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 Arc- tic 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 exter- nal mixture (all primarily scattering species are in separate particles from BC) or internal mixture (all primarily scat- tering 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 ultrahigh-sensitivity aerosol spectrometer (UHSAS) mea- surements from the Alfred Wegener Institute (AWI) Polar 6 flights from the NETCARE/PAMARCMIP2015 campaign to estimate coating thickness as a function of refractory BC (rBC) core diameter and the fraction of particles contain- ing rBC in the springtime Canadian high Arctic. For rBC core diameters in the range of 140 to 220 nm, we find av- erage coating thicknesses of approximately 45 to 40 nm, re- spectively, resulting in ratios of total particle diameter to rBC core diameters ranging from 1.6 to 1.4. For total par- ticle diameters ranging from 175 to 730 nm, rBC-containing particle number fractions range from 16% to 3%, respec- tively. We combine the observed mixing-state constraints with simulated size-resolved aerosol mass and number dis- tributions from GEOS-Chem–TOMAS to estimate the DRE with observed bounds on mixing state as opposed to assuming an entirely external or internal mixture. We find that the pan-Arctic average springtime DRE ranges fro