Abstract. We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ∼1-42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EU-CAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and Correspondence to: H. E. Manninen (hanna.manninen@helsinki.fi) relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, Published by Copernicus Publications on behalf of the European Geosciences Union. 7908H. E. Manninen et al.: EUCAARI ion spectrometer measurements nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1-30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.

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Multiyear surface PM10 measurements performed on Crete Island, Greece, have been used in conjunction with satellite (Total Ozone Mapping Spectrometer (TOMS)) and ground‐based remote sensing measurements (Aerosol Robotic Network (AERONET)) to enhance our understanding of the evolution of mineral dust events over the eastern Mediterranean. An analysis of southerly air masses at altitudes of 1000 and 3000 m over a 5 year period (2000–2005), showed that dust can potentially arrive over Crete, either simultaneously in the lower free troposphere and inside the boundary layer (vertical extended transport (VET)) or initially into the free troposphere with the heavier particles gradually being scavenged inside the boundary layer (free troposphere transport (FTT)). Both pathways present significant seasonal variations but on an annual basis contribute almost equally to the dust transport in the area. During VET the aerosol index (AI) derived from TOMS was significantly correlated with surface PM10, and in general AI was found to be adequate for the characterization of dust loadings over the eastern Mediterranean on a climatological basis. A significant covariance between PM10 and AOT was observed during VET as well, indicating that AOT levels from AERONET may be estimated by PM10 levels at the surface. Surface measurements are thus crucial for the validation of remote sensing measurements and hence are a powerful tool for the investigation of the impact of aerosols on climate.

Abstract. 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.

Abstract. The aerosol chemical composition in air masses affected by wildfires from the Greek islands of Chios, Euboea and Andros, the Dalmatian Coast and Sicily, during late summer of 2012 was characterized at the remote background site of Finokalia, Crete. Air masses were transported several hundreds of kilometers, arriving at the measurement station after approximately half a day of transport, mostly during nighttime. The chemical composition of the particulate matter was studied by different high-temporal-resolution instruments, including an aerosol chemical speciation monitor (ACSM) and a seven-wavelength aethalometer. Despite the large distance from emission and long atmospheric processing, a clear biomass-burning organic aerosol (BBOA) profile containing characteristic markers is derived from BC (black carbon) measurements and positive matrix factorization (PMF) analysis of the ACSM organic mass spectra. The ratio of fresh to aged BBOA decreases with increasing atmospheric processing time and BBOA components appear to be converted to oxygenated organic aerosol (OOA). Given that the smoke was mainly transported overnight, it appears that the processing can take place in the dark. These results show that a significant fraction of the BBOA loses its characteristic AMS (aerosol mass spectrometry) signature and is transformed to OOA in less than a day. This implies that biomass burning can contribute almost half of the organic aerosol mass in the area during periods with significant fire influence.

Total and dissolved inorganic phosphorus (IP) was measured in both rainwater and aerosol samples collected from two remote coastal areas: on the island of Crete (Greece) and at Erdemli (Turkey). Particle size distributions of P, as well as total deposition were also measured. Wet and dry deposition of dissolved inorganic phosphorus (DIP) from Crete are compared with simultaneously obtained dissolved inorganic nitrogen (DIN) and with productivity data from the literature. Our results indicate that (1) in both wet and dry deposition, the DIN/DIP molar ratio ranges between 63 and 349, exceeding by a factor of up to 22 the N/P ratio observed in seawater (ranging from 25 to 28) and (2) atmospheric deposition of DIP could reasonably account for a significant part of the new production (up to 38%) observed during the summer and autumn period (i.e., when water stratification is at its maximum).

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