Abstract. Particle number concentration and size distribution are important variables needed to constrain the role of atmospheric particles in the Earth radiation budget, both directly and indirectly through CCN activation. They are also linked to regulated variables such as particle mass (PM) and therefore of interest to air quality studies. However, data on their long-term variability are scarce, in particular at high altitudes. In this paper, we investigate the diurnal and seasonal variability of the aerosol total number concentration and size distribution at the puy de Dôme research station (France, 1465 m a.s.l.). We report a variability of aerosol particle total number concentration measured over a five-year (2003-2007) period for particles larger than 10 nm and aerosol size distributions between 10 and 500 nm over a two-year period (January 2006 to December 2007). Concentrations show a strong seasonality with maxima during summer and minima during winter. A diurnal variation is also observed with maxima between 12:00 and 18:00 UTC. At night (00:00-06:00 UTC), the median hourly total concentration varies from 600 to 800 cm −3 during winter and from 1700 to 2200 cm −3 during summer. During the day (08:00-18:00 UTC), the concentration is in the range of 700 to 1400 cm −3 during winter and of 2500 to 3500 cm −3 during summer. An averaged size distribution of particles (10-500 nm) was calculated for each season. The total aerosol number concentrations are dominated by the Aitken mode integral concentrations, which drive most of the winter to summer total concentrations increase. The night to day increase in dominated by the nucleation mode integral number concentration. Because the site is located in the free troposphere Correspondence to: K. Sellegri (k.sellegri@opgc.univ-bpclermont.fr) only a fraction of the time, in particular at night and during the winter season, we have subsequently analyzed the variability for nighttime and free tropospheric (FT)/residual layer (RL) conditions only. We show that a seasonal variability is still observed for these FT/RL conditions. The FT/RL seasonal variation is due to both seasonal changes in the air mass origin from winter to summer and enhanced concentrations of particles in the residual layer/free troposphere in summer. The later observation can be explained by higher emissions intensity in the boundary layer, stronger exchanges between the boundary layer and the free troposphere as well as enhanced photochemical processes. Finally, aerosols mean size distributions are calculated for a given air mass type (marine/continental/regional) according to the season for the specific conditions of the residual layer/free troposphere. The seasonal variability in aerosol sources seems to be predominant over the continent compared to the seasonal variation of marine aerosol sources. These results are of regional relevance and can be used to constrain chemical-transport models over Western Europe.

Abstract. Aerosol–cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set – ready to be used for model validation – of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles > 20 nm) across the range of 0.1 to 1.0 % supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, κ, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2–0.3). We performed closure studies based on κ–Köhler theory to predict CCN number concentrations. The ratio of predicted to measured CCN concentrations is between 0.87 and 1.4 for five different types of κ. The temporal variability is also well captured, with Pearson correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to better characterise ACI and their radiative forcing. But long-term comprehensive aerosol particle characterisations are labour intensive and costly. Hence, we recommend operating “migrating-CCNCs” to conduct collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can only be calculated based on continued particle number size distribution information and greater spatial coverage of long-term measurements can be achieved.

Atmospheric Chemistry and PhysicsNew particle formation and ultrafine charged aerosol climatology at a high altitude site in the Alps (Jungfraujoch, 3580 m a.s.l., Switzerland) Abstract. We investigate the formation and growth of charged aerosols clusters at Jungfraujoch, in the Swiss Alps (3580 m a.s.l.), the highest altitude site of the European EU-CAARI project intensive campaign. Charged particles and clusters (0.5 − 1.8 nm) were measured from April 2008 to April 2009 and allowed the detection of nucleation events in this very specific environment (presence of free tropospheric air and clouds). We found that the naturally charged aerosol concentrations, which are dominated by the cluster size class, shows a strong diurnal pattern likely linked to valley breezes transporting surface layer ion precursors, presumably radon. Cosmic rays were found not to be the major ion source at the measurement site. However, at night, when air masses are more representative of free tropospheric conditions, we found that the cluster concentrations are still high. The charged aerosol size distribution and concentration are strongly influenced by the presence of clouds at the station. Clouds should be taken into account when deriving high altitude nucleation statistics. New particle formation occurs on average 17.5% of the measurement period and shows a weak seasonality with a minimum of frequency during winter, but this seasonality is enhanced when the data set is screened forCorrespondence to: J. Boulon (j.boulon@opgc.univ-bpclermont.fr) periods when the atmospheric station is out of clouds. The role of ions in the nucleation process was investigated and we found that the ion-mediated nucleation explains 22.3% of the particle formation. The NPF events frequency is correlated with UV radiation but not with calculated H 2 SO 4 concentrations, suggesting that other compounds such as organic vapors are involved in the nucleation and subsequently growth process. In fact, NPF events frequency also surprisingly increases with the condensational sink (CS), suggesting that at Jungfraujoch, the presence of condensing vapours probably coupled with high CS are driving the occurrence of NPF events. A strong link to the air mass path was also pointed out and events were observed to be frequently occurring in Eastern European air masses, which present the highest condensational sink. In these air masses, pre-existing cluster concentrations are more than three time larger than in other air masses during event days, and no new clusters formation is observed, contrarily to what is happening in other air mass types.

Abstract. In this work we present an analysis of the occurrence of nucleation events during more than three years of measurements at two different rural altitude sites, the puy de Dôme research station (1465 m a.s.l.) and the Opme station (660 m a.s.l.), central France. The collected database is a unique combination of scanning mobility particle sizer (10-400 nm), air ion spectrometers (from 0.8 to 42 nm for NTP-conditions), and, neutral clusters and air ion spectrometers (from 0.8 to 42 nm for NTP-conditions) measurements at these two different altitudes nearly located research stations, from February 2007 to June 2010. The seasonality of the frequency of nucleation events was studied at the puy de Dôme station and maximum of events frequency was found during early spring and early autumn. During the measurement period, neither the particle formation rates (J 2 = 1.382 ± 0.195 s −1 ) nor the growth rates (ḠR 1.3−20 nm = 6.20 ± 0.12 nm h −1 ) differ from one site to the other on average. Hovewer, we found that, on 437 sampling days in common to the two sites, the nucleation frequency was higher at the puy de Dôme station (35.9 %, 157 days) than at the low elevation station of Opme (20.8 %, 91 days). LIDAR measurements and the evolution of the potential equivalent temperature revealed that the nucleation could be triggered either (i) within the whole low tropospheric column at the same time from the planetary boundary layer to the top of the interface layer (29.2 %, 47 events), (ii) above the planetary boundary layer upper limit (43.5 %, 70 events), and (iii) at low altitude and then transported, conserving dynamic and properties, at high altitude (24.8 %, 40 events). This is the first time that the vertical extent of nucleation can be studied over a long observational period, allowing for a rigorous statistical analysis of the occurrence of nucleation over the whole lower troposphere. This work Correspondence to: J. Boulon (j.boulon@opgc.univ-bpclermont.fr) highlights the fact that nucleation can occur over a large vertical extent, at least the whole low tropospheric column, and also the fact that it occurs twice as frequently as actually detected in the planetary boundary layer. The role of sulfuric acid and ions in the nucleation process was investigated at the altitude station and no correlation was found between nucleation events and the estimated sulfuric acid concentrations. However, the contribution of ion-induced nucleation was found to be relatively high (12.49 ± 2.03 % of the total nucleation rate).