The chemical composition of aerosols has been determined in 30 size-resolved samples collected using a Berner lowpressure impactor during two campaigns conducted at a coastal site in the Eastern Mediterranean in July 2000 and in January 2001. Sulfate ðSO 4 accounting for up to 38% of the total fine mass and up to 65% of the total ionic mass during both seasons. On the other hand, nitrate ðNO À 3 Þ; chloride ðCl À Þ; sodium ðNa þ Þ and calcium ðCa 2þ Þ were identified as the main components of the super-micron mode. The ionic organic compounds (including carboxylic, dicarboxylic and ketoacids) were distributed both between sub-micron and super-micron mode, indicating origin from both gas-to-particle conversion and heterogeneous reactions on pre-existing particles. The total water-soluble ionic organic fraction although accounting for only up to 1-2% of both coarse ð> 1 mmÞ and fine ðo1 mmÞ mass fractions, accounts for up to 15% of the organic carbon (OC) mass. NH þ 4 was found to be significantly correlated to non-sea-salt sulfate (nss-SO 2À 4 ), with NH þ 4 =nss-SO 2À 4 molar ratio ranging from 1.3 to 2, the lower ratio associated with transport from the W sector. Chloride depletion was observed mainly during summer and was significantly correlated with NO À 3 concentrations, with a molar ratio of 0.80, indicating the reaction of nitric acid with NaCl as the main source of NO À 3 in the area. Total ionic mass both in the fine and coarse fraction accounted for up to 58% of the total aerosol mass during both seasons. An attempt to perform a mass closure analysis indicates that nss-SO 2À 4 and organic carbon are the main components of the fine fraction with relative contributions of 38% and 16%, respectively. In the coarse fraction, the ionic part accounts for 58%, mineral dust for 32% and the remaining non-identified part of 12-30% could be partly attributed to water. r

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.

Abstract. Long-term (5-year) measurements of Elemental Carbon (EC) and Organic Carbon (OC) in bulk aerosols are presented here for the first time in the Mediterranean Basin (Crete Island). A multi-analytical approach (including thermal, optical, and thermo-optical techniques) was applied for these EC and OC measurements. Light absorbing dust aerosols were shown to poorly contribute (+12% on a yearly average) to light absorption coefficient (b abs ) measurements performed by an optical method (aethalometer). Long-range transport of agricultural waste burning from European countries surrounding the Black Sea was shown for each year during two periods (March-April and July-September). The contribution of biomass burning to the concentrations of EC and OC was shown to be rather small (20 and 14%, respectively, on a yearly basis), although this contribution could be much higher on a monthly basis and showed important seasonal and interannual variability. By removing the biomass burning influence, our data revealed an important seasonal variation of OC, with an increase by almost a factor of two for the spring months of May and June, whereas BC was found to be quite stable throughout the year. Preliminary measurements of Water Soluble Organic Carbon (WSOC) have shown that the monthly mean WSOC/OC ratio remains stable throughout the year (0.45±0.12), suggesting that the partitioning between water soluble and water insoluble organic matter is not significantly affected by biomass burning and secondary organic aerosol (SOA) formation. A chemical mass closure performed in the fine mode (Aerodynamic Diameter, A.D.<1.5µm) showed that the mass contribution of organic matter (POM) was found to be essentially invariable during the year (monthly average of 26±5%).

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Abstract. Organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and main ions were measured in a total of 1510 PM 2.5 daily aerosol samples collected from May 2008 to April 2013 in Athens, Greece. OC and EC concentrations were 2.1 ± 1.3 µg m −3 and 0.54 ± 0.39 µg m −3 , accounting for 11 ± 3 % and 3 ± 1 % of PM 2.5 mass, respectively, with an average OC / EC ratio of 4.7 ± 3.1. Significant correlation was found between OC and EC during the whole period, indicating emissions by common primary sources on a regional scale. WSOC concentration ranged from 0.03 to 10.6 µg m −3 , with an average of 1.5 ± 0.9 µg m −3 . By considering the Finokalia (Crete) station as a reference, it was estimated that, during the warm season in Athens, 67 ± 7 % of emitted OC and 53 ± 12 % of emitted EC is regional, while, during cold months, the regional contribution of OC is only 33 ± 7 % and of EC 29 ± 8 %. Furthermore, secondary organic carbon (SOC) was calculated for the warm period of the year (April to October). The estimated SOC constituted about 75 ± 6 % of PM 2.5 organic carbon in Athens, highlighting significant aging processes on a regional scale. In the period 2011-2013 and during wintertime, an increase in OC and EC levels was observed, attributed to an increase in wood burning for domestic heating due to the economic crisis.