During Biogenic Aerosols—Effects on Clouds and Climate (BAECC), the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Program deployed the Second ARM Mobile Facility (AMF2) to Hyytiälä, Finland, for an 8-month intensive measurement campaign from February to September 2014. The primary research goal is to understand the role of biogenic aerosols in cloud formation. Hyytiälä is host to the Station for Measuring Ecosystem–Atmosphere Relations II (SMEAR II), one of the world’s most comprehensive surface in situ observation sites in a boreal forest environment. The station has been measuring atmospheric aerosols, biogenic emissions, and an extensive suite of parameters relevant to atmosphere–biosphere interactions continuously since 1996. Combining vertical profiles from AMF2 with surface-based in situ SMEAR II observations allows the processes at the surface to be directly related to processes occurring throughout the entire tropospheric column. Together with the inclusion of extensive surface precipitation measurements and intensive observation periods involving aircraft flights and novel radiosonde launches, the complementary observations provide a unique opportunity for investigating aerosol–cloud interactions and cloud-to-precipitation processes in a boreal environment. The BAECC dataset provides opportunities for evaluating and improving models of aerosol sources and transport, cloud microphysical processes, and boundary layer structures. In addition, numerical models are being used to bridge the gap between surface-based and tropospheric observations.

Abstract. Ambient aerosol particles can take up water and thus change their optical properties depending on the hygroscopicity and the relative humidity (RH) of the surrounding air. Knowledge of the hygroscopicity effect is of crucial importance for radiative forcing calculations and is also needed for the comparison or validation of remote sensing or model results with in situ measurements. Specifically, particle light scattering depends on RH and can be described by the scattering enhancement factor f (RH), which is defined as the particle light scattering coefficient at defined RH divided by its dry value (RH < 30-40 %).Here, we present results of an intensive field campaign carried out in summer 2013 at the SMEAR II station at Hyytiälä, Finland. Ground-based and airborne measurements of aerosol optical, chemical and microphysical properties were conducted. The f (RH) measured at ground level by a humidified nephelometer is found to be generally lower (e.g. 1.63 ± 0.22 at RH = 85 % and λ = 525 nm) than observed at other European sites. One reason is the high organic mass fraction of the aerosol encountered at Hyytiälä to which f (RH) is clearly anti-correlated (R 2 ≈ 0.8). A simplified parametrization of f (RH) based on the measured chemical mass fraction can therefore be derived for this aerosol type. A trajectory analysis revealed that elevated values of f (RH) and the corresponding elevated inorganic mass fraction are partially caused by transported hygroscopic sea spray particles. An optical closure study shows the consistency of the ground-based in situ measurements.Our measurements allow to determine the ambient particle light extinction coefficient using the measured f (RH). By combining the ground-based measurements with intensive aircraft measurements of the particle number size distribution and ambient RH, columnar values of the particle extinction coefficient are determined and compared to columnar measurements of a co-located AERONET sun photometer. The water uptake is found to be of minor importance for the column-averaged properties due to the low particle hygroscopicity and the low RH during the daytime of the summer months. The in situ derived aerosol optical depths (AOD) clearly correlate with directly measured values of the sun photometer but are substantially lower compared to the directly measured values (factor of ∼ 2-3). The comparison degrades for longer wavelengths. The disagreement between in situ derived and directly measured AOD is hypothesized Published by Copernicus Publications on behalf of the European Geosciences Union. 7248 P. Zieger et al.: Scattering enhancement of boreal aerosol and columnar closure study to originate from losses of coarse and fine mode particles through dry deposition within the canopy and losses in the in situ sampling lines. In addition, elevated aerosol layers (above 3 km) from long-range transport were observed using an aerosol lidar at Kuopio, Finland, about 200 km east-northeast of Hyytiälä. These elevated layers further explain parts of the disagree...

Abstract. The smelter industry in Kola Peninsula is the largest source of anthropogenic SO 2 in the Arctic part of Europe and one of the largest within the Arctic domain. Due to socio-economic changes in Russia, the emissions have been decreasing especially since the late 1990s resulting in decreased SO 2 concentrations close to Kola in eastern Lapland, Finland. At the same time, the frequency of new particle formation days has been decreasing distinctively at SMEAR I station in eastern Lapland, especially during spring and autumn. We show that sulfur species, namely sulfur dioxide and sulfuric acid, have an important role in both new particle formation and subsequent growth and that the decrease in new particle formation days is a result of the reduction of sulfur emissions originating from Kola Peninsula. In addition to sulfur species, there are many other quantities, such as formation rate of aerosol particles, condensation sink and nucleation mode particle number concentration, which are related to the number of observed new particle formation (NPF) days and need to be addressed when linking sulfur emissions and NPF. We show that while most of these quantities exhibit statistically significant trends, the reduction in Kola sulfur emissions is the most obvious reason for the rapid decline in NPF days. Sulfuric acid explains approximately 20-50 % of the aerosol condensational growth observed at SMEAR I, and there is a large seasonal variation with highest values obtained during spring and autumn. We found that (i) particles form earlier after sunrise during late winter and early spring due to high concentrations of SO 2 and H 2 SO 4 ; (ii) several events occurred during the absence of light, and they were connected to higher than average concentrations of SO 2 ; and (iii) high SO 2 concentrations could advance the onset of nucleation by several hours. Moreover, air masses coming over Kola Peninsula seemed to favour new particle formation.

Abstract. This work presents airborne observations of sub-3 nm particles in the lower troposphere and investigates new particle formation (NPF) within an evolving boundary layer (BL). We studied particle concentrations together with supporting gas and meteorological data inside the planetary BL over a boreal forest site in Hyytiälä, southern Finland. The analysed data were collected during three flight measurement campaigns: May–June 2015, August 2015 and April–May 2017, including 27 morning and 26 afternoon vertical profiles. As a platform for the instrumentation, we used a Cessna 172 aircraft. The analysed flight data were collected horizontally within a 30 km distance from SMEAR II in Hyytiälä and vertically from 100 m above ground level up to 2700 m. The number concentration of 1.5–3 nm particles was observed to be, on average, the highest near the forest canopy top and to decrease with increasing altitude during the mornings of NPF event days. This indicates that the precursor vapours emitted by the forest play a key role in NPF in Hyytiälä. During daytime, newly formed particles were observed to grow in size and the particle population became more homogenous within the well-mixed BL in the afternoon. During undefined days with respect to NPF, we also detected an increase in concentration of 1.5–3 nm particles in the morning but not their growth in size, which indicates an interrupted NPF process during these undefined days. Vertical mixing was typically stronger during the NPF event days than during the undefined or non-event days. The results shed light on the connection between boundary layer dynamics and NPF.

Abstract. We investigated atmospheric aerosol particle dynamics in a boreal forest zone in northern Scandinavia. We used aerosol number size distribution data measured with either a differential mobility particle sizer (DMPS) or scanning mobility particle sizer (SMPS) at three stations (Värriö, Pallas and Abisko), and combined these data with the HYS-PLIT (Hybrid Single Particle Lagrangian Integrated Trajectory) air mass trajectory analysis. We compared three approaches: analysis of new particle formation events, investigation of aerosol particle number size distributions during the air mass transport from the ocean to individual stations with different overland transport times, and analysis of changes in aerosol particle number size distributions during the air mass transport from one measurement station to another. Aitkenmode particles were found to have apparent average growth rates of 0.6-0.7 nm h −1 when the air masses traveled over land. Particle growth rates during the new particle formation (NPF) events were 3-6 times higher than the apparent particle growth during the summer period. When comparing aerosol dynamics for different overland transport times between the different stations, no major differences were found, except that in Abisko the NPF events were observed to take place in air masses with shorter overland times than at the other stations. We speculate that this is related to the meteorological differences along the paths of air masses caused by the land surface topology. When comparing air masses traveling in an east-to-west direction with those traveling in a west-to-east direction, clear differences in the aerosol dynamics were seen. Our results suggest that the condensation growth has an important role in aerosol dynamics even when NPF is not evident.

15This study explores the vertical and horizontal variability of the particle number size distribution from two flight measurements campaigns over a boreal forest in Hyytiälä, Finland during May-June 2013 and March-April 2014, respectively. Our other aims were to study the spatial extent of new particle formation events and to compare the airborne observation with the ground measurements from the SMEAR II (Station for Measuring Ecosystem-Atmosphere Relations) field station located in Hyytiälä.The airborne measurements extended vertically 3.8 km and horizontally 30 km from the station. A Cessna 172 aircraft was 20 used as a measurement platform. The measured parameters included the particle number concentration (>3 nm) and particle number size distribution (10-400 nm). The airborne data used in this study were equal to 111 flight hours. The measurements showed that despite local fluctuations there was a good agreement between the on-ground and airborne measurements inside the planetary boundary layer. On median, the airborne total number concentration was found to be 10 % larger than at the ground level. The seasonal and meteorological differences between the campaigns were reflected in aerosol properties. NPF 25 days showed areas of intensified NPF on a scale from kilometres up to couple of tens of kilometres in the planetary boundary layer. NPF was also observed frequently in the free troposphere.Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016Discuss., doi:10.5194/acp- -556, 2016 Manuscript under review for journal Atmos. Chem. Phys. Published: 18 July 2016 c Author(s) 2016. CC-BY 3.0 License. 2 IntroductionAtmospheric measurements performed at ground-based stations are often generalized to represent the conditions on the larger scale. However, the spatial and temporal scales of the complex atmospheric phenomena, like new particle formation (NPF), and information on spatial variability of aerosol properties is needed for correct extrapolation and parametrization of groundbased observations to larger scale and for use in modelling studies. 5Numerous measurement have shown that the NPF from precursor gases (Kulmala et al. 2013) occurs frequently around the world (Kulmala and Kerminen 2008, Kulmala et al. 2004, Zhang et al. 2012, and that the subsequent growth of these fresh-born particles is a climatically important source of cloud condensation nuclei (CCN) . Model studies by Spracklen et al (2008) and Merikanto et al (2009) show that NPF in the planetary boundary layer (PBL) can increase the global PBL CCN production up to 50 %. The Hyytiälä SMEAR II (Station for Measuring Ecosystem-10Atmosphere Relations) measurement site located in Southern Finland has provided an extensive two-decade long measurement time series of aerosol properties in a rural boreal forest environment (Hari and Kulmala 2005, Nieminen et al. 2014). In Hyytiälä, NPF days are occurring regularly on around 25% of the days with a peak observed during the spring when NPF occurs almost every other day on average , Nieminen et al. 2014....

Abstract. Understanding the distribution of aerosol layers is important for determining long-range transport and aerosol radiative forcing. In this study we combine airborne in situ measurements of aerosol with data obtained by a ground-based high spectral resolution lidar (HSRL) and radiosonde profiles to investigate the temporal and vertical variability of aerosol properties in the lower troposphere. The HSRL was deployed in Hyytiälä, southern Finland, from January to September 2014 as a part of the U.S. DOE ARM (Atmospheric Radiation Measurement) mobile facility during the BAECC (Biogenic Aerosols – Effects on Cloud and Climate) Campaign. Two flight campaigns took place in April and August 2014 with instruments measuring the aerosol size distribution from 10 nm to 5 µm at altitudes up to 3800 m. Two case studies with several aerosol layers present were selected from the flight campaigns for further investigation: one clear-sky and one partly cloudy case. During the clear-sky case, turbulent mixing ensured small temporal and spatial variability in the measured aerosol size distribution in the boundary layer, whereas mixing was not as homogeneous in the boundary layer during the partly cloudy case. The elevated layers exhibited larger temporal and spatial variability in aerosol size distribution, indicating a lack of mixing. New particle formation was observed in the boundary layer during the clear-sky case, and nucleation mode particles were also seen in the elevated layers that were not mixing with the boundary layer. Interpreting local measurements of elevated layers in terms of long-range transport can be achieved using back trajectories from Lagrangian models, but care should be taken in selecting appropriate arrival heights, since the modelled and observed layer heights did not always coincide. We conclude that higher confidence in attributing elevated aerosol layers to their air mass origin is attained when back trajectories are combined with lidar and radiosonde profiles.

Abstract. Recent studies have shown the importance of new particle formation (NPF) to global cloud condensation nuclei (CCN) production, as well as to air pollution in megacities. In addition to the necessary presence of low-volatility vapors that can form new aerosol particles, both numerical and observational studies have shown that the dynamics of the planetary boundary layer (BL) plays an important role in NPF. Evidence from field observations suggests that roll vortices might be favorable for inducing NPF in a convective BL. However, direct observations and estimates of the potential importance of this phenomenon to the production of new aerosol particles are lacking. Here we show that rolls frequently induce NPF bursts along the horizontal circulations and that the small clusters and particles originating from these localized bursts grow in size similar to particles typically ascribed to atmospheric NPF that occur almost homogeneously at a regional scale. We outline a method to identify roll-induced NPF from measurements and, based on the collected data, estimate the impact of roll vortices on the overall aerosol particle production due to NPF at a boreal forest site (83 % ± 34 % and 26 % ± 8 % overall enhancement in particle formation for 3 and 10 nm particles, respectively). We conclude that the formation of roll vortices should be taken into account when estimating particle number budgets in the atmospheric BL.