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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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Measuring the spatial variability of black carbon in Athens during wintertime
Georgios Grivas, Iasonas Stavroulas, Eleni Liakakou, Dimitris G. Kaskaoutis, Aikaterini Bougiatioti, D. Paraskevopoulou, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2019, original scientific article

Abstract: 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.
Keywords: mobile measurements, microaethalometer, Athens, mapping, traffic, biomass burning
Published in RUNG: 10.05.2024; Views: 299; Downloads: 3
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Long-term variability, source apportionment and spectral properties of black carbon at an urban background site in Athens, Greece
Eleni Liakakou, Iasonas Stavroulas, Dimitris G. Kaskaoutis, Georgios Grivas, D. Paraskevopoulou, Umesh Chandra Dumka, M. Tsagkaraki, Aikaterini Bougiatioti, K. Oikonomou, J. Sciare, 2020, original scientific article

Abstract: This study aims to delineate the characteristics of Black Carbon (BC) in the atmosphere over Athens, Greece, using 4-year (May 2015–April 2019) Aethalometer (AE-33) measurements. The average BC concentration is 1.9 ± 2.5 μg m−3 (ranging from 0.1 to 32.7 μg m−3; hourly values), with a well-defined seasonality from 1.3 ± 1.1 μg m−3 in summer to 3.0 ± 4.0 μg m−3 in winter. Pronounced morning and evening/night peaks are found in the BC concentrations in winter, while during the rest of the seasons, this diurnal cycle appears to flatten out, with the exception of the morning traffic peak. On an annual basis, the biomass-burning fraction (BB%) of BC accounts for 22 ± 12%, while the fossil-fuel combustion (BCff) component (traffic emissions and domestic heating) dominates during summer (83%) and in the morning hours. BCwb exhibits higher contribution in winter (32%), especially during the night hours (39%). BC levels are effectively reduced by precipitation, while they significantly build-up for wind speeds <3 m s−1 and mixing-layer height (MLH) < 500 m. Normalizing the BC diurnal course by the MLH variations on a seasonal basis reveals that the residential wood-burning emissions are mostly responsible for the large BC increase during winter nights, whereas the low BC levels during daytime in the warm season are mainly attributed to dilution into a deeper MLH. BCwb is highly correlated with other BB tracers during winter nights (e.g. levoglucosan, non-sea-salt-K+, m/z 60 fragment), as well as with the fine fraction (PM2.5) OC and EC. The Delta-C, which represents the spectral dependence of BC as the absorption difference between 370 and 880 nm, is analyzed for the first time in Athens. It exhibits a pronounced seasonality with maximum values in winter night-time, and it appears as a valid qualitative marker for wood combustion.
Keywords: black carbon, wood burning, source apportionment, mixing layer, biomass burning tracers, Athens
Published in RUNG: 10.05.2024; Views: 294; Downloads: 1
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On the regional aspects of new particle formation in the Eastern Mediterranean : a comparative study between a background and an urban site based on long term observations
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Georgios Grivas, Iasonas Stavroulas, Nikos Kalivitis, Eleni Liakakou, Evangelos Gerasopoulos, Christodoulos Pilinis, Nikolaos Mihalopoulos, 2020, original scientific article

Abstract: Atmospheric new particle formation (NPF) is an important source of submicron particles. In remote background environments where local sources are scarce such processes may impact significantly on climate-relevant parameters. On the other hand, in urban environments, newly-formed particles are adding up to submicron particles emitted from primary sources. As the exact mechanism which triggers NPF still remains elusive, so are the circumstances for simultaneous occurrence of such events in two different environments (urban vs. regional background). In this study, concurrent number size distribution measurements were conducted in the urban environment of Athens and at the regional background site of Finokalia, Crete, located 340 km away and spanning a 2-year period. It occurred that the relative frequency of NPF was similar at both sites (around 20%), with a higher frequency during spring and autumn at the urban site, while at the background site most events took place in August and December, during the studied period. There were 35 event days when NPF took place at both sites simultaneously, all associated with air masses originating from the Northern sector, indicating the presence of regional events in the extended geographical area and characterized by low condensation sink (CS). By comparing the common with the non-common class I NPF episodes, we conclude that the conditions applying when regional NPF events with growth are observed in the same day at the surface level of both areas, are: (i) lower CS, (ii) higher SO2 concentrations, (iii) lower RH, and finally (iv) lower formation and growth rates than those observed during the site-specific and more rapidly evolving NPF events.
Keywords: NPF, Athens, Eastern Mediterranean, particle number concentrations, size distributions, concurrent regional events
Published in RUNG: 10.05.2024; Views: 303; Downloads: 0
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Integrating in situ measurements and city scale modelling to assess the COVID–19 lockdown effects on emissions and air quality in Athens, Greece
Georgios Grivas, Eleni Athanasopoulou, Anastasia Kakouri, Jennifer Bailey, Eleni Liakakou, Iasonas Stavroulas, Panayiotis Kalkavouras, Aikaterini Bougiatioti, Dimitris G. Kaskaoutis, Michel Ramonet, 2020, original scientific article

Abstract: 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.
Keywords: pandemic, urban air pollution, traffic, chemical transport model, TAPM, mapping
Published in RUNG: 10.05.2024; Views: 333; Downloads: 2
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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: 301; Downloads: 1
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Field evaluation of low-cost PM sensors (Purple Air PA-II) under variable urban air quality conditions, in Greece
Iasonas Stavroulas, Georgios Grivas, Panagiotis Michalopoulos, Eleni Liakakou, Aikaterini Bougiatioti, Panayiotis Kalkavouras, Kyriaki Maria Fameli, Nikolaos Hatzianastassiou, Nikolaos Mihalopoulos, Evangelos Gerasopoulos, 2020, original scientific article

Abstract: 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.
Keywords: particulate matter, PM2.5, air quality, low-cost sensors, optical particle counter
Published in RUNG: 10.05.2024; Views: 281; Downloads: 3
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Carbonaceous aerosols in contrasting atmospheric environments in Greek cities : evaluation of the EC-tracer methods for secondary organic carbon estimation
Dimitris G. Kaskaoutis, Georgios Grivas, Christina Theodosi, M. Tsagkaraki, D. Paraskevopoulou, Iasonas Stavroulas, Eleni Liakakou, Antonis Gkikas, Nikolaos Hatzianastassiou, Cheng Wu, 2020, original scientific article

Abstract: This study examines the carbonaceous-aerosol characteristics at three contrasting urban environments in Greece (Ioannina, Athens, and Heraklion), on the basis of 12 h sampling during winter (January to February 2013), aiming to explore the inter-site differences in atmospheric composition and carbonaceous-aerosol characteristics and sources. The winter-average organic carbon (OC) and elemental carbon (EC) concentrations in Ioannina were found to be 28.50 and 4.33 µg m−3, respectively, much higher than those in Heraklion (3.86 µg m−3 for OC and 2.29 µg m−3 for EC) and Athens (7.63 µg m−3 for OC and 2.44 µg m−3 for EC). The winter OC/EC ratio in Ioannina (6.53) was found to be almost three times that in Heraklion (2.03), indicating a larger impact of wood combustion, especially during the night, whereas in Heraklion, emissions from biomass burning were found to be less intense. Estimations of primary and secondary organic carbon (POC and SOC) using the EC-tracer method, and specifically its minimum R-squared (MRS) variant, revealed large differences between the sites, with a prevalence of POC (67–80%) in Ioannina and Athens and with a larger SOC fraction (53%) in Heraklion. SOC estimates were also obtained using the 5% and 25% percentiles of the OC/EC data to determine the (OC/EC)pri, leading to results contrasting to the MRS approach in Ioannina (70–74% for SOC). Although the MRS method provides generally more robust results, it may significantly underestimate SOC levels in environments highly burdened by biomass burning, as the fast-oxidized semi-volatile OC associated with combustion sources is classified in POC. Further analysis in Athens revealed that the difference in SOC estimates between the 5% percentile and MRS methods coincided with the semi-volatile oxygenated organic aerosol as quantified by aerosol mass spectrometry. Finally, the OC/Kbb+ ratio was used as tracer for decomposition of the POC into fossil-fuel and biomass-burning components, indicating the prevalence of biomass-burning POC, especially in Ioannina (77%).
Keywords: carbonaceous aerosols, inorganic species, POC-SOC estimation, biomass burning, MRS method, Greece
Published in RUNG: 10.05.2024; Views: 265; Downloads: 3
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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: 291; Downloads: 2
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In situ identification of aerosol types in Athens, Greece, based on long-term optical and on online chemical characterization
Dimitris G. Kaskaoutis, Georgios Grivas, Iasonas Stavroulas, Eleni Liakakou, Umesh Chandra Dumka, Konstantinos Dimitriou, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2021, original scientific article

Abstract: Absorption Ångström Exponent (AAE) and Scattering Ångström Exponent (SAE) values, derived from aethalometer and nephelometer measurements during a period of 3 years at an urban background site in Athens, are combined for the first aerosol type classification using in situ measurements in the eastern Mediterranean. In addition, single scattering albedo (SSA) and its wavelength dependence (dSSA), as well as the chemical composition of fine aerosols and precursor gases from collocated measurements, are utilized to provide further insights on the optical-chemical characterization and related sources of seven identified aerosol types. Urban aerosols are mostly characterized as Black Carbon (BC)-dominated (76.3%), representing a background atmosphere where fossil-fuel combustion is dominant throughout the year, while 14.3% of the cases correspond to the mixed Brown Carbon (BrC)-BC type, with a higher frequency in winter. The BrC type is associated with the highest scattering and absorption coefficients during winter nights, representing the impact from residential wood-burning emissions. Dust mixed with urban pollution (1.2%) and large particles mixed with BC (5.3%) have a higher frequency in spring. Furthermore, aging processes and BC coating with organic and inorganic species with weak spectral absorption (AAE<1) account for 2.2%, with a differentiation between small and large particles. dSSA is recognized as a useful parameter for aerosol characterization, since fine aerosols are associated with negative dSSA values. The identified aerosol types are examined on a seasonal, monthly, hourly basis and by potential source areas, as well as in comparison with fine-aerosol chemical composition and apportioned organic aerosol source contributions, in an attempt to explore the linkage between optical, physical and chemical aerosol properties. Chemical analysis indicates high organic fraction (60–68%) for the BrC and BrC/BC, 20–30% larger compared to other types. The results are essential for parametrization in chemical transport models and for reducing the uncertainty in the assessment of aerosol radiative effects.
Keywords: aerosol types, classification, AAE, SAE, dSSA, chemical composition, sources, Athens
Published in RUNG: 10.05.2024; Views: 273; Downloads: 2
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