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Dimethylamine (DMA) has a stabilizing effect on sulfuric acid (SA) clusters, and the SA and DMA molecules and clusters likely play important roles in both aerosol particle formation and growth in the atmosphere. We use the monodisperse particle growth model for acid-base chemistry in nanoparticle growth (MABNAG) together with direct and indirect observations from the CLOUD4 and CLOUD7 experiments in the cosmics leaving outdoor droplets (CLOUD) chamber at CERN to investigate the size and composition evolution of freshly formed particles consisting of SA, DMA, and water as they grow to 20 nm in dry diameter. Hygroscopic growth factors are measured using a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA), which combined with simulations of particle water uptake using the thermodynamic extended-aerosol inorganics model (E-AIM) constrain the chemical composition. MABNAG predicts a particle-phase ratio between DMA and SA molecules of 1.1–1.3 for a 2 nm particle and DMA gas-phase mi...

The Arctic region is warming considerably faster than the rest of the globe(1), with important consequences for the ecosystems(2) and human exploration of the region(3). However, the reasons behind ...

The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change–cryosphere interactions that affect Arctic amplification., The CRAICC team acknowledges the following institutions for financial support: the Finnish Cultural Foundation grant, Markku Kulmala “International Working Groups”; Russian mega-grant no. 11.G34.31.0048 (University of Nizhny Novgorod); Academy of Finland contracts 259537, 257411, and 254195; Beautiful Beijing (Finland–China collaboration project) funded by TEKES; Nordforsk CRAICC-PEEX (amendment to contract 26060); CRAICC-CRUCIAL (project no. 81257); Icelandic Research Fund (Rannis) grant no. 152248-051; Danish Environmental Protection Agency with means from the Dancea fund for environmental support to the Arctic region (M 112 002700); the Villum Foundation; the Carlsberg Foundation (project 009_1_0515); COST1303 (TOPROF); COST ES1404 (HarmoSnow); and the Pan-Eurasian Experiment (PEEX). The development and use of NorESM1 was supported by the Norwegian Research Council through the projects EarthClim (207711/E10), EVA (grant no. 229771), NOTUR (nn2345k), and NorStore (ns2345k) and through the Nordic Centre of Excellence eSTICC (57001) and the EU H2020 project CRESCENDO (grant no. 641816). The CRAICC team also thanks Rogier Floors for providing Fig. 8 and Christoph Münkel for Fig. 9. The authors and entire CRAICC community would like to thank and acknowledge the work and inspiration of Jon Egill Kristjansson, whose life was cut short during these collaborations. Jon Egill Kristjansson is deeply missed, but his scientific legacy continues.

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH‐dependent SOA water‐uptake with solubility and phase separation; (2) show that laboratory data on IP‐ and MT‐SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single‐parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources., Key Points Phase separation effects explain differences in water affinity of biogenic secondary organic aerosol (SOA) at subsaturation and supersaturationLaboratory data for monoterpene and isoprene SOA are representative of field observations with corresponding gas‐phase organic profilesImportance of organic aerosol‐water interactions for global climate is governed by highly uncertain organic aerosol budgets

We have developed an inorganic sea spray source function that is based upon state-of-the-art measurements of sea spray aerosol production using a temperature-controlled plunging jet sea spray aerosol chamber. The size-resolved particle production was measured between 0.01 and 10 μm dry diameter. Particle production decreased non-linearly with increasing seawater temperature (between −1 and 30 °C) similar to previous findings. In addition, we observed that the particle effective radius, as well as the particle surface, particle volume and particle mass, increased with increasing seawater temperature due to increased production of particles with dry diameters greater than 1 μm. By combining these measurements with the volume of air entrained by the plunging jet we have determined the size-resolved particle flux as a function of air entrainment. Through the use of existing parameterisations of air entrainment as a function of wind speed, we were subsequently able to scale our laboratory measurements of particle production to wind speed. By scaling in this way we avoid some of the difficulties associated with defining the "white area" of the laboratory whitecap – a contentious issue when relating laboratory measurements of particle production to oceanic whitecaps using the more frequently applied whitecap method. The here-derived inorganic sea spray source function was implemented in a Lagrangian particle dispersion model (FLEXPART – FLEXible PARTicle dispersion model). An estimated annual global flux of inorganic sea spray aerosol of 5.9 ± 0.2 Pg yr−1 was derived that is close to the median of estimates from the same model using a wide range of existing sea spray source functions. When using the source function derived here, the model also showed good skill in predicting measurements of Na+ concentration at a number of field sites further underlining the validity of our source function. In a final step, the sensitivity of a large-scale model (NorESM – the Norwegian Earth System Model) to our new source function was tested. Compared to the previously implemented parameterisation, a clear decrease of sea spray aerosol number flux and increase in aerosol residence time was observed, especially over the Southern Ocean. At the same time an increase in aerosol optical depth due to an increase in the number of particles with optically relevant sizes was found. That there were noticeable regional differences may have important implications for aerosol optical properties and number concentrations, subsequently also affecting the indirect radiative forcing by non-sea spray anthropogenic aerosols.

Emissions of biogenic volatile organic compounds (BVOC) have changed in the past millennium due to changes in land use, temperature and CO2 concentrations. Recent model reconstructions of BVOC emissions over the past millennium predicted changes in dominant secondary organic aerosol (SOA) producing BVOC classes (isoprene, monoterpenes and sesquiterpenes). The reconstructions predicted that global isoprene emissions have decreased (land-use changes to crop/grazing land dominate the reduction), while monoterpene and sesquiterpene emissions have increased (temperature increases dominate the increases); however, all three show regional variability due to competition between the various influencing factors. These BVOC changes have largely been anthropogenic in nature, and land-use change was shown to have the most dramatic effect by decreasing isoprene emissions. In this work, we use two modeled estimates of BVOC emissions from the years 1000 to 2000 to test the effect of anthropogenic changes to BVOC emissions on SOA formation, global aerosol size distributions, and radiative effects using the GEOS-Chem-TOMAS global aerosol microphysics model. With anthropogenic emissions (e.g. SO2, NOx, primary aerosols) held at present day values and BVOC emissions changed from year 1000 to year 2000 values, decreases in the number concentration of particles of size Dp > 80 nm (N80) of >25% in year 2000 relative to year 1000 were predicted in regions with extensive land-use changes since year 1000 which led to regional increases in direct plus indirect aerosol radiative effect of >0.5 W m−2 in these regions. We test the sensitivity of our results to BVOC emissions inventory, SOA yields and the presence of anthropogenic emissions; however, the qualitative response of the model to historic BVOC changes remains the same in all cases. Accounting for these uncertainties, we estimate millennial changes in BVOC emissions cause a global mean direct effect of between +0.022 and +0.163 W m−2 and the global mean cloud-albedo aerosol indirect effect of between −0.008 and −0.056 W m−2. This change in aerosols, and the associated radiative forcing, could be a~largely overlooked and important anthropogenic aerosol effect on regional climates.

We investigated the millennial variability (1000 A.D.–2000 A.D.) of global biogenic volatile organic compound (BVOC) emissions by using two independent numerical models: The Model of Emissions of Gases and Aerosols from Nature (MEGAN), for isoprene, monoterpene, and sesquiterpene, and Lund-Potsdam-Jena-General Ecosystem Simulator (LPJ-GUESS), for isoprene and monoterpenes. We found the millennial trends of global isoprene emissions to be mostly affected by land cover and atmospheric carbon dioxide changes, whereas monoterpene and sesquiterpene emission trends were dominated by temperature change. Isoprene emissions declined substantially in regions with large and rapid land cover change. In addition, isoprene emission sensitivity to drought proved to have significant short-term global effects. By the end of the past millennium MEGAN isoprene emissions were 634 TgC yr−1 (13% and 19% less than during 1750–1850 and 1000–1200, respectively), and LPJ-GUESS emissions were 323 TgC yr−1 (15% and 20% less than during 1750–1850 and 1000–1200, respectively). Monoterpene emissions were 89 TgC yr−1 (10% and 6% higher than during 1750–1850 and 1000–1200, respectively) in MEGAN, and 24 TgC yr−1 (2% higher and 5% less than during 1750–1850 and 1000–1200, respectively) in LPJ-GUESS. MEGAN sesquiterpene emissions were 36 TgC yr−1 (10% and 4% higher than during 1750–1850 and 1000–1200, respectively). Although both models capture similar emission trends, the magnitude of the emissions are different. This highlights the importance of building better constraints on VOC emissions from terrestrial vegetation.

Nature Geoscience 9, 277–281 (2016); published online 14 March 2016; corrected after print 5 May 2016. In the version of the Letter originally published, the following reference was mistakenly omitted: 27. Yang, Q., Bitz, C. M. & Doherty, S. J. Offsetting effects of aerosols on Arctic and globalclimate in the late 20th century.