Mineral dusts originating from Earth’s crust are known to be important atmospheric ice nuclei. In agreement with earlier studies, feldspar was found as the most active of the tested natural mineral dusts. Here we investigated in closer detail the reasons for its activity and the difference in the activity of the different feldspars. Conclusions are drawn from scanning electron microscopy, X-ray powder diffraction, infrared spectroscopy, and oil-immersion freezing experiments. K-feldspar showed by far the highest ice nucleation activity. Finally, we give a potential explanation of this effect, finding alkali-metal ions having different hydration shells and thus an influence on the ice nucleation activity of feldspar surfaces.

The summertime Arctic lower troposphere is a relatively pristine background aerosol environment dominated by nucleation and Aitken mode particles. Understanding the mechanisms that control the formation and growth of aerosol is crucial for our ability to predict cloud properties and therefore radiative balance and climate. We present an analysis of an aerosol growth event observed in the Canadian Arctic Archipelago during summer as part of the NETCARE project. Under stable and clean atmospheric conditions, with low inversion heights, carbon monoxide less than 80aEuro-ppb(v), and black carbon less than 5aEuro-ngaEuro-m(-3), we observe growth of small particles, < aEuro-20aEuro-nm in diameter, into sizes above 50aEuro-nm. Aerosol growth was correlated with the presence of organic species, trimethylamine, and methanesulfonic acid (MSA) in particles similar to aEuro-80aEuro-nm and larger, where the organics are similar to those previously observed in marine settings. MSA-to-sulfate ratios as high as 0.15 were observed during aerosol growth, suggesting an important marine influence. The organic-rich aerosol contributes significantly to particles active as cloud condensation nuclei (CCN, supersaturationaEuro- = aEuro-0.6aEuro-%), which are elevated in concentration during aerosol growth above background levels of similar to 100 to similar to 220aEuro-cm(-3). Results from this case study highlight the potential importance of secondary organic aerosol formation and its role in growing nucleation mode aerosol into CCN-active sizes in this remote marine environment

Abstract. Observations addressing effects of aerosol particles on summertime Arctic clouds are limited. An airborne study, carried out during July 2014 from Resolute Bay, Nunavut, Canada, as part of the Canadian NETCARE project, provides a comprehensive in situ look into some effects of aerosol particles on liquid clouds in the clean environment of the Arctic summer. Median cloud droplet number concentrations (CDNC) from 62 cloud samples are 10 cm−3 for low-altitude cloud (clouds topped below 200 m) and 101 cm−3 for higher-altitude cloud (clouds based above 200 m). The lower activation size of aerosol particles is  ≤  50 nm diameter in about 40 % of the cases. Particles as small as 20 nm activated in the higher-altitude clouds consistent with higher supersaturations (S) for those clouds inferred from comparison of the CDNC with cloud condensation nucleus (CCN) measurements. Over 60 % of the low-altitude cloud samples fall into the CCN-limited regime of Mauritsen et al. (2011), within which increases in CDNC may increase liquid water and warm the surface. These first observations of that CCN-limited regime indicate a positive association of the liquid water content (LWC) and CDNC, but no association of either the CDNC or LWC with aerosol variations. Above the Mauritsen limit, where aerosol indirect cooling may result, changes in particles with diameters from 20 to 100 nm exert a relatively strong influence on the CDNC. Within this exceedingly clean environment, as defined by low carbon monoxide and low concentrations of larger particles, the background CDNC are estimated to range between 16 and 160 cm−3, where higher values are due to activation of particles  ≤  50 nm that likely derive from natural sources. These observations offer the first wide-ranging reference for the aerosol cloud albedo effect in the summertime Arctic.

Abstract. Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013. (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water (up to 75 nM) and the overlying atmosphere (up to 1 ppbv) in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source (with DMS concentrations of up to 6 nM and a potential contribution to atmospheric DMS of 20 % in the study area). (2) Evidence of widespread particle nucleation and growth in the marine boundary layer was found in the CAA in the summertime, with these events observed on 41 % of days in a 2016 cruise. As well, at Alert, Nunavut, particles that are newly formed and grown under conditions of minimal anthropogenic influence during the months of July and August are estimated to contribute 20 % to 80 % of the 30–50 nm particle number density. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from seabird-colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic aerosol (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds (OVOCs) were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol–climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms, with evidence for a dominant springtime contribution from eastern and southern Asia to the middle troposphere, and a major contribution from northern Asia to the surface. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow (0.03 cm s−1).

Abstract. Size-resolved and vertical profile measurements of single particle chemical composition (sampling altitude range 50-3000 m) were conducted in July 2014 in the Canadian high Arctic during an aircraft-based measurement campaign (NETCARE 2014). We deployed the single particle laser ablation aerosol mass spectrometer ALABAMA (vacuum aerodynamic diameter range approximately 200-1000 nm) to identify different particle types and their mixing states. On the basis of the single particle analysis, we found that a significant fraction (23 %) of all analyzed particles (in total: 7412) contained trimethylamine (TMA). Two main pieces of evidence suggest that these TMA-containing particles originated from emissions within the Arctic boundary layer. First, the maximum fraction of particulate TMA occurred in the Arctic boundary layer. Second, compared to particles observed aloft, TMA particles were smaller and less oxidized. Further, air mass history analysis, associated wind data and comparison with measurements of methanesulfonic acid give evidence of a marine-biogenic influence on particulate TMA. Moreover, the external mixture of TMAcontaining particles and sodium and chloride ("Na / Cl-") containing particles, together with low wind speeds, suggests particulate TMA results from secondary conversion of precursor gases released by the ocean. In contrast to TMAcontaining particles originating from inner-Arctic sources, particles with biomass burning markers (such as levoglucosan and potassium) showed a higher fraction at higher altitudes, indicating long-range transport as their source. Our measurements highlight the importance of natural, marine inner-Arctic sources for composition and growth of summertime Arctic aerosol.

Motivated by increasing levels of open ocean in the Arctic summer and the lack of prior altitude-resolved studies, extensive aerosol measurements were made during 11 flights of the NETCARE July 2014 airborne campaign from Resolute Bay, Nunavut. Flights included vertical profiles (60 to 3000 m above ground level) over open ocean, fast ice, and boundary layer clouds and fogs. A general conclusion, from observations of particle numbers between 5 and 20 nm in diameter (N5 − 20), is that ultrafine particle formation occurs readily in the Canadian high Arctic marine boundary layer, especially just above ocean and clouds, reaching values of a few thousand particles cm−3. By contrast, ultrafine particle concentrations are much lower in the free troposphere. Elevated levels of larger particles (for example, from 20 to 40 nm in size, N20 − 40) are sometimes associated with high N5 − 20, especially over low clouds, suggestive of aerosol growth. The number densities of particles greater than 40 nm in diameter (N >  40) are relatively depleted at the lowest altitudes, indicative of depositional processes that will lower the condensation sink and promote new particle formation. The number of cloud condensation nuclei (CCN; measured at 0.6 % supersaturation) are positively correlated with the numbers of small particles (down to roughly 30 nm), indicating that some fraction of these newly formed particles are capable of being involved in cloud activation. Given that the summertime marine Arctic is a biologically active region, it is important to better establish the links between emissions from the ocean and the formation and growth of ultrafine particles within this rapidly changing environment

Abstract. Black carbon (BC) contributes to Arctic warming, yet sources of Arctic BC and their geographic contributions remain uncertain. We interpret a series of recent airborne (NETCARE 2015; PAMARCMiP 2009 and 2011 campaigns) and ground-based measurements (at Alert, Barrow and Ny-Ålesund) from multiple methods (thermal, laser incandescence and light absorption) with the GEOS-Chem global chemical transport model and its adjoint to attribute the sources of Arctic BC. This is the first comparison with a chemical transport model of refractory BC (rBC) measurements at Alert. The springtime airborne measurements performed by the NETCARE campaign in 2015 and the PAMARCMiP campaigns in 2009 and 2011 offer BC vertical profiles extending to above 6 km across the Arctic and include profiles above Arctic ground monitoring stations. Our simulations with the addition of seasonally varying domestic heating and of gas flaring emissions are consistent with ground-based measurements of BC concentrations at Alert and Barrow in winter and spring (rRMSE < 13 %) and with airborne measurements of the BC vertical profile across the Arctic (rRMSE = 17 %) except for an underestimation in the middle troposphere (500-700 hPa).Sensitivity simulations suggest that anthropogenic emissions in eastern and southern Asia have the largest effect on the Arctic BC column burden both in spring (56 %) and annually (37 %), with the largest contribution in the middle troposphere (400-700 hPa). Anthropogenic emissions from northern Asia contribute considerable BC (27 % in spring and 43 % annually) to the lower troposphere (below 900 hPa). Biomass burning contributes 20 % to the Arctic BC column annually.At the Arctic surface, anthropogenic emissions from northern Asia (40-45 %) and eastern and southern Asia (20-40 %) are the largest BC contributors in winter and spring, followed by Europe (16-36 %). Biomass burning from North America is the most important contributor to all stations in summer, especially at Barrow.Our adjoint simulations indicate pronounced spatial heterogeneity in the contribution of emissions to the Arctic BC column concentrations, with noteworthy contributions from emissions in eastern China (15 %) and western Siberia (6.5 %). Although uncertain, gas flaring emissions from oilfields in western Siberia could have a striking impact (13 %) on Arctic BC loadings in January, comparable to the total influence of continental Europe and North America (6.5 % each in January). Emissions from as far as the Indo-Gangetic Plain could have a substantial influence (6.3 % annually) on Arctic BC as well.

Ship‐based aerosol measurements in the summertime Arctic indicate elevated concentrations of ultrafine particles with occasional growth to cloud condensation nuclei (CCN) sizes. Focusing on one episode with two continuously growing modes, growth occurs faster for a large, preexisting mode (dp ≈ 90 nm) than for a smaller nucleation mode (dp ≈ 20 nm). We use microphysical modeling to show that growth is largely via organic condensation. Unlike results for midlatitude forested regions, most of these condensing species behave as semivolatile organics, as lower volatility organics would lead to faster growth of the smaller mode. The magnitude of the CCN hygroscopicity parameter for the growing particles, ~0.1, is also consistent with organic species constituting a large fraction of the particle composition. Mixing ratios of common aerosol growth precursors, such as isoprene and sulfur dioxide, are not elevated during the episode, indicating that an unidentified aerosol growth precursor is present in this high‐latitude marine environment.