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The FHH adsorption activation theory has become a popular way to characterize the CCN activation properties of insoluble aerosols. Based on the combination of the two parameter Frenkel-Halsey-Hill multilayer adsorption model and the Kelvin equation, the FHH adsorption activation theory can in principle be used to predict CCN activation provided that the two FHH parameters are determined from an experimental adsorption isotherm. However, CCN experiments have shown that the experimental critical supersaturations are in general considerably lower than those predicted using the adsorption isotherms. A few years ago, we suggested that a better correspondence between theory and experiments might be obtained if physical surface heterogeneity – i.e. the influence of pores, steps, kinks etc. – was accounted for by using the surface fractal dimension (Laaksonen et al., Sci. Rep. 6, 2554, 2016). Our results were promising but with rather large uncertainty limits, due in part to the fact that we made use of literature data from a number of different sources. Here, we test the theoretical approach using several different aerosol species, including metal oxides and minerals. Importantly, we use the same samples in the CCN experiments and in the water adsorption and surface fractal dimension measurements, which decreases the uncertainty limits of our results compared to the initial study. This permits us to make firm conclusions on the impact of CCN surface properties on the closure between adsorption-based predictions and CCN activation experiments., The 28th IUGG General Assembly (IUGG2023) (Berlin 2023)

The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nanoparticle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e., in conditions in which neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.5 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.5 nm. At this size, more than 90 % of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.5 nm. Observations at Hyytiälä, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy., published version, peerReviewed

The northern Eurasian regions and Arctic Ocean will very likely undergo substantial changes during the next decades. The Arctic-boreal natural environments play a crucial role in the global climate via albedo change, carbon sources and sinks as well as atmospheric aerosol production from biogenic volatile organic compounds. Furthermore, it is expected that global trade activities, demographic movement, and use of natural resources will be increasing in the Arctic regions. There is a need for a novel research approach, which not only identifies and tackles the relevant multi-disciplinary research questions, but also is able to make a holistic system analysis of the expected feedbacks. In this paper, we introduce the research agenda of the Pan-Eurasian Experiment (PEEX), a multi-scale, multi-disciplinary and international program started in 2012 (https://www.atm.helsinki.fi/peex/). PEEX sets a research approach by which large-scale research topics are investigated from a system perspective and which aims to fill the key gaps in our understanding of the feedbacks and interactions between the land-Atmosphere-Aquatic-society continuum in the northern Eurasian region. We introduce here the state of the art for the key topics in the PEEX research agenda and present the future prospects of the research, which we see relevant in this context.

In this study we introduce a new flow tube suitable for binary and ternary homogeneous nucleation studies. The production of sulfuric acid and water vapor mixture, the experimental setup and the method of sulfuric acid concentration determination are discussed in detail. Wall losses were estimated from the measured sulfuric acid concentration profiles along the flow tube and compared to a theoretical prediction. In this investigation the experimental evidence of new particle formation was observed at a concentration of 109 molecules cm−3 of sulfuric acid and the nucleation rates measured at three relative humidities (RH) 10, 30 and 50%, cover six orders of magnitude, from 10−3 to 103 particles cm−3. Particle free air was used as a carrier gas. Our initial results are compared to the theoretical prediction of binary homogeneous nucleation, to results obtained by other investigators, and to atmospheric nucleation.

The Finnish Meteorological Institute, in collaboration with the University of Helsinki, has established a new ground-based remote-sensing network in Finland. The network consists of five topographically, ecologically and climatically different sites distributed from southern to northern Finland. The main goal of the network is to monitor air pollution and boundary layer properties in near real time, with a Doppler lidar and ceilometer at each site. In addition to these operational tasks, two sites are members of the Aerosols, Clouds and Trace gases Research InfraStructure Network (ACTRIS); a Ka band cloud radar at Sodankylä will provide cloud retrievals within CloudNet, and a multi-wavelength Raman lidar, PollyXT (POrtabLe Lidar sYstem eXTended), in Kuopio provides optical and microphysical aerosol properties through EARLINET (the European Aerosol Research Lidar Network). Three C-band weather radars are located in the Helsinki metropolitan area and are deployed for operational and research applications. We performed two inter-comparison campaigns to investigate the Doppler lidar performance, compare the backscatter signal and wind profiles, and to optimize the lidar sensitivity through adjusting the telescope focus length and data-integration time to ensure sufficient signal-to-noise ratio (SNR) in low-aerosol-content environments. In terms of statistical characterization, the wind-profile comparison showed good agreement between different lidars. Initially, there was a discrepancy in the SNR and attenuated backscatter coefficient profiles which arose from an incorrectly reported telescope focus setting from one instrument, together with the need to calibrate. After diagnosing the true telescope focus length, calculating a new attenuated backscatter coefficient profile with the new telescope function and taking into account calibration, the resulting attenuated backscatter profiles all showed good agreement with each other. It was thought that harsh Finnish winters could pose problems, but, due to the built-in heating systems, low ambient temperatures had no, or only a minor, impact on the lidar operation – including scanning-head motion. However, accumulation of snow and ice on the lens has been observed, which can lead to the formation of a water/ice layer thus attenuating the signal inconsistently. Thus, care must be taken to ensure continuous snow removal.

© 2014 American Geophysical Union. All Rights Reserved Concentrations of atmospheric black carbon, [BC], were determined from filter samples collected weekly at Kevo, Finland (69°45′N, 27°02′E), from 1964 to 2010 using optical and thermal optical methods. The data provide the longest record of directly measured [BC] in the Arctic. The mean winter, spring, summer, and autumn [BC] based on the entire data set were 339, 199, 127, and 213 ng m−3, respectively. Annual mean [BC] decreased from ~300 in ~1970 to 82 ng m−3 in 2010. [BC] data sets from other Arctic sites show similar trends, but concentrations at Kevo are generally higher. From ~1970 to 2010 the [BC] decreased by ~1.8% yr−1. However, [BC] did not decrease monotonically. Instead, cyclical peaks occurred around 1976–1977, 1985–1987, and 1999. During such periods, nickel concentrations were well correlated with [BC]. This suggests that emissions from extensive ore smelting on the Kola Peninsula were significant contributors of particulate matter observed at Kevo. Simulations of [BC] at Kevo using the OsloCTM3 model using different emission inventories and meteorological data sets were performed. Modeled concentrations were lower than observed by a factor of 4. The results indicated that circulation changes can explain year to year variability, but the downward trend in the observations is mostly explained by emissions. Emission inventories in Europe, Russia, and the former Soviet Union are poorly constrained and appear to need revision in order to match observed trends in BC atmospheric concentrations.

International audience; Atmospheric new particle formation is generally thought to occur due to homogeneous or ion-induced nucleation of sulphuric acid. We compare ambient nucleation rates with laboratory data from nucleation experiments involving either sulphuric acid or oxidized SO2. Atmospheric nucleation occurs at H2SO4 concentrations 2?4 orders of magnitude lower than binary or ternary H2SO4 nucleation. In contrast, the atmospheric nucleation rates and H2SO4 concentrations are very well replicated in the SO2 oxidation experiments. We explain these features by the formation of free HSO5 radicals in pace with H2SO4 during the SO2 oxidation. We suggest that at temperatures above ~250 K these radicals produce nuclei of new aerosols much more efficiently than H2SO4. These nuclei are activated to further growth by H2SO4 and possibly other trace species. However, at lower temperatures the atmospheric relative acidity is high enough for the H2SO4?H2O nucleation to dominate.

Surface tension of ternary solution of sodium chloride, succinic acid and water was measured as a function of both composition and temperature by using the capillary rise technique. Both sodium chloride and succinic acid are found in atmospheric aerosols, the former being main constituent of marine aerosol. Succinic acid was found to decrease the surface tension of water already at very low concentrations. Sodium chloride increased the surface tension linearly as a function of the concentration. Surface tensions of both binary solutions agreed well with the previous measurements. Succinic acid was found to lower the surface tension even if sodium chloride is present, indicating that succinic acid as a surface active compound tends to concentrate to the surface. An equation based on thermodynamical relations was fitted to the data. As a result, a surface tension parameterization of ternary solution was obtained over the whole concentration range. The parameterization can safely be used at temperatures from 10 to 30°C. These kinds of parameterizations are important for example in atmospheric nucleation models. To investigate the influence of surface tension on cloud droplet activation, the surface tension parameterization was included in an adiabatic air parcel model. Usually in cloud models the surface tension of pure water is used. Simulations were done for characteristic marine aerosol size distributions consisting of the considered ternary mixture. We found that by using the surface tension of pure water, the amount of activated particles is underestimated up to 8% if particles contain succinic acid and overestimated it up to 8% if particles contain only sodium chloride. The surface tension effect was found to increase with increasing updraft velocity.

Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March-April 2003, in Hyytiala, Finland. Our aim was to understand the role of oxidation products of VOC's such as mono- and sesquiterpenes in atmospheric nucleation events. Particle chemical compositions were measured using the Aerodyne Aerosol Mass Spectrometer, and chemical compositions of aerosol samples collected with low-pressure impactors and a high volume sampler were analysed using a number of techniques. The results indicate that during and after new particle formation, all particles larger than 50 nm in diameter contained similar organic substances that are likely to be mono- and sesquiterpene oxidation products. The oxidation products identified in the high volume samples were shown to be mostly aldehydes. In order to study the composition of particles in the 10-50 nm range, we made use of Tandem Differential Mobility Analyzer results. We found that during nucleation events, both 10 and 50 nm particle growth factors due to uptake of ethanol vapour correlate strongly with gas-phase monoterpene oxidation product (MTOP) concentrations, indicating that the organic constituents of particles smaller than 50 nm in diameter are at least partly similar to those of larger particles. We furthermore showed that particle growth rates during the nucleation events are correlated with the gas-phase MTOP concentrations. This indicates that VOC oxidation products may have a key role in determining the spatial and temporal features of the nucleation events. This conclusion was supported by our aircraft measurements of new 3-10 nm particle concentrations, which showed that the nucleation event on 28 March 2003, started at the ground layer, i.e. near the VOC source, and evolved together with the mixed layer. Furthermore, no new particle formation was detected upwind away from the forest, above the frozen Gulf of Bothnia.