Search

During summer, the Southern Ocean is largely unaffected by anthropogenic emissions, which makes this region an ideal place to investigate marine natural aerosol sources and processes. A better understanding of natural aerosol is key to constrain the preindustrial aerosol state and reduce the aerosol radiative forcing uncertainty in global climate models. We report the concentrations of gaseous sulfuric acid, iodic acid, and methanesulfonic acid (MSA) together with a characterization of new particle formation (NPF) events over a large stretch of the Southern Ocean. Measurements were conducted on board the Russian icebreaker Akademik Tryoshnikov from January to March 2017. Iodic acid is characterized by a particular diurnal cycle with reduced concentration around noon, suggesting a lower formation yield when solar irradiance is higher. Gaseous MSA does not have a diurnal cycle and measured concentrations in gas and condensed phase are compatible with this species being primarily produced via heterogeneous oxidation of dimethyl sulfide and subsequent partitioning into the gas phase. We also found that NPF in the boundary layer is mainly driven by sulfuric acid but it occurred very rarely over the vast geographical area probed and did not contribute to the cloud condensation nuclei budget in a directly observable manner. Despite the near absence of NPF events in the boundary layer, Aitken mode particles were frequently measured, supporting the hypothesis of a free tropospheric source. Iodic acid and MSA were not found to participate in nucleation, however, MSA may contribute to aerosol growth via heterogeneous formation in the aqueous phase.

The Cape Verde Atmospheric Observatory (CVAO), which is influenced by both, marine and desert dust air masses, has been used for long-term measurements of different properties of the atmospheric aerosol from 2008 to 2017. These properties include particle number size distributions (PNSD), light absorbing carbon (LAC) and concentrations of cloud condensation nuclei (CCN) together with their hygroscopicity. Here we summarize the results obtained for these properties and use an unsupervised machine learning algorithm for the classification of aerosol types. Five types of aerosols, i.e., marine, freshly-formed, mixture, moderate dust and heavy dust, were classified. Air masses during marine periods are from the Atlantic Ocean and during dust periods are from the Sahara. Heavy dust was more frequently present during wintertime, whereas the clean marine periods were more frequently present during springtime. It was observed that during the dust periods CCN number concentrations at a supersaturation of 0.30 % are roughly 2.5 times higher than during marine periods, but the hygroscopicity (κ) of particles in the size range from ∼30 to ∼175 nm during marine and dust periods are comparable. The long-term data presented here, together with the aerosol classification, can be used as a base to improve our understanding of annual cycles of the atmospheric aerosol in the eastern tropical Atlantic and on aerosol-cloud interactions and it can be used as a base for driving, evaluating and constraining atmospheric model simulations.

Aerosol particles acting as cloud condensation nuclei (CCN) or ice nucleating particles (INP) play a major role in the formation and glaciation of clouds. Thereby they exert a strong impact on the radiation budget of the Earth. Data on abundance and properties of both types of particles are sparse, especially for remote areas of the world, such as the Southern Ocean (SO). In this work, we present unique results from ship-borne aerosol-particle-related in situ measurements and filter sampling in the SO region, carried out during the Antarctic Circumnavigation Expedition (ACE) in the Austral summer of 2016/17. An overview of CCN and INP concentrations on the Southern Ocean is provided and using additional quantities, insights regarding possible CCN and INP sources and origins are presented. CCN number concentrations spanned 2 orders of magnitude, e.g., for a supersaturation of 0.3 % values ranged roughly from 3 to 590 cm⁻³. CCN showed variable contributions of organic and inorganic material (inter-quartile range of hygroscopicity parameter κ from 0.2 to 0.9). No distinct size-dependence of κ was apparent, indicating homogeneous composition across sizes (critical dry diameter on average between 37 and 123 nm). The contribution of sea spray aerosol (SSA) to the CCN number concentration was on average small. Ambient INP number concentrations were measured in the temperature range from −5 to −27°C. Concentrations spanned up to 3 orders of magnitude, e.g., at −16°C from 0.2 to 100 m⁻³. Elevated values (above 10 m⁻³ at −16°C) were measured when the research vessel was in the vicinity of land, with lower and more constant concentrations when at sea. This hints towards terrestrial and/or coastal INP sources being dominant close to land. In pristine marine areas INP may originate from both oceanic sources and/or long range transport. Sampled aerosol particles (PM10) were analysed for sodium and methanesulfonic acid (MSA). Resulting mass concentrations were used as tracers for primary marine and secondary aerosol particles, respectively. Sodium, with an average concentration around 2.8 μg m⁻³, was found to dominate the sampled particle mass. MSA was highly variable over the SO, with concentrations up to 0.5 μg m⁻³ near the sea ice edge. A correlation analysis yielded strong correlations between sodium mass concentration and particle number concentration in the coarse mode, unsurprisingly indicating a significant contribution of SSA to that mode. CCN number concentration was highly correlated with the number concentration of Aitken and accumulation mode particles. This, together with a lack of correlation between sodium mass and Aitken and accumulation mode number concentrations, underlines the important contribution of non-SSA, probably secondarily formed particles, to the CCN population. INP number concentrations did not significantly correlate with any other measured aerosol physico-chemical parameter.

24 pages, 8 figures, supporting information https://doi.org/10.1029/2021JD034811.-- Data Availability Statement: The data set used in this study are available in (1) Antoine et al. (2019) available at https://doi.org/10.5281/zenodo.3406983; (2) Chen et al. (2019) available at https://doi.org/10.5281/zenodo.3559982; (3) Landwehr et al. (2020) available at https://doi.org/10.5281/zenodo.3836439; (4) Landwehr, Thurnherr et al. (2020) available at https://doi.org/10.5194/amt-13-3487-2020; (5) Schmale et al. (2019) available at https://doi.org/10.5281/zenodo.2636709; (6) Tatzelt et al. (2020) available at https://doi.org/10.5281/zenodo.3922147; (7) Thomalla et al., (2020) available at https://doi.org/10.5281/zenodo.3859515; (8) Thurnherr et al. (2020) available at https://doi.org/10.5281/zenodo.4031705; In addition, the fluorescent aerosol and gel–like POM measurements have been uploading as supplementary information supporting this article, In this study, we investigate the occurrence of primary biological aerosol particles (PBAP) over all sectors of the Southern Ocean (SO) based on a 90-day data set collected during the Antarctic Circumnavigation Expedition (ACE) in austral summer 2016–2017. Super-micrometer PBAP (1–16 µm diameter) were measured by a wide band integrated bioaerosol sensor (WIBS-4). Low (3σ) and high (9σ) fluorescence thresholds are used to obtain statistics on fluorescent and hyper-fluorescent PBAP, respectively. Our focus is on data obtained over the pristine ocean, that is, more than 200 km away from land. The results indicate that (hyper-)fluorescent PBAP are correlated to atmospheric variables associated with sea spray aerosol (SSA) particles (wind speed, total super-micrometer aerosol number concentration, chloride and sodium concentrations). This suggests that a main source of PBAP over the SO is SSA. The median percentage contribution of fluorescent and hyper-fluorescent PBAP to super-micrometer SSA was 1.6% and 0.13%, respectively. We demonstrate that the fraction of (hyper-)fluorescent PBAP to total super-micrometer particles positively correlates with concentrations of bacteria and several taxa of pythoplankton measured in seawater, indicating that marine biota concentrations modulate the PBAP source flux. We investigate the fluorescent properties of (hyper-)fluorescent PBAP for several events that occurred near land masses. We find that the fluorescence signal characteristics of particles near land is much more variable than over the pristine ocean. We conclude that the source and concentration of fluorescent PBAP over the open ocean is similar across all sampled sectors of the SO, The authors acknowledge funding for ACE-SPACE, ACE-SORPASSO by the Swiss Polar Institute, and Ferring Pharmaceuticals. ACE-SPACE was carried out with additional support from the European FP7 project BACCHUS (Grant Agreement 49603445). Gang Chen received funding from the cost action of Chemical On-Line cOmpoSition and Source Apportionment of fine aerosol (COLOSSAL, CA16109), a COST related project of the Swiss National Science Foundation, Source apportionment using long-term Aerosol Mass Spectrometry and Aethalometer Measurements (SAMSAM, IZCOZ0_177063). Sebastian Landwehr received funding from the Swiss Data Science Center project c17-02. Andrea Baccarin received funding from the Swiss National Science Foundation (Grant 200021_169090). Julia Schmale holds the Ingvar Kamprad Chair. Martin Gysel-Beer received funding from the ERC under Grant ERC-CoG-615922-BLACARAT. Charlotte Robinson received funding from the Australian Research Council (Grand ARC DP160103387), With the funding support of the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S), of the Spanish Research Agency (AEI)

Aerosol characteristics over the Southern Ocean are surprisingly heterogeneous because of the distinct regional dynamics and marine microbial regimes. Satellite observations and model simulations underestimate the abundance of cloud condensation nuclei. Uncertainty in radiative forcing caused by aerosol-cloud interactions is about twice as large as for CO2 and remains the least well-understood anthropogenic contribution to climate change. A major cause of uncertainty is the poorly-quantified state of aerosols in the pristine-preindustrial atmosphere, which defines the baseline against which anthropogenic effects are calculated. The Southern Ocean is one of the few remaining near-pristine aerosol environments on Earth, but there are very few measurements to evaluate models. The Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and their Climate Effects (ACE-SPACE) took place between December 2016 and March 2017 and covered the entire Southern Ocean region (Indian, Pacific and Atlantic Oceans, ship track > 33,000 km) including previously unexplored areas. In situ measurements covered aerosol characteristics (e.g., chemical composition, size distributions, and cloud condensation nuclei (CCN) number concentrations), trace gases and meteorological variables. Remote sensing observations of cloud properties, the physical and microbial ocean state, as well as back trajectory analyses are used to interpret the in situ data. The contribution of sea spray to CCN in the westerly wind belt can be larger than 50%. The abundance of methanesulfonic acid indicates local and regional microbial influence on CCN abundance in Antarctic coastal waters and in the open ocean. We use the in situ data to evaluate simulated CCN concentrations from a global aerosol model. The extensive, available ACE-SPACE dataset (https://zenodo.org/communities/spi-ace?page=1&size=20) provides an unprecedented opportunity to evaluate models and to reduce the uncertainty in radiative forcing associated with the natural processes of aerosol emission, formation, transport and processing occurring over the pristine Southern Ocean.

In a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment, is important for interpreting aerosol–cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements were made on-board research vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10–50 nm) number concentrations increased from background values of approx. 40 up to 4000 cm−3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1 m s−1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase in the CCN number concentration by a factor of 2 to 5 compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50 nm in diameter and the activated fraction of 15–50 nm particles was on average below 10 %, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. This implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles in Arctic cloud formation.

We report on the Azores Stratocumulus Measurements of Radiation, Turbulence and Aerosols (ACORES) campaign, which took place around Graciosa and Pico Islands/Azores in July 2017. The main objective was to investigate the vertical distribution of aerosol particles, stratocumulus microphysical and radiative properties, and turbulence parameters in the eastern North Atlantic. The vertical exchange of mass, momentum, and energy between the free troposphere (FT) and the cloudy marine boundary layer (MBL) was explored over a range of scales from submeters to kilometers. To cover these spatial scales with appropriate measurements, helicopter-borne observations with unprecedented high resolution were realized using the Airborne Cloud Turbulence Observation System (ACTOS) and Spectral Modular Airborne Radiation Measurement System–Helicopter-Borne Observations (SMART-HELIOS) instrumental payloads. The helicopter-borne observations were combined with ground-based aerosol measurements collected at two continuously running field stations on Pico Mountain (2,225 m above sea level, in the FT), and at the Atmospheric Radiation Measurement (ARM) station on Graciosa (at sea level). First findings from the ACORES observations we are discussing in the paper are as follows: (i) we have observed a high variability of the turbulent cloud-top structure on horizontal scales below 100 m with local temperature gradients of up to 4 K over less than 1 m vertical distance, (ii) we have collected strictly collocated radiation measurements supporting the relevance of small-scale processes by revealing significant inhomogeneities in cloud-top brightness temperature to scales well below 100 m, and (iii) we have concluded that aerosol properties are completely different in the MBL and FT with often-complex stratification and frequently observed burst-like new particle formation.

Within the framework of the RACEPAC (Radiation–Aerosol–Cloud Experiment in the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based station in Tuktoyaktuk (Mackenzie River delta area, Canada), was characterized during a period of 3 weeks in May 2014. Basic meteorological parameters and particle number size distributions (PNSDs) were observed and two distinct types of air masses were found. One type were typical Arctic haze air masses, termed accumulation-type air masses, characterized by a monomodal PNSD with a pronounced accumulation mode at sizes above 100 nm. These air masses were observed during a period when back trajectories indicate an air mass origin in the north-east of Canada. The other air mass type is characterized by a bimodal PNSD with a clear minimum around 90 nm and with an Aitken mode consisting of freshly formed aerosol particles. Back trajectories indicate that these air masses, termed Aitken-type air masses, originated from the North Pacific. In addition, the application of the PSCF receptor model shows that air masses with their origin in active fire areas in central Canada and Siberia, in areas of industrial anthropogenic pollution (Norilsk and Prudhoe Bay Oil Field) and the north-west Pacific have enhanced total particle number concentrations (NCN). Generally, NCN ranged from 20 to 500 cm−3, while cloud condensation nuclei (CCN) number concentrations were found to cover a range from less than 10 up to 250 cm−3 for a supersaturation (SS) between 0.1 and 0.7 %. The hygroscopicity parameter κ of the CCN was determined to be 0.23 on average and variations in κ were largely attributed to measurement uncertainties. Furthermore, simultaneous PNSD measurements at the ground station and on the Polar 6 research aircraft were performed. We found a good agreement of ground-based PNSDs with those measured between 200 and 1200 m. During two of the four overflights, particle number concentrations at 3000 m were found to be up to 20 times higher than those measured below 2000 m; for one of these two flights, PNSDs measured above 2000 m showed a different shape than those measured at lower altitudes. This is indicative of long-range transport from lower latitudes into the Arctic that can advect aerosol from different regions in different heights.

In the framework of the MarParCloud (Marine biological production, organic aerosol particles and marine clouds: a Process Chain) project, measurements were carried out on the islands of Cape Verde, to investigate the abundance, properties, and sources of aerosol particles in general and cloud condensation nuclei (CCN) in particular, both close to sea and cloud level heights. A thorough comparison of particle number concentration (PNC), particle number size distribution (PNSD) and CCN number concentration (NCCN) at the Cape Verde Atmospheric Observatory (CVAO, sea level station) and Monte Verde (MV, cloud level station) reveals that during times without clouds the aerosol at CVAO and MV are similar and the boundary layer is generally well mixed. Therefore, data obtained at CVAO can be used to describe the aerosol particles at cloud level. Cloud events were observed at MV during roughly 58 % of the time and during these, a large fraction of particles were activated to cloud droplets. A trimodal parameterization method was deployed to characterize PNC at CVAO. Based on number concentrations in different aerosol modes, four well separable types of PNSDs were found, which were named the marine type, mixture type, dust type1 and dust type2. Aerosol particles differ depending on their origins. When the air masses came from the Atlantic Ocean, sea spray can be assumed to be one source for particles, besides for new particle formation. For these air masses, PNSDs featured the lowest number concentration in Aitken, accumulation and coarse mode. Particle number concentrations for the sea spray aerosol (SSA, i.e., the coarse mode for these air masses) accounted for about 3.7 % of NCCN,0.30 % (CCN number concentration at 0.30 % supersaturation) and about 1.1 % to 4.4 % of Ntotal (total particle number concentration). When the air masses came from the Saharan desert, we observed enhanced Aitken, accumulation and coarse mode particle number concentrations and overall increased NCCN. NCCN,0.30 % during the strongest observed dust periods is about 2.5 times higher than that during marine periods. However, the particle hygroscopicity parameter κ for these two most different periods shows no significant difference and is generally similar, independent of air mass. Overall, κ averaged 0.28, suggesting the presence of organic material in particles. This is consistent with previous model work and field measurement. There is a slight increase of κ with increasing particle size, indicating the addition of soluble, likely inorganic material during cloud processing.

This study presents vertical profiles up to a height of 2300 m a.s.l. of aerosol microphysical and optical properties and cloud condensation nuclei (CCN). Corresponding data have been measured during a field campaign as part of the High-Definition Clouds and Precipitation for Advancing Climate Prediction (HD(CP)2) Observational Prototype Experiments (HOPE), which took place at Melpitz, Germany from September 9 to 29, 2013. The helicopter-borne payload ACTOS (Airborne Cloud and Turbulence Observation System) was used to determine the aerosol particle number size distribution (PNSD), the number concentrations of aerosol particles (PNC) and cloud condensation nuclei (CCN) (CCN-NC), the ambient relative humidity (RH), and temperature (T). Simultaneous measurements on ground provided a holistic view on aerosol microphysical properties such as the PNSD, the chemical composition and the CCN-NC. Additional measurements of a 3 + 2 wavelength polarization lidar system (PollyXT) provided profiles of the aerosol particle light backscatter coefficient (σbsc) for three wavelengths (355, 532 and 1064 nm). From profiles of σbsc profiles of the aerosol particle light extinction coefficient (σext) were determined using the extinction-to-backscatter ratio. Furthermore, CCN-NC profiles were estimated on basis of the lidar-measurements. Ambient state optical properties of aerosol particles were derived on the basis of airborne in situ measurements of ACTOS (PNSD) and in situ measurements on ground (chemical aerosol characterization) using Mie-theory. On the basis of ground-based and airborne measurements, this work investigates the representativeness of ground-based aerosol microphysical properties for the boundary layer for two case-studies. The PNSD measurements on ground showed a good agreement with the measurements provided with ACTOS for lower altitudes. The ground-based measurements of PNC and CCN-NC are representative for the PBL when the PBL is well mixed. Locally isolated new particle formation events on ground or at the top of the PBL led to vertical variability in the here presented cases and ground-based measurements are not representative for the PBL. Furthermore, the lidar-based estimates of CCN-NC profiles were compared with the airborne in situ measurements of ACTOS. This comparison showed good agreements within the uncertainty range. Finally, this work provides a closure study between the optical aerosol particle properties in ambient state based on the airborne ACTOS measurements and derived with the lidar measurements. The investigation of the optical properties shows for 14 measurement-points that the airborne-based particle light backscatter coefficient is for 1064 nm 50 % smaller than the measurements of the lidar system, 27.6 % smaller for 532 nm and 29.9 % smaller for 355 nm. These results are quite promising, since in-situ measurement based Mie-calculations of the particle light backscattering are scarce and the modelling is quite challenging. In contradiction for the particle light extinction coefficient retrieved from the airborne in situ measurements were found a good agreement. The airborne-based particle light extinction coefficient was just 7.9 % larger for 532 nm and 3.5 % smaller for 355 nm, for an assumed lidar ratio (LR) of 55 sr. The particle light extinction coefficient for 1064 nm was derived with a LR of 30 sr. For this wavelength, the airborne-based particle light extinction coefficient is 5.2 % smaller than the lidar-measurements. Also, the correlation for the particle light extinction coefficient in combination with Mie-based LR's are in agreement for typical LR's of European background aerosol.

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). Numerous observations of CCN number concentration exist, and many closure studies have been performed to predict CCN number concentrations based on particle number size distributions, chemical composition, and the κ-Köhler theory. Most of these studies provide details for short time periods or focus on special environmental conditions. These observations, however, cannot address questions of large-scale temporal and spatial CCN variability. Here we analyze long-term observations of CCN number concentrations, particle number size distributions and chemical composition from twelve sites on three continents. Eight of these stations are part of the European Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS). We group the observatories into categories according to their official classification: coastal background (Barrow, Alaska; Mace Head, Ireland; Finokalia, Crete; Noto Peninsula, Japan), rural background (Melpitz, Germany; Cabauw, the Netherlands; Vavihill, Sweden), alpine sites (Puy de Dôme, France; Jungfraujoch, Switzerland), remote forest sites (ATTO, Brazil; SMEAR, Finland) and the urban environment (Seoul, South Korea). Expectedly, CCN characteristics are highly variable across regions. However, they also vary within categories, 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 behavior, most continental stations exhibit very similar relative activation ratios across the range of 0.1 to 1.0 % supersaturation. At the coastal sites the activation ratios spread more widely across the SS 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 (forest fire influence in fall). 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 the lowest at the rain forest station ATTO (0.2–0.3). We performed closure studies to predict CCN number concentrations from the particle number size distribution and chemical composition measurements. The prediction accuracy for the average concentrations is high. The ratio between predicted and measured CCN concentrations is between 0.87 and 1.4. The temporal variability is also well represented, as reflected by Pearson correlation coefficients > 0.87. We also conducted a series of sensitivity studies for the ratio of predicted versus measured CCN concentration, where we varied the hygroscopicity parameter κ, and made simple assumptions for aerosol particle number concentrations and size distributions. Uncertain particle number concentrations and their size distributions significantly impair the accuracy in predicting temporal variability and hence of absolute concentrations, while the effect of uncertain κ values is limited to the predicted CCN number concentration. Information on CCN number concentrations at many locations is important to better characterize ACI and their radiative forcing. Long-term comprehensive aerosol particle characterizations are labor intensive and costly. For observatories where such efforts are out of scope to obtain nevertheless long-term information of CCN number concentrations, we recommend conducting 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 be calculated based on continued particle number size distribution information only. This approach is a good alternative to deriving kappa from time-resolved chemical composition measurements which are costly and may still not cover the appropriate size range. Additionally, given the variability in observations at sites of the same category, a certain density in spatial coverage of observations is needed, especially along coastlines. We recommend operating "migrating-CCNCs" at priority locations, identified by model evaluation, around the globe where long-term particle number size distribution data are already available.

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

Scattering and absorption coefficients have been measured continuously at several wavelengths since March 2001 at the high altitude site Jungfraujoch (3580ma.s.l.). From these data, the wavelength dependences of the Ångström exponent and particularly of the single scattering albedo are determined. While the exponent of the single scattering albedo usually increases with wavelength, it decreases with wavelength during Saharan dust events (SDE) due to the greater size of the mineral aerosol particles and their different chemical composition. This change in the sign of the single scattering exponent turns out to be a sensitive means for detecting Saharan dust events. The occurrence of SDE detected by this new method was confirmed by visual inspection of filter colors and by studying long-range back-trajectories. An examination of SDE over a 22-month period shows that SDE are more frequent during the March-June period as well as during October and November. The trajectory analysis indicated a mean traveling time of 96.5h, with the most important source countries situated in the northern and north-western part of the Saharan desert. Most of the SDE do not lead to a detectable increase of the 48-h total suspended particulate matter (TSP) concentration at the Jungfraujoch. During Saharan dust events, the average contribution of this dust to hourly TSP at the Jungfraujoch is 16µg/m3, which corresponds to an annual mean of 0.8µg/m3 or 24% of TSP.

The largest uncertainty in the estimation of climate forcing stems from atmospheric aerosols. In early spring and summer of 2009, two periods of in-situ measurements on aerosol physical and chemical properties were conducted within the HaChi (Haze in China) project at Wuqing, a town between Beijing and Tianjin in the North China Plain (NCP). Aerosol optical properties, including the scattering coefficient (σsp), the hemispheric back scattering coefficient (σbsp), the absorption coefficient (σap), as well as the single scattering albedo (ω), are presented. The diurnal and seasonal variations are analyzed together with meteorology and satellite data. The mean values of σsp, 550 nm of the dry aerosol in spring and summer are 280±253 and 379±251 Mm−1, respectively. The average σap for the two periods is respectively 47±38 and 43±27 Mm−1. The mean values of ω at the wavelength of 637 nm are 0.82±0.05 and 0.86±0.05 for spring and summer, respectively. The relative high levels of σsp and σbsp are representative of the regional aerosol pollution in the NCP. Pronounced diurnal cycle of $σsp, σap and ω are found, mainly influenced by the evolution of boundary layer and the accumulation of local emissions during nighttime. The pollutants transported from the southwest of the NCP are more significant than that from the two megacities, Beijing and Tianjin, in both spring and summer. An optical closure experiment is conducted to better understand the uncertainties of the measurements. Good correlations (R>0.98) are found between the values measured by the nephelometer and the values calculated with a modified Mie model. The Monte Carlo simulation shows an uncertainty of about 30 % for the calculations. Considering all possible uncertainties of measurements, calculated σsp and σbsp agree well with the measured values, indicating a stable performance of instruments and thus reliable aerosol optical data.

[1] This study reports the first long-term trend analysis of aerosol optical measurements at the high-alpine site Jungfraujoch, which started 10.5 years ago. Since the aerosol variables are approximately lognormally distributed, the seasonal Kendall test and Sen's slope estimator were applied as nonparametric methods to detect the long-term trends for each month. The yearly trend was estimated by a least-mean-square fit, and the number of years necessary to detect this trend was calculated. The most significant trend is the increase (4–7% yr−1) in light-scattering coefficients during the September to December period. The light absorption and backscattering coefficients and the aerosol number concentration also show a positive trend during this time of the year. The hemispheric backscattering fraction and the scattering exponent calculated with the smaller wavelengths (450 and 550 nm), which relate to the small aerosol size fraction, decrease except during the summer, whereas the scattering exponent calculated with the larger wavelengths (550 and 700 nm) remains constant. Generally, the summer months at the Jungfraujoch, which are strongly influenced by planetary boundary layer air masses, do not show any long-term trend. The trends determined by least-mean-square fits of the scattering and backscattering coefficients, the hemispheric backscattering fractions, and the scattering exponent are significant, and the number of years necessary to detect them is shorter than 10 years. For these variables, the trends and the slopes estimated by the seasonal Kendall test are therefore confirmed by the least-mean-square fit results.

[1] Within the Global Atmosphere Watch (GAW) Aerosol Program of the World Meteorological Organization (WMO), the aerosol chemical composition has been continuously measured since July 1999 at the Jungfraujoch (JFJ) of which the first 1.5-year data set is presented. Sampling is performed in two size classes (total suspended particles (TSP) and particles with aerodynamic diameters smaller than 1 μm). The filters are analyzed for major ions, which constitute 30% of the total dry aerosol mass collected at this site. As annual mean, a total ion mass concentration of 1.04 μg m−3 was observed. Sulfate, ammonium, and nitrate were the major components of the fine aerosol fraction, while calcium and nitrate were two major water-soluble components in the coarse mode. Single particle analysis confirmed the internal mixture of calcium and nitrate in the coarse mode. The total ion mass concentration showed strong seasonal differences, with 1.25, 1.62, 0.70, and 0.25 μg m−3 for spring, summer, fall, and winter, respectively. The variability was stronger for sulfate, ammonium, and nitrate than for calcium. The reason for this is believed to be local sources of calcium, which do not require vertical transport, along with Sahara dust episodes, which occur occasionally over the whole year, independent from the season.