In the central Arctic Ocean the formation of clouds and their properties are sensitive to the availability of cloud condensation nuclei (CCN). The vapors responsible for new particle formation (NPF), potentially leading to CCN, have remained unidentified since the first aerosol measurements in 1991. Here, we report that all the observed NPF events from the Arctic Ocean 2018 expedition are driven by iodic acid with little contribution from sulfuric acid. Iodic acid largely explains the growth of ultrafine particles (UFP) in most events. The iodic acid concentration increases significantly from summer towards autumn, possibly linked to the ocean freeze-up and a seasonal rise in ozone. This leads to a one order of magnitude higher UFP concentration in autumn. Measurements of cloud residuals suggest that particles smaller than 30 nm in diameter can activate as CCN. Therefore, iodine NPF has the potential to influence cloud properties over the Arctic Ocean.

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 help 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; length of 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, and 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.

Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W) in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS), was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA) profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass), a methanesulfonic acid OA factor (MSA-OA, 25%), a marine oxygenated OA factor (M-OOA, 41%), a sea spray OA fraction (SS-OA, 7%) and locally produced hydrocarbon-like OA (HOA, 9%). The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13), has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA). However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not associated with sea salt particles during 19% of the time, indicating the presence of biogenic particles in addition to the MSA-OA and AA-OA factors

Abstract. Lineshaped contrails were detected with the research aircraft Falcon during the CONCERT -CONtrail and Cirrus ExpeRimenT -campaign in October/November 2008. The Falcon was equipped with a set of instruments to measure the particle size distribution, shape, extinction and chemical composition as well as trace gas mixing ratios of sulfur dioxide (SO 2 ), reactive nitrogen and halogen species (NO, NO y , HNO 3 , HONO, HCl), ozone (O 3 ) and carbon monoxide (CO). During 12 mission flights over Europe, numerous contrails, cirrus clouds and a volcanic aerosol layer were probed at altitudes between 8.5 and 11.6 km and at temperatures above 213 K. 22 contrails from 11 different aircraft were observed near and below ice saturation. The observed NO mixing ratios, ice crystal and soot number densities are compared to a process based contrail model. On 19 November 2008 the contrail from a CRJ-2 aircraft was penetrated in 10.1 km altitude at a temperature of 221 K. The contrail had mean ice crystal number densities of 125 cm −3 with effective radii r eff of 2.6 µm. The presence of particles with r>50 µm in the less than 2 min old contrail suggests that natural cirrus crystals were entrained in the contrail. Mean HONO/NO (HONO/NO y ) ratios of 0.037 (0.024) and the fuel sulfur conCorrespondence to: C. Voigt (christiane.voigt@dlr.de) version efficiency to H 2 SO 4 ( S↓ ) of 2.9 % observed in the CRJ-2 contrail are in the range of previous measurements in the gaseous aircraft exhaust. On 31 October 2010 aviation NO emissions could have contributed by more than 40% to the regional scale NO levels in the mid-latitude lowest stratosphere. The CONCERT observations help to better quantify the climate impact from contrails and will be used to investigate the chemical processing of trace gases on contrails.

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

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Light‐absorbing impurities (LAIs) in snow of the southeastern Tibetan Plateau (TP) and their climatic impacts are of interest not only because this region borders areas affected by the South Asian atmospheric brown clouds but also because the seasonal snow and glacier melt from this region form important headwaters of large rivers. In this study, we collected surface snow and snowpit samples from four glaciers in the southeastern TP in June 2015 to investigate the comprehensive observational data set of LAIs. Results showed that the LAI concentrations were much higher in the aged snow and granular ice than in the fresh snow and snowpits due to postdepositional processes. Impurity concentrations fluctuated across snowpits, with maximum LAI concentrations frequently occurring toward the bottom of snowpits. Based on the SNow ICe Aerosol Radiative model, the albedo simulation indicated that black carbon and dust account for approximately 20% of the albedo reduction relative to clean snow. The radiative forcing caused by black carbon and dust deposition on the glaciers were between 1.0–141 W m−2 and 1.5–120 W m−2, respectively. Black carbon (BC) played a larger role in albedo reduction and radiative forcing than dust in the study area, enhancing approximately 15% of glacier melt. Analysis based on the Fire INventory from NCAR indicated that nonbiomass‐burning sources of BC played an important role in the total BC deposition, especially during the monsoon season. This study suggests that eliminating anthropogenic BC could mitigate glacier melt in the future of the southeastern TP.

Air pollution in the Arctic caused by local emission sources is a challenge that is important but often overlooked. Local Arctic air pollution can be severe and significantly exceed air quality standards, impairing public health and affecting ecosystems. Specifically in the wintertime, pollution can accumulate under inversion layers. However, neither the contributing emission sources are well identified and quantified nor the relevant atmospheric mechanisms forming pollution are well understood. In the summer, boreal forest fires cause high levels of atmospheric pollution. Despite the often high exposure to air pollution, there are neither specific epidemiological nor toxicological health impact studies in the Arctic. Hence, effects on the local population are difficult to estimate at present. Socioeconomic development of the Arctic is already occurring and expected to be significant in the future. Arctic destination shipping is likely to increase with the development of natural resource extraction, and tourism might expand. Such development will not only lead to growth in the population living in the Arctic but will likely increase emission types and magnitudes. Present‐day inventories show a large spread in the amount and location of emissions representing a significant source of uncertainty in model predictions that often deviate significantly from observations. This is a challenge for modeling studies that aim to assess the impacts of within Arctic air pollution. Prognoses for the future are hence even more difficult, given the additional uncertainty of estimating emissions based on future Arctic economic development scenarios.