A likely important feature of the poorly understood aerosol‐cloud interactions over the Southern Ocean (SO) is the dominant role of sea spray aerosol, versus terrestrial aerosol. Ice nucleating particles (INPs), or particles required for heterogeneous ice nucleation, present over the SO have not been studied in several decades. In this study, boundary layer aerosol properties and immersion freezing INP number concentrations (nINPs) were measured during a ship campaign that occurred south of Australia (down to 53°S) in March–April 2016. Ocean surface chlorophyll a concentrations ranged from 0.11 to 1.77 mg/m3, and nINPs were a factor of 100 lower than historical surveys, ranging from 0.38 to 4.6 m−3 at −20 °C. The INP population included organic heat‐stable material, with contributions from heat‐labile material. Lower INP source potentials of SO seawater samples compared to Arctic seawater were consistent with lower ice nucleating site densities in this study compared to north Atlantic air masses.

A B S T R A C T Two-point radon gradients provide a direct, unambiguous measure of near-surface atmospheric mixing. A 31-month data set of hourly radon measurements at 2 and 50 m is used to characterize the seasonality and diurnal variability of radon concentrations and gradients at a site near Sydney. Vertical differencing allows separation of remote (fetchrelated) effects on measured radon concentrations from those due to diurnal variations in the strength and extent of vertical mixing. Diurnal composites, grouped according to the maximum nocturnal radon gradient ( C max ), reveal strong connections between radon, wind, temperature and mixing depth on subdiurnal timescales. Comparison of the bulk Richardson Number (Ri B ) and the turbulence kinetic energy (TKE) with the radon-derived bulk diffusivity (K B ) helps to elucidate the relationship between thermal stability, turbulence intensity and the resultant mixing. On nights with large C max , K B and TKE levels are low and Ri B is well above the 'critical' value. Conversely, when C max is small, K B and TKE levels are high and Ri B is near zero. For intermediate C max , however, Ri B remains small whereas TKE and K B both indicate significantly reduced mixing. The relationship between stability and turbulence is therefore non-linear, with even mildly stable conditions being sufficient to suppress mixing.

Radon (222Rn) is a powerful natural tracer of mixing and exchange processes in the atmospheric boundary layer. The authors present and discuss the main features of a unique dataset of 50 high-resolution vertical radon profiles up to 3500 m above ground level, obtained in clear and cloudy daytime terrestrial boundary layers over an inland rural site in Australia using an instrumented motorized research glider. It is demonstrated that boundary layer radon profiles frequently exhibit a complex layered structure as a result of mixing and exchange processes of varying strengths and extents working in clear and cloudy conditions within the context of the diurnal cycle and the synoptic meteorology. Normalized aircraft radon measurements are presented, revealing the characteristic structure and variability of three major classes of daytime boundary layer: 1) dry convective boundary layers, 2) mixed layers topped with residual layers, and 3) convective boundary layers topped with coupled nonprecipitating clouds. Robust and unambiguous signatures of important atmospheric processes in the boundary layer are identifiable in the radon profiles, including “top-down” mixing associated with entrainment in clear-sky cases and strongly enhanced venting and subcloud-layer mixing when substantial active cumulus are present. In poorly mixed conditions, radon gradients in the daytime atmospheric surface layer significantly exceed those predicted by Monin–Obukhov similarity theory. In two case studies, it is demonstrated for the first time that a sequence of vertical radon profiles measured over the course of a single day can consistently reproduce major structural features of the evolving boundary layer.

Vertical mixing of the nocturnal stable boundary layer (SBL) over a complex land surface is investigated for a range of stabilities, using a decoupling index (0 < D rb < 1) based on the 2-50 m bulk gradient of the ubiquitous natural trace gas radon-222. The relationship between D rb and the bulk Richardson number (R ib ) exhibits three broad regions: (1) a well-mixed region (D rb ≈ 0.05) in weakly stable conditions (R ib < 0.03); (2) a steeply increasing region (0.05 < D rb < 0.9) for "transitional" stabilities (0.03 < R ib < 1); and (3) a decoupled region (D rb ≈ 0.9-1.0) in very stable conditions (R ib > 1). D rb exhibits a large variability within individual R ib bins, however, due to a range of competing processes influencing bulk mixing under different conditions. To explore these processes in R ib -D rb space, we perform a bivariate analysis of the bulk thermodynamic gradients, various indicators of external influences, and key turbulence quantities at 10 and 50 m. Strong and consistent patterns are found, and five distinct regions in R ib -D rb space are identified and associated with archetypal stable boundary-layer regimes. Results demonstrate that the introduction of a scalar decoupling index yields valuable information about turbulent mixing in the SBL that cannot be gained directly from a single bulk thermodynamic stability parameter. A significant part of the high variability observed in turbulence statistics during very stable conditions is attributable to changes in the degree of decoupling of the SBL from the residual layer above. When examined in R ib -D rb space, it is seen that very different turbulence regimes can occur for the same value of R ib , depending on the particular combination of values for the bulk temperature gradient and wind shear, together with external factors. Extremely low turbulent variances and fluxes are found at 50 m height when R ib > 1 and D rb ≈ 1 (fully decoupled). These "quiescent" cases tend to occur when geostrophic forcing is very weak and subsidence is present, but are not associated with the largest bulk temperature gradients. Humidity and net radiation data indicate the presence of low cloud, patchy fog or dew, any of which may aid decoupling in these cases by preventing temperature gradients from increasing sufficiently to favour gravity wave activity. The largest temperature gradients in our dataset are actually associated with smaller values of the decoupling index (D rb < 0.7), indicating the presence of mixing. Strong evidence is seen from enhanced turbulence levels, fluxes and submeso activity at 50 m, as well as high temperature variances and heat flux intermittencies at 10 m, suggesting this region of the R ib -D rb distribution can be identified as a top-down mixing regime. This may indicate an important role for gravity waves and other wave-like phenomena in providing the energy required for sporadic mixing at this complex terrain site.

Abstract. We have integrated the atmospheric chemistry and transport model TM5 into the global climate model EC-Earth version 2.4. We present an overview of the TM5 model and the two-way data exchange between TM5 and the IFS model from the European Centre for Medium-Range Weather Forecasts (ECMWF), the atmospheric general circulation model of EC-Earth. In this paper we evaluate the simulation of tropospheric chemistry and aerosols in a oneway coupled configuration. We have carried out a decadal simulation for present-day conditions and calculated chemical budgets and climatologies of tracer concentrations and aerosol optical depth. For comparison we have also performed offline simulations driven by meteorological fields from ECMWF's ERA-Interim reanalysis and output from the EC-Earth model itself. Compared to the offline simulations, the online-coupled system produces more efficient vertical mixing in the troposphere, which reflects an improvement of the treatment of cumulus convection. The chemistry in the EC-Earth simulations is affected by the fact that the current version of EC-Earth produces a cold bias with too dry air in large parts of the troposphere. Compared to the ERA-Interim driven simulation, the oxidizing capacity in EC-Earth is lower in the tropics and higher in the extratropics. The atmospheric lifetime of methane in EC-Earth is 9.4 years, which is 7 % longer than the lifetime obtained with ERA-Interim but remains well within the range reported in the literature. We further evaluate the model by comparing the simulated climatologies of surface radon-222 and carbon monoxide, tropospheric and surface ozone, and aerosol optical depth against observational data. The work presented in this study is the first step in the development of EC-Earth into an Earth system model with fully interactive atmospheric chemistry and aerosols.