nitrates and supermicrometer nitrate associated with sea-salt and dust. Dust was a significant PM10 constituent in all areas and was quite variable in space showing the importance of the local sources.
Keywords: PM2.5, sulfate aerosol, secondary inorganic aerosol, secondary organic aerosol, Greece
Published in RUNG: 13.05.2024; Views: 306; Downloads: 0
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2.
Sources and processes that control the submicron organic aerosol composition in an urban Mediterranean environment (Athens) : a high temporal-resolution chemical composition measurement study
Iasonas Stavroulas, Aikaterini Bougiatioti, Georgios Grivas, D. Paraskevopoulou, M. Tsagkaraki, Pavlos Zarmpas, Eleni Liakakou, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2019, original scientific article

Abstract: 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.
Keywords: ACSM, organic aerosol, PMF, source apportionment
Published in RUNG: 13.05.2024; Views: 289; Downloads: 2
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3.
Yearlong measurements of monoterpenes and isoprene in a Mediterranean city (Athens) : natural vs anthropogenic origin
Anastasia Panopoulou, Eleni Liakakou, Stéphane Sauvage, Valérie Gros, Nadine Locoge, Iasonas Stavroulas, Bernard Bonsang, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2020, original scientific article

Abstract: Monoterpenes and isoprene are important constituents of the volatile organic compounds (VOCs) due to their high reactivity and participation in ozone and secondary aerosol formation. The current work focuses on the results of a 13-month intensive campaign of high resolution time-resolved measurements of these compounds, at an urban background site in Athens, Greece. On an annual basis, monoterpenes (α-pinene and limonene) surpass the isoprene levels presenting mean values of 0.70 ± 0.83 μg m−3, 0.33 ± 0.78 μg m−3 and 0.19 ± 0.36 μg m−3, respectively. The large standard deviation highlights the significant diurnal and day-to-day variability. Isoprene presents a typical seasonal cycle, with a photochemically induced summer-time maximum. Enhanced noon levels are observed during summer, whereas a morning peak in the autumn and winter profiles occurs, despite the generally low levels encountered during these seasons. The monoterpenes deviate from the expected biogenic pattern, presenting higher mean levels during the cold period and a night-to-early morning enhancement strongly related to local anthropogenic tracers such as BC, CO, NO or toluene, as well as increased levels under wind speeds lower than 3 m s−1. Estimations of the anthropogenic and biogenic fractions based on the enhancement ratios of α-pinene versus a variety of anthropogenic tracers, demonstrate a clear dominance of the anthropogenic sources in all studied seasons. Simultaneously, the biogenic fraction increased during summer relative to winter by more than 10 times. Both α-pinene and limonene significantly contribute to locally formed secondary organic aerosol (SOA), determined by means of an ACSM, accounting for at least 22% and 13% of their levels in summer and winter respectively. Additionally, monoterpenes and isoprene contribute 6% to the observed oxidants levels (O3 + NOx) during summer.
Keywords: volatile organic compounds, biogenic compounds, monoterpenes, isoprene, Athens
Published in RUNG: 10.05.2024; Views: 321; Downloads: 2
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4.
5.
Long-term brown carbon spectral characteristics in a Mediterranean city (Athens)
Eleni Liakakou, Dimitris G. Kaskaoutis, Georgios Grivas, Iasonas Stavroulas, M. Tsagkaraki, D. Paraskevopoulou, Aikaterini Bougiatioti, Umesh Chandra Dumka, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2020, original scientific article

Abstract: This study analyses 4-years of continuous 7-λ Aethalometer (AE-33) measurements in an urban-background environment of Athens, to resolve the spectral absorption coefficients (babs) for black carbon (BC) and brown carbon (BrC). An important BrC contribution (23.7 ± 11.6%) to the total babs at 370 nm is estimated for the period May 2015–April 2019, characterized by a remarkable seasonality with winter maximum (33.5 ± 13.6%) and summer minimum (18.5 ± 8.1%), while at longer wavelengths the BrC contribution is significantly reduced (6.8 ± 3.6% at 660 nm). The wavelength dependence of the total babs gives an annual-mean AAE370-880 of 1.31, with higher values in winter night-time. The BrC absorption and its contribution to babs presents a large increase reaching up to 39.1 ± 13.6% during winter nights (370 nm), suggesting residential wood burning (RWB) emissions as a dominant source for BrC. This is supported by strong correlations of the BrC absorption with OC, EC, the fragment ion m/z 60 derived from ACSM and PMF-analyzed organic fractions related to biomass burning (e.g. BBOA). In contrast, BrC absorption decreases significantly during daytime as well as in the warm period, reaching to a minimum during the early-afternoon hours in all seasons due to photo-chemical degradation. Estimated secondary BrC absorption is practically evident only during winter night-time, implying the fast oxidation of BrC species from RWB emissions. Changes in mixing-layer height do not significantly affect the BrC absorption in winter, while they play a major role in summer.
Keywords: spectral aerosol absorption, brown carbon, wood burning, organic aerosols, chemical composition, Athens
Published in RUNG: 10.05.2024; Views: 302; Downloads: 1
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6.
Online chemical characterization and sources of submicron aerosol in the major mediterranean port city of Piraeus, Greece
Iasonas Stavroulas, Georgios Grivas, Eleni Liakakou, Panayiotis Kalkavouras, Aikaterini Bougiatioti, Dimitris G. Kaskaoutis, Maria Lianou, Kyriaki Papoutsidaki, M. Tsagkaraki, Evangelos Gerasopoulos, Pavlos Zarmpas, Nikolaos Mihalopoulos, 2021, original scientific article

Abstract: 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.
Keywords: Athens, harbor, shipping emissions, PM1, chemical speciation, organic aerosol, black carbon, ACSM, aethalometer, PMF
Published in RUNG: 10.05.2024; Views: 292; Downloads: 2
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7.
Absorption enhancement of black carbon particles in a Mediterranean city and countryside : effect of particulate matter chemistry, ageing and trend analysis
Jesús Yus-Díez, Marta Via, Andrés Alastuey, Angeliki Karanasiou, Maria Cruz Minguillon, Noemí Perez, Xavier Querol, Cristina Reche, Matic Ivančič, Martin Rigler, 2022, original scientific article

Abstract: Abstract. Black carbon (BC) is recognized as the most important warming agent among atmospheric aerosol particles. The absorption efficiency of pure BC is rather well-known, nevertheless the mixing of BC with other aerosol particles can enhance the BC light absorption efficiency, thus directly affecting Earth's radiative balance. The effects on climate of the BC absorption enhancement due to the mixing with these aerosols are not yet well constrained because these effects depend on the availability of material for mixing with BC, thus creating regional variations. Here we present the mass absorption cross-section (MAC) and absorption enhancement of BC particles (Eabs), at different wavelengths (from 370 to 880 nm for online measurements and at 637 nm for offline measurements) measured at two sites in the western Mediterranean, namely Barcelona (BCN; urban background) and Montseny (MSY; regional background). The Eabs values ranged between 1.24 and 1.51 at the urban station, depending on the season and wavelength used as well as on the pure BC MAC used as a reference. The largest contribution to Eabs was due to the internal mixing of BC particles with other aerosol compounds, on average between a 91 % and a 100 % at 370 and 880 nm, respectively. Additionally, 14.5 % and 4.6 % of the total enhancement at the short ultraviolet (UV) wavelength (370 nm) was due to externally mixed brown carbon (BrC) particles during the cold and the warm period, respectively. On average, at the MSY station, a higher Eabs value was observed (1.83 at 637 nm) compared to BCN (1.37 at 637 nm), which was associated with the higher fraction of organic aerosols (OA) available for BC coating at the regional station, as denoted by the higher organic carbon to elemental carbon (OC:EC) ratio observed at MSY compared to BCN. At both BCN and MSY, Eabs showed an exponential increase with the amount of non-refractory (NR) material available for coating (RNR-PM). The Eabs at 637 nm at the MSY regional station reached values up to 3 during episodes with high RNR-PM, whereas in BCN, Eabs kept values lower than 2 due to the lower relative amount of coating materials measured at BCN compared to MSY. The main sources of OA influencing Eabs throughout the year were hydrocarbon OA (HOA) and cooking-related OA (COA), i.e. primary OA (POA) from traffic and cooking emissions, respectively, at both 370 and 880 nm. At the short UV wavelength (370 nm), a strong contribution to Eabs from biomass burning OA (BBOA) and less oxidized oxygenated OA (LO-OOA) sources was observed in the colder period. Moreover, we found an increase of Eabs with the ageing state of the particles, especially during the colder period. This increase of Eabs with particle ageing was associated with a larger relative amount of secondary OA (SOA) compared to POA. The availability of a long dataset at both stations from offline measurements enabled a decade-long trend analysis of Eabs at 637 nm, that showed statistically significant (s.s.) positive trends of Eabs during the warmer months at the MSY station. This s.s. positive trend in MSY mirrored the observed increase of the OC:EC ratio over time. Moreover, in BCN during the COVID-19 lockdown period in spring 2020 we observed a sharp increase of Eabs due to the observed sharp increase of the OC:EC ratio. Our results show similar values of Eabs to those found in the literature for similar background stations.
Keywords: black carbomn, coating, organic aerosol, light absorption
Published in RUNG: 10.05.2024; Views: 324; Downloads: 2
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8.
Development and evaluation of an improved offline aerosol mass spectrometry technique
Christina Vasilakopoulou, Kalliopi Florou, Christos Kaltsonoudis, Iasonas Stavroulas, Nikolaos Mihalopoulos, Spyros N. Pandis, 2023, original scientific article

Abstract: Abstract. The offline aerosol mass spectrometry technique is a useful tool for the source apportionment of organic aerosol (OA) in areas and periods during which an aerosol mass spectrometer (AMS) is not available. However, the technique is based on the extraction of aerosol samples in water, while several atmospheric OA components are partially or fully insoluble in water. In this work an improved offline technique was developed and evaluated in an effort to capture most of the partially soluble and insoluble organic aerosol material, reducing significantly the uncertainty of the corresponding source apportionment. A major advantage of the proposed approach is that no corrections are needed for the offline analysis to account for the limited water solubility of some OA components. The improved offline AMS analysis was tested in three campaigns: two during winter and one during summer. Collocated online AMS measurements were performed for the evaluation of the offline method. Source apportionment analysis was performed separately for the online and the offline measurements using positive matrix factorization (PMF). The PMF results showed that the fractional contribution of each factor to the total OA differed between the online and the offline PMF results by less than 15 %. The differences in the AMS spectra of the factors of the two approaches could be significant, suggesting that the use of factor profiles from the literature in the offline analysis may lead to complications. Part of the good agreement between the online and the offline PMF results is due to the ability of the improved offline AMS technique to capture a bigger part of the OA, including insoluble organic material. This was evident by the significant fraction of submicrometer suspended insoluble particles present in the water extract and by the reduced insoluble material on the filters after the extraction process. More than half of the elemental carbon (EC) was on average missing from the filters after the water extraction. Significant EC concentrations were measured in the produced aerosol that was used as input to the AMS during the offline analysis.
Keywords: organic aerosol, receptor modeling, offline PMF, Greece
Published in RUNG: 10.05.2024; Views: 274; Downloads: 2
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9.
10.
The effect of the averaging period for PMF analysis of aerosol mass spectrometer measurements during offline applications
Christina Vasilakopoulou, Iasonas Stavroulas, Nikolaos Mihalopoulos, Spyros N. Pandis, 2022, original scientific article

Abstract: Offline aerosol mass spectrometer (AMS) measurements can provide valuable information about ambient organic aerosols in areas and periods in which online AMS measurements are not available. However, these offline measurements have a low temporal resolution, as they are based on filter samples usually collected over 24 h. In this study, we examine whether and how this low time resolution affects source apportionment results. We used a five-month period (November 2016–March 2017) of online measurements in Athens, Greece, and performed positive matrix factorization (PMF) analysis to both the original dataset, which consists of 30 min measurements, and to time averages from 1 up to 24 h. The 30 min results indicated that five factors were able to represent the ambient organic aerosol (OA): a biomass burning organic aerosol factor (BBOA), which contributed 16 % of the total OA; hydrocarbon-like OA (HOA) (29 %); cooking OA (COA) (20 %); more-oxygenated OA (MO-OOA) (18 %); and less-oxygenated OA (LO-OOA) (17 %). Use of the daily averages resulted in estimated average contributions that were within 8 % of the total OA compared with the high-resolution analysis for the five-month period. The most important difference was for the BBOA contribution, which was overestimated (25 % for low resolution versus 17 % for high resolution) when daily averages were used. The estimated secondary OA varied from 35 % to 28 % when the averaging interval varied between 30 min and 24 h. The high-resolution results are expected to be more accurate, both because they are based on much larger datasets and because they are based on additional information about the temporal source variability. The error for the low-resolution analysis was much higher for individual days, and its results for high-concentration days in particular are quite uncertain. The low-resolution analysis introduces errors in the determined AMS profiles for the BBOA and LO-OOA factors but determines the rest relatively accurately (theta angle around 10∘ or less).
Keywords: AMS, offline PMF, ACSM, organic aerosols
Published in RUNG: 10.05.2024; Views: 335; Downloads: 3
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