Julia Burkart

Identification of ice nucleation active sites on feldspar dust particles.

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.

Evidence for marine biogenic influence on summertime Arctic aerosol

We present vertically-resolved observations of aerosol composition during pristine summertime Arctic background conditions. The methansulfonic acid (MSA)-to-sulfate ratio peaked near the surface (mean 0.10), indicating a contribution from ocean-derived biogenic sulfur. Similarly, the organic aerosol (OA)-to-sulfate ratio increased towards the surface (mean 2.0). Both MSA-to-sulfate and OA-to-sulfate ratios were significantly correlated with FLEXPART-WRF-predicted airmass residence time over open water, indicating marine influenced OA. External mixing of sea salt aerosol from a larger number fraction of organic, sulfate and amine-containing particles, together with low wind speeds (median 4.7 m s−1), suggests a role for secondary organic aerosol formation. Cloud condensation nuclei concentrations were nearly constant (∼120 cm−3) when the OA fraction was <60% and increased to 350 cm−3 when the organic fraction was larger and residence times over open water were longer. Our observations illustrate the importance of marine-influenced OA under Arctic background conditions, which are likely to change as the Arctic transitions to larger areas of open water.

Organic condensation and particle growth to CCN sizes in the summertime marine Arctic is driven by materials more semi-volatile than at continental sites

Ship-based aerosol measurements in the summertime Arctic indicate elevated concentrations of ultrafine particles with occasional growth to CCN sizes. Focusing on one episode with two continuously growing modes, growth occurs faster for a large, pre-existing 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 mid-latitude forested regions, most of these condensing species behave as semi-volatile 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.

Size-resolved mixing state of black carbon in the Canadian high Arctic and implications for simulated direct radiative effect

Transport of anthropogenic aerosol into the Arctic in the spring months has the potential to affect regional climate; however, modeling estimates of the aerosol direct radiative effect (DRE) are sensitive to uncertainties in the mixing state of black carbon (BC). A common approach in previous modeling studies is to assume an entirely external mixture (all primarily 15 scattering species are in separate particles from BC) or internal mixture (all primarily scattering species are mixed in the same particles as BC). To provide constraints on the size-resolved mixing state of BC, we use airborne Single Particle Soot Photometer (SP2) and Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) measurements from the Alfred Wegener Institute (AWI) POLAR6 flights from the NETCARE/PAMARCMIP2015 campaign to estimate coating thickness as a function of refractory BC (rBC) core diameter as well as the fraction of particles containing rBC in the springtime Canadian 20 high Arctic. For rBC core diameters in the range of 140 to 220 nm, we find average coating thicknesses of approximately 45 to 40 nm, respectively, resulting in ratios of total particle diameter to rBC core diameters ranging from 1.6 to 1.4. For total particle diameters ranging from 175 to 730 nm, rBC-containing particle number fractions range from 16 to 3%, respectively. We combine the observed mixing-state constraints with simulated size-resolved aerosol mass and number distributions from GEOS-Chem-TOMAS to estimate the DRE with observed bounds on mixing state as opposed to assuming an entirely 25 external or internal mixture. We find that the pan-Arctic average springtime DRE ranges from -1.65 W m to -1.34 W m when assuming entirely externally or internally mixed BC. Using the observed mixing-state constraints, we find the DRE is 0.05 W m and 0.19 W m less negative than the external mixing-state assumption when constraining by coating thickness of the mixed particles and by BC-containing particle number fraction, respectively. The difference between these methods is due to an underestimation of BC mass fraction in the springtime Arctic in GEOS-Chem-TOMAS compared to POLAR6 30 observations. Measurements of mixing state provide important constraints for model estimates of DRE. Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-171 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 19 February 2018 c

Modelling Regional Air Quality in the Canadian Arctic: Simulation of an Arctic Summer Field Campaign

Model simulations of an Arctic summer field campaign were carried out. The model results were compared with observational data from both ground-based monitoring and in situ measurements on-board multiple mobile platforms. The model was able to well capture regional sources and transport affecting the Arctic air quality. It is shown that the study area was impacted by North American (NA) regional biomass burning emissions. The model-observation comparison also corroborates previous findings on possible roles of marine-biogenic sources in aerosol production in the Arctic MBL during summertime.