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Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.

Understanding aerosol particle activation is essential for evaluating aerosol indirect effects (AIEs) on climate. Long-term measurements of aerosol particle activation help to understand the AIEs and narrow down the uncertainties of AIEs simulation. However, they are still scarce. In this study, more than 4 years of comprehensive aerosol measurements were utilized at the central European research station of Melpitz, Germany, to gain insight into the aerosol particle activation and provide recommendations on improving the prediction of number concentration of cloud condensation nuclei (CCN, NCCN). (1) The overall CCN activation characteristics at Melpitz are provided. As supersaturation (SS) increases from 0.1 % to 0.7 %, the median NCCN increases from 399 to 2144 cm−3, which represents 10 % to 48 % of the total particle number concentration with a diameter range of 10–800 nm, while the median hygroscopicity factor (κ) and critical diameter (Dc) decrease from 0.27 to 0.19 and from 176 to 54 nm, respectively. (2) Aerosol particle activation is highly variable across seasons, especially at low-SS conditions. At SS=0.1 %, the median NCCN and activation ratio (AR) in winter are 1.6 and 2.3 times higher than the summer values, respectively. (3) Both κ and the mixing state are size-dependent. As the particle diameter (Dp) increases, κ increases at Dp of ∼40 to 100 nm and almost stays constant at Dp of 100 to 200 nm, whereas the degree of the external mixture keeps decreasing at Dp of ∼40 to 200 nm. The relationships of κ vs. Dp and degree of mixing vs. Dp were both fitted well by a power-law function. (4) Size-resolved κ improves the NCCN prediction. We recommend applying the κ–Dp power-law fit for NCCN prediction at Melpitz, which performs better than using the constant κ of 0.3 and the κ derived from particle chemical compositions and much better than using the NCCN (AR) vs. SS relationships. The κ–Dp power-law fit measured at Melpitz could be applied to predict NCCN for other rural regions. For the purpose of improving the prediction of NCCN, long-term monodisperse CCN measurements are still needed to obtain the κ–Dp relationships for different regions and their seasonal variations.

Understanding aerosol particle activation is essential for evaluating aerosol indirect effects (AIEs) on climate. Long-term measurements on aerosol particle activation help to understand the AIEs and narrow down the uncertainties of AIEs simulation; however, they are still scarce. In this study, more than 4-year aerosol comprehensive measurements were utilized at the central European research station Melpitz, Germany, to gain insight into the aerosol particle activation and provide recommendations on improving prediction. The overall characteristics of aerosol particle activation at Melpitz are first summarized. For supersaturation (SS) levels of 0.1 %, 0.2 %, 0.3 %, 0.5 %, and 0.7 %, the mean cloud condensation nuclei (CCN) number concentration (NCCN) increases with the increase of SS from 513 to 2477 cm-3, which represents 11 % to 52 % of the total particle number concentration with diameter ranging from 10 to 800 nm, while the hygroscopicity factor (k) and the critical diameter (Dc) decrease from 0.28±0.08 (mean value ± one standard deviation) to 0.20±0.09 and from 177±19 to 54±8 nm, respectively. Aerosol particle activation is highly variable across seasons, especially at low SS conditions. At SS = 0.1 %, the seasonal mean NCCN is 681 cm-3 in winter, which is almost twice higher than the summer value (347 cm-3); the seasonal mean activation ratio (AR) in winter (0.18) is three times higher than the summer one. Subsequently, size dependency of both k and the state of mixing were investigated. As the particle diameter (Dp) increases, k increases at Dp of ~40 to 100 nm and almost stays constant at Dp of 100 to 200 nm, whereas the degree of the external mixture keeps decreasing at Dp of ~40 to 200 nm. The relationships of k vs. Dp and mixture degree vs. Dp were both fitted well by the power-law function for each season. Finally, we recommend applying the k - Dp power-law fit for NCCN prediction, which can narrow down the median uncertainty within 10 % for different SS conditions and seasons at Melpitz; it also could be applied to predict NCCN at other rural and continental regions with a similar aerosol background. Additionally, the mean k value over Dp of 100 to 200 nm also works well on the NCCN prediction when SS is less than 0.2 %.

Environmental monitoring involves the quantification of microscopic cells and particles such as algae, plant cells, pollen, or fungal spores. Traditional methods using conventional microscopy require expert knowledge, are time-intensive and not well-suited for automated high throughput. Multispectral imaging flow cytometry (MIFC) allows measurement of up to 5000 particles per second from a fluid suspension and can simultaneously capture up to 12 images of every single particle for brightfield and different spectral ranges, with up to 60x magnification. The high throughput of MIFC has high potential for increasing the amount and accuracy of environmental monitoring, such as for plant-pollinator interactions, fossil samples, air, water or food quality that currently rely on manual microscopic methods. Automated recognition of particles and cells is also possible, when MIFC is combined with deep-learning computational techniques. Furthermore, various fluorescence dyes can be used to stain specific parts of the cell to highlight physiological and chemical features including: vitality of pollen or algae, allergen content of individual pollen, surface chemical composition (carbohydrate coating) of cells, DNA- or enzyme-activity staining. Here, we outline the great potential for MIFC in environmental research for a variety of research fields and focal organisms. In addition, we provide best practice recommendations.

Ice nucleating particles (INPs) are rare but important atmospheric particles as they induce the formation of primary ice in mixed phase clouds and also in some cirrus clouds. A plethora of substances which can be found in atmospheric particles can induce ice nucleation. The most important ice active particle types in the atmosphere are assumed to be mineral dust and biological particles, which can originate from a large number of sources. It is hence not surprising that INP concentrations vary over several orders of magnitude at any ice nucleation temperature, with concentrations being typically larger in continental than in marine environments. Although research concerning INP and their global occurrence has seen a steep rise in the past years, global INP concentrations are still not well known, and not all important INP sources are clear, neither are there good parameterizations for describing INP concentrations in models.To increase the knowledge of typical global INP concentrations and to draw conclusions about INP sources, we examined INP concentrations in the Antarctic region, namely at the German research Station Neumayer III, located at shelf ice in close proximity (only some 10 km) to the ice edge, at the Belgian research Station Princess Elisabeth, located roughly 200 km inland and at an altitude of 1390 m, and during a campaign including ship- and land-based data at the Antarctic peninsula. We used our well-established methods of filter collection and off-line analysis with cold-stages to derive INP concentrations in these locations.For Neumayer, two years of data are available. INP concentrations there were generally lower than values derived, e.g., for northern mid latitudes, and they were similar to values published for the Southern Ocean in literature. No pronounced annual cycle was observed. Around and on the Antarctic peninsula, INP concentrations were roughly similar to those observed at Neumayer. However, the Princess Elisabeth station, for which only data obtained during two austral summers are available, showed the lowest values detected in this study. Our results suggest that sources of INP in the Antarctic region are rare, and particularly so on Antarctica itself.

The sources and abundance of ice-nucleating particles (INPs) that initiate cloud ice formation remain understudied, especially in the Southern Hemisphere. In this study, we present INP measurements taken close to Punta Arenas, Chile, at the southernmost tip of South America from May 2019 to March 2020, during the Dynamics, Aerosol, Cloud, And Precipitation Observations in the Pristine Environment of the Southern Ocean (DACAPO-PESO) campaign. The highest ice nucleation temperature was observed at −3◦C, and from this temperature down to ∼ −10◦C, a sharp increase of INP number concentration (NINP) was observed. Heating of the samples revealed that roughly 90 % and 80 % of INPs are proteinaceous-based biogenic particles at > −10 and −15◦C, respectively. The NINP at Punta Arenas is much higher than that in the Southern Ocean, but it is comparable with an agricultural area in Argentina and forestry environment in the US. Ice active surface site density (ns) is much higher than that for marine aerosol in the Southern Ocean, but comparable to English fertile soil dust. Parameterization based on particle number concentration in the size range larger than 500 nm (N>500 nm) from the global average (DeMott et al., 2010) overestimates the measured INP, but the parameterization representing biological particles from a forestry environment (Tobo et al., 2013) yields NINP comparable to this study. No clear seasonal variation of NINP was observed. High precipitation is one of the most important meteorological parameters to enhance the NINP in both cold and warm seasons. A comparison of data from in situ and lidar measurements showed good agreement for concentrations of large aerosol particles (> 500 nm) when assuming continental conditions for retrieval of the lidar data, suggesting that these particles were well mixed within the planetary boundary layer (PBL). This corroborates the continental origin of these particles, consistent with the results from our INP source analysis. Overall, we suggest that a high NINP of biogenic INPs originated from terrestrial sources and were added to the marine air masses during the overflow of a maximum of roughly 150 km of land before arriving at the measurement station.

Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigated the chemical composition and provided an overview of the phase state of individual particles that have been long-range transported over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP), in the Azores. OMP is an ideal site for studying long-range transported free tropospheric particles with negligible influence from local emissions and rare contributions from the boundary layer. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origin and transport trajectories of sampled air masses and found that most originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis show that the sampled air masses were highly aged (average plume age > 10 days). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results show that the most abundant particle types were carbonaceous (~29.9 to 82.0 %), sea salt (~0.3 to 31.6 %), and sea salt with sulfate (~2.4 to 31.5 %). We used a tilted stage interfaced within an Environmental Scanning Electron Microscope (ESEM) to determine the phase state of individual submicron particles. We found that most particles (~47 to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed a substantial fraction of solid and semisolid particles (~0 to 30 % and ~1 to 42 %, respectively) during different transport patterns/events, reflecting the particles' phase state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would overestimate the viscosity of free tropospheric particles. Our findings warrant future investigation on the quantitative assessment of the influence of internal mixing on the phase state of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can benefit models to reduce uncertainties in ambient aerosol particles' effects on climate.

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.

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)

The Southern Ocean is a critical component of Earth’s climate system, but its remoteness makes it challenging to develop a holistic understanding of its processes from the small to the large scale. As a result, our knowledge of this vast region remains largely incomplete. The Antarctic Circumnavigation Expedition (ACE, austral summer 2016/2017) surveyed a large number of variables describing the dynamic state of the ocean and the atmosphere, the freshwater cycle, atmospheric chemistry, ocean biogeochemistry and microbiology. This circumpolar cruise included visits to twelve remote islands, the marginal ice zone, and the Antarctic coast. Here, we use 111 of the observed variables to study the latitudinal gradients, seasonality, shorter term variations, the geographic setting of environmental processes, and interactions between them over the duration of 90 days. To reduce the dimensionality and complexity of the dataset and make the relations between variables interpretable, we applied a sparse Principal Component Analysis (sPCA), which describes environmental processes through 14 latent variables. To derive a robust statistical perspective on these processes and to estimate the uncertainty in the sPCA decomposition, we have developed a bootstrap approach. We identified temporal patterns from diurnal to seasonal cycles, as well as geographical gradients and “hotspots” of interaction. Our results establish connections of oceanic, atmospheric, biological and terrestrial processes in an innovative way, while confirming many well known relations of the Southern Ocean system. More specifically, we identify: the important role of the oceanic circulations, frontal zones, and islands in shaping the nutrient availability that controls biological community composition and productivity; that sea ice predominantly controls sea water salinity, dampens the wave field, and is associated with increased phytoplankton growth and net community productivity possibly due to iron fertilization and reduced light limitation; and clear regional patterns of aerosol characteristics emerged, stressing the role of the sea state, atmospheric chemical processing, as well as source processes near “hotspots” for the availability of cloud condensation nuclei and hence cloud formation. A set of key variables and their combinations, such as the difference between the air and sea surface temperature, atmospheric pressure, sea surface height, geostrophic currents, upper ocean layer light intensity, surface wind speed and relative humidity, played an important role in the majority of latent variables, highlighting their importance for a large variety of processes and the necessity for Earth System Models to represent them adequately. In conclusion, our study highlights the use of sPCA to identify key ocean-atmosphere interactions across physical, chemical, and biological processes and their associated spatio-temporal scales. The sPCA processing code is available as open-access and we believe that our approach is widely applicable to other environmental field studies.

Concentrations of atmospheric ice nucleating particles (INP) were obtained from weekly filter samples which were collected from May 2019 until March 2020 in southern Chile. Sampling took place at an altitude of 620m above sea level, on top of Cerro Mirador, a mountain directly to the west of Punta Arenas (53°S, 71°W). Additional aerosol properties such as particle number size distributions were measured as well. In parallel, ground-based remote sensing measurements with lidar and cloud radar were made in Punta Arenas.INP concentrations were obtained from washing atmospheric aerosol particles off from deployed polycarbonate filters and subsequent analysis of the samples on two different freezing arrays which were used and described by us earlier (e.g., in Gong et al., 2019 and Hartmann et al., 2020). INP concentrations could be obtained over a broad temperature range from above -5°C down to -25°C.INP concentrations were clearly higher than data obtained for the Southern Ocean region as reported in McCluskey et al. (2018) and Welti et al. (2020). Indeed, they were comparable to concentrations measured at Cape Verde (Gong et al., 2020). INP concentrations obtained during the warm season were spreading over ~ 2 orders of magnitude at any temperature. Data obtained for the cold season almost all were at the upper end of the observed INP concentration range, with only one weekly sample featuring low concentrations.Heating of the samples was also applied, and the heated samples had clearly lower INP concentrations across the examined temperatures, implying a biological fraction among the INP of ~ 80%. Therefore, local terrestrial sources may be the source of the observed INP.The assumption of local terrestrial sources is strengthened by a case study. For that, two subsequent samples obtained during the cold season were examined in more detail. These were the one sample with low INP concentrations which was obtained during the cold season during the week from August 14 to August 22, and the subsequent sample collected from August 22 to August 29, which was amongst the highest samples. Backward trajectories together with an analysis of Lidar data showed that the low INP concentrations were obtained for a time during which air masses predominantly came in from the south with little contact to land and for calm weather conditions. Conditions were not as stable during the following week which featured air masses mostly coming in from the north-west. The aerosol backscatter coefficient at the height level of the in-situ measurements was obtained from lidar observations for both weeks and shows about 50 % lower aerosol load for the first week, when INP concentrations were low.All of this hints to local terrestrial sources for the observed highly ice active biogenic INP. Literature:Gong et al. (2019), Atmos. Chem. Phys., 19, 10883-10900, doi:10.5194/acp-19-10883-2019.Gong et al. (2020), Atmos. Chem. Phys., 20, 1451-1468, doi:10.5194/acp-20-1451-2020.Hartmann et al. (2020), Geophys. Res. Lett., 47, doi:10.1029/2020GL087770.McCluskey et al. (2018), Geophys. Res. Lett., 45, doi:10.1029/2018gl079981.Welti et a. (2020), Atmos. Chem. Phys. 20, doi:10.5194/acp-2020-466.

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.

Ambient concentrations of ice-forming particles measured during ship expeditions are collected and summarised with the aim of determining the spatial distribution and variability in ice nuclei in oceanic regions. The presented data from literature and previously unpublished data from over 23 months of ship-based measurements stretch from the Arctic to the Southern Ocean and include a circumnavigation of Antarctica. In comparison to continental observations, ship-based measurements of ambient ice nuclei show 1 to 2 orders of magnitude lower mean concentrations. To quantify the geographical variability in oceanic areas, the concentration range of potential ice nuclei in different climate zones is analysed by meridionally dividing the expedition tracks into tropical, temperate and polar climate zones. We find that concentrations of ice nuclei in these meridional zones follow temperature spectra with similar slopes but vary in absolute concentration. Typically, the frequency with which specific concentrations of ice nuclei are observed at a certain temperature follows a log-normal distribution. A consequence of the log-normal distribution is that the mean concentration is higher than the most frequently measured concentration. Finally, the potential contribution of ship exhaust to the measured ice nuclei concentration on board research vessels is analysed as function of temperature. We find a sharp onset of the influence at approximately −36 ∘C but none at warmer temperatures that could bias ship-based measurements.

Aerosol concentrations over Europe and Germany were simulated for the years 1985 and 2013 using the aerosol-chemistry transport model COSMO-MUSCAT. The aerosol fields from the two simulations were used in a high-resolution meteorological model for a sensitivity study on cloud properties. The modelled aerosol and cloud variables were compared to a variety of available observations, including satellites, remote sensing and in-situ observations. Finally, the radiative forcing of the aerosol could be estimated from the different sensitivity simulations.Due to reduction of emissions the ambient aerosol mass and number in Europe was strongly decreased since the 1980s. Hence, today’s number of particles in the CCN size range is smaller. The HD(CP)2 (High Definition Clouds and Precipitation for Climate Prediction) project amongst others aimed at analysing the effect of the emission reduction on cloud properties.As a pre-requiste, the aerosol mass, number, and composition over Germany were simulated for 1985 and 2013 using the regional chemistry-transport-model COSMO-MUSCAT. The EDGAR emission inventory was used for both years.The model results were compared to observations from the two HD(CP)2 campaigns that took place in 2013 (HOPE, HOPE-Melpitz) as well as the AVHRR aerosol optical thickness product, which is available from 1981 onwards. Despite the fact, that emissions of the 1980s are very uncertain, the modelled AOD is in good agreement with observations. The modelled mean CCN number concentration in 1985 is a factor of 2-4 higher than in 2013.Within HD(CP)2, the ICON weather forecast model was applied in a configuration allowing for large-eddy simulations. In these simulations, the time-varying CCN fields for the year 1985 and 2013 calculated with COSMO-MUSCAT were used as input for ICON-LEM. In the present-day simulation, the cloud droplet number agrees with observations, whereas the perturbed (1985) simulation does not with droplet numbers about twice as high as in 2013. Also, for other cloud variables systematic changes between the two scenarios were observed.

Aerosol measurements over the Southern Ocean are used to constrain aerosol-cloud interaction radiative forcing uncertainty in a global climate model. Aerosol forcing uncertainty is quantified using one million climate model variants that sample the uncertainty in nearly 30 model parameters. Ship-based measurements of cloud condensation nuclei, particle number concentrations and sulfate mass concentrations from the Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and Their Climate Effects (ACE-SPACE) are used to identify observationally implausible variants and thereby reduce the spread in the simulated forcing. Southern Ocean measurements strongly constrain natural aerosol emissions: default sea spray emissions in the model need to be increased by around a factor of 3 to be consistent with measurements. Aerosol forcing uncertainty is reduced by around 7 % using these measurements, which is comparable to the 8 % reduction achieved using an extensive set of over 9000 predominantly Northern Hemisphere measurements. The radiative forcing due to aerosol–cloud interactions (RFaci) is constrained to −2.61 to −1.10 W m−2 (95 % confidence) and the effective radiative forcing from aerosol-cloud interactions (ERFaci) is constrained to −2.43 to −0.54 W m−2. When Southern Ocean and Northern Hemisphere measurements are combined, the uncertainty in RFaci is reduced by 21 % and the strongest 20 % of forcing values are ruled out as implausible. In this combined constraint the observationally plausible RFaci is around 0.17 W m−2 weaker (less negative) with credible values ranging from −2.51 to −1.17 W m−2 and from −2.18 to −1.46 W m−2 when using one standard deviation to quantify the uncertainty. The Southern Ocean and Northern Hemisphere measurement datasets are complementary because they constrain different processes. These results highlight the value of remote marine aerosol measurements.

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.

Atmospheric aerosol particles are the precondition for the formation of cloud droplets and therefore have large influence on the microphysical and radiative properties of clouds. In this work, four different methods to derive or measure number concentrations of cloud condensation nuclei (CCN) were analyzed and compared for present-day aerosol conditions: (i) a model parameterization based on simulated particle concentrations, (ii) the same parameterization based on gravimetrical particle measurements, (iii) direct CCN measurements with a CCN counter, and (iv) lidar-derived and in situ measured vertical CCN profiles. In order to allow for sensitivity studies of the anthropogenic impact, a scenario to estimate the maximum CCN concentration under peak aerosol conditions of the mid-1980s in Europe was developed as well. In general, the simulations are in good agreement with the observations. At ground level, average values between 0.7 and 1.5×109 CCN m−3 at a supersaturation of 0.2 % were found with the different methods under present-day conditions. The discrimination of the chemical species revealed an almost equal contribution of ammonium sulfate and ammonium nitrate to the total number of CCN for present-day conditions. This was not the case for the peak aerosol scenario, in which it was assumed that no ammonium nitrate was formed while large amounts of sulfate were present, consuming all available ammonia during ammonium sulfate formation. The CCN number concentration at five different supersaturation values has been compared to the measurements. The discrepancies between model and in situ observations were lowest for the lowest (0.1 %) and highest supersaturations (0.7 %). For supersaturations between 0.3 % and 0.5 %, the model overestimated the potentially activated particle fraction by around 30 %. By comparing the simulation with observed profiles, the vertical distribution of the CCN concentration was found to be overestimated by up to a factor of 2 in the boundary layer. The analysis of the modern (year 2013) and the peak aerosol scenario (expected to be representative of the mid-1980s over Europe) resulted in a scaling factor, which was defined as the quotient of the average vertical profile of the peak aerosol and present-day CCN concentration. This factor was found to be around 2 close to the ground, increasing to around 3.5 between 2 and 5 km and approaching 1 (i.e., no difference between present-day and peak aerosol conditions) with further increasing height.

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 have been done 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 of 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. It 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 on Arctic cloud formation.

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.

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.

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.

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. The observations of basic meteorological parameters and particle number size distributions (PNSDs) were indicative for the rapid transition from Arctic spring to summer that took place during the measurement period. Two distinct types of air masses were found. One type were typical Arctic haze air masses, termed as spring-type air masses, characterized by a mono-modal 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 bi-modal 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 as summer-type air masses, originated from the northern Pacific. Generally total particle number concentrations (NCN) ranged from 20 to 500 cm−3, while cloud condensation nuclei (CCN) number concentrations were found to cover a range between 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 kappa 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 twenty times higher than those measured below 2000 m, and for one of these two flights, PNSDs measured above 2000 m showed a different shape than those measured at lower altitudes. This is indicative for long range transport from lower latitudes into the Arctic that can advect aerosol from different regions in different heights.

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.

Particle hygroscopic growth at 90% RH (relative humidity), cloud condensation nuclei (CCN) activity, and size-resolved chemical composition were concurrently measured in the Thüringer Wald mid-level mountain range in central Germany in the fall of 2010. The median hygroscopicity parameter values, κ, of 50, 75, 100, 150, 200, and 250 nm particles derived from hygroscopicity measurements are respectively 0.14, 0.14, 0.17, 0.21, 0.24, and 0.28 during the sampling period. The closure between HTDMA (Hygroscopicity Tandem Differential Mobility Analyzers)-measured (κHTDMA) and chemical composition-derived (κchem) hygroscopicity parameters was performed based on the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. Using size-averaged chemical composition, the κ values are substantially overpredicted (30 and 40% for 150 and 100 nm particles). Introducing size-resolved chemical composition substantially improved closure. We found that the evaporation of NH4NO3, which may happen in a HTDMA system, could lead to a discrepancy in predicted and measured particle hygroscopic growth. The hygroscopic parameter of the organic fraction, κorg, is positively correlated with the O : C ratio (κorg = 0.19 × (O : C) − 0.03). Such correlation is helpful to define the κorg value in the closure study. κ derived from CCN measurement was around 30% (varied with particle diameters) higher than that determined from particle hygroscopic growth measurements (here, hydrophilic mode is considered only). This difference might be explained by the surface tension effects, solution non-ideality, gas-particle partitioning of semivolatile compounds, and the partial solubility of constituents or non-dissolved particle matter. Therefore, extrapolating from HTDMA data to properties at the point of activation should be done with great care. Finally, closure study between CCNc (cloud condensation nucleus counter)-measured (κCCN) and chemical composition (κCCN, chem) was performed using CCNc-derived κ values for individual components. The results show that the κCCN can be well predicted using particle size-resolved chemical composition and the ZSR mixing rule.

The hygroscopic growth and droplet activation of uncoated soot particles and such coated with succinic acid and sulfuric acid were investigated during the IN-11 campaign at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) facility. A GFG-1000 soot generator applying either nitrogen or argon as carrier gas and a miniCAST soot generator were utilized to generate soot particles. Different organic carbon (OC) to black carbon (BC) ratios were adjusted for the CAST-soot by varying the fuel to air ratio. The hygroscopic growth was investigated by means of the mobile Leipzig Aerosol Cloud Interaction Simulator (LACIS-mobile) and two different Hygroscopicity Tandem Differential Mobility Analyzers (HTDMA, VHTDMA). Two Cloud Condensation Nucleus Counter (CCNC) were applied to measure the activation of the particles. For the untreated soot particles neither hygroscopic growth nor activation was observed at a supersaturation of 1%, with exception of a partial activation of GFG-soot generated with argon as carrier gas. Coatings of succinic acid lead to a detectable hygroscopic growth of GFG-soot and enhanced the activated fraction of GFG- (carrier gas: argon) and CAST-soot, whereas no hygroscopic growth of the coated CAST-soot was found. Sulfuric acid coatings led to an OC-content dependent hygroscopic growth of CAST-soot. Such a dependence was not observed for activation measurements. Coating with sulfuric acid decreased the amount of Polycyclic Aromatic Hydrocarbons (PAH), which were detected by AMS-measurements in the CAST-soot, and increased the amount of substances with lower molecular weight than the initial PAHs. We assume that these reaction products increased the hygroscopicity of the coated particles in addition to the coating substance itself.

Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP), which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A Cloud Condensation Nuclei (CCN) closure study is conducted with bulk CCN number concentration (NCCN) and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties. The observed CCN number concentration (NCCN-obs) are higher than those observed in other locations than China, with average NCCN-obs of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm) is calculated based on the NCCN-obs and aerosol number size distribution assuming homogeneous chemical composition. The inferred cut-off diameters are in the ranges of 190–280, 160–260, 95–180, 65–120 and 50–100 nm at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.7%, with their mean values 230.1, 198.4, 128.4, 86.4 and 69.2 nm, respectively. Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. The calculated CCN number concentrations (NCCN-calc) based on the size-resolved activation ratio and aerosol number size distribution correlate well with the NCCN-obs, and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the NCCN at each supersaturation is well predicted with the campaign average of size-resolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The CCN number concentration can be reliably estimated using time-averaged, size-resolved activation efficiencies without accounting for the temporal variations.

During the first Cloud and Aerosol Characterization Experiment (CLACE-1) in February and March 2000 various methods were used to characterize the aerosol at the high-alpine site Jungfraujoch, Switzerland (3580 m asl). One aim of the campaign was to perform the size-resolved chemical analysis of single particles under conditions of the free troposphere in real-time. Evaluation of single particle spectra measured predominantly in the size range between 0.5 and 5 μ m and determination of spectra patterns of the most frequent particle classes showed a great variability ranging from pure carbon particles over carbon particles internally mixed with salts and/or secondary components to mineral dust particles. Such mineral particles sometimes showed internal mixtures with carbon indicating scavenging effects of carbonaceous material by minerals. This can be due to coagulation or condensation of organic molecules on the mineral particles. Observation of internally mixed carbon particles is an indication for atmospheric transformation processes of pure carbon particles. Such internally mixed particles can strongly influence cloud formation due to an increase in particle size and hygroscopicity. High abundance of mineral and carbon-containing particles could be correlated to enhanced light absorption and light scattering coefficients, respectively. Semi-quantitative evaluation of mass spectra using relative sensitivity factors showed comparable ratios of selected ion pairs compared to bulk concentrations determined by ion chromatography.

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.

In a field campaign at the high-alpine site Jungfraujoch (JFJ, 3580 m asl), in-situ aerosol size distributions were measured simultaneously outdoor at ambient conditions (temperature T < −5 °C) and indoor at dry conditions ( T ≈ 25 °C and relative humidity RH < 10%) by means of two scanning mobility particle sizers (SMPS). In addition, measurements of hygroscopic growth factors were performed with a hygroscopicity tandem differential mobility analyzer (H-TDMA). The measured growth factors, being a monotonic function of the relative humidity (RH), were fitted with a modified Kohler model. A comparison between dry and ambient size distributions shows two main features: First, the dry total number concentration is often considerably smaller (on average 28%) than the ambient total number concentration, and is most likely due to the evaporation of volatile material at the higher temperature. These particle losses mainly concern small particles (dry diameter D ≲ 100 nm ), and therefore have only a minimal affect on the surface and volume concentrations. A slight correlation between ambient RH and the magnitude of particle loss was observed, but it was not possible to establish an empirical model for a quantification. Second, the dry number size distribution is shifted towards smaller particles, reflecting the hygroscopic behavior of the aerosols. To link the ambient and the dry size distributions we modeled this shift using the H-TDMA measurements and a modified Kohler model. The corrected dry surface and volume concentrations are in good agreement with the ambient measurements for the whole RH range, but the correction works best for RH < 80%. The results indicate that size distribution data measured at indoor conditions (i.e. dry and warm) may be successfully corrected to reflect ambient conditions, which are relevant for determining the impact of aerosol on climate. DOI: 10.1034/j.1600-0889.2003.00067.x

Microphysical and chemical aerosol properties and their influence on cloud formation were studied in a field campaign at the high-alpine site Jungfraujoch (JFJ, 3580 m asl). Due to its altitude, this site is suitable for ground-based in-cloud measurements, with a high cloud frequency of 40%. Dry total and interstitial aerosol size distributions [18 nm 100 nm) number concentration (Ntot,Dp>100) was only found for concentrations less than 100 cm−3. For higher values of Ntot,Dp>100 the D50 remained constant. Furthermore, a decrease of the effective radius of cloud droplets (Reff) with increasing Ntot,Dp>100 was observed, providing experimental evidence for the microphysical relation predicted by the Twomey effect. A modified Köhler model was used to quantify the critical supersaturation for the aerosol observed at the JFJ. Ambient supersaturations were determined from the derived supersaturation curve and the calculated D50. As an example, a critical supersaturation of 0.2% was found for 100 nm particles.DOI: 10.1034/j.1600-0889.2002.00299.x

Within the framework of the "Hill Cap Cloud Thuringia 2010" (HCCT-2010) international cloud experiment, the influence of cloud processing on the activation properties of ambient aerosol particles was investigated. Particles were probed upwind and downwind of an orographic cap cloud on Mt Schmücke, which is part of a large mountain ridge in Thuringia, Germany. The activation properties of the particles were investigated by means of size-segregated cloud condensation nuclei (CCN) measurements at 3 to 4 different supersaturations. The observed CCN spectra together with the total particle spectra were used to calculate the hygroscopicity parameter κ for the upwind and downwind stations. The upwind and downwind critical diameters and κ values were then compared for defined cloud events (FCE) and non-cloud events (NCE). Cloud processing was found to increase the hygroscopicity of the aerosol particles significantly, with an average increase in κ of 50%. Mass spectrometry analysis and isotopic analysis of the particles suggest that the observed increase in the hygroscopicity of the cloud-processed particles is due to an enrichment of sulfate and possibly also nitrate in the particle phase.

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.

The hygroscopic properties of submicron aerosol particles were determined at a suburban site (Wuqing) in the North China Plain among a cluster of cities during the period 17 July to 12 August 2009. A High Humidity Tandem Differential Mobility Analyser (HH-TDMA) instrument was applied to measure the hygroscopic growth factor (GF) at 90%, 95% and 98.5% relative humidity (RH) for particles with dry diameter between 50–250 nm. The probability distribution of GF (GF-PDF) averaged over the period shows a distinct bimodal pattern, namely, a dominant more-hygroscopic (MH) group and a smaller nearly-hydrophobic (NH) group. The MH group particles were highly hygroscopic, and their GF was relatively constant during the period with average values of 1.54±0.02, 1.81±0.04 and 2.45±0.07 at 90%, 95% and 98.5% RH (D0=100 nm), respectively. The NH group particles grew very slightly when exposed to high RH, with GF values of 1.08±0.02, 1.13±0.06 and 1.24±0.13, respectively at 90%, 95% and 98.5% RH (D0=100 nm). The hygroscopic growth behaviours at different RHs were well represented by the hygroscopicity parameter κ with a single-parameter Köhler model. Thus, the calculation of GF as a function of RH and dry diameter could be facilitated by an empirical parameterization of κ as function of dry diameter. A strong diurnal pattern in number fraction of different hygroscopic groups was observed, indicating a diurnal variation of aerosol mixing state and/or chemical composition. The average number fraction of NH particles during the day was about 8%, while during the nighttime fractions up to 20% were reached. Correspondingly, the state of mixing in terms of water uptake varied significantly during a day. The high fraction of NH particles measured during the night denotes a high degree of external mixing of ambient aerosols, while during the day the degree of external mixing decreased. Simulations using a particle-resolved aerosol box model (PartMC-MOSAIC) suggest that the diurnal variations of aerosol hygroscopicity and mixing state were mainly caused by the evolution of the atmospheric mixing layer. The shallow nocturnal boundary layer during the night facilitated the accumulation of freshly emitted carbonaceous particles (mainly hydrophobic) near the surface while in the morning turbulence entrained the more aged and more hygroscopic particles from aloft and diluted the NH particles near the surface resulting in a decrease in the fraction of NH particles.

Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP), which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A CCN (Cloud Condensation Nuclei) closure study is conducted with bulk CCN number concentration (NCCN) and calculated NCCN based on the aerosol number size distribution and size-resolved activation properties. The observed NCCN are higher than those observed in other locations than China, with average NCCN of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm) is calculated based on the measured NCCN and aerosol number size distribution assuming homogeneous chemical composition. This inferred cut off diameter varies in a wide range, indicating that it is impossible to predict NCCN with a fixed critical diameter. Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. This conclusion is confirmed by hygroscopicity measurements performed during two intensive field studies in 2009. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlate well with the measured NCCN, and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the NCCN for each supersaturation is well predicted with the campaign average of size-resolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The NCCN can be estimated with average activation curve, along with a well described aerosol number size distribution.