Abstract.A GLObal Model of Aerosol Processes (GLOMAP) has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN >3 nm) vary between about 250-500 cm −3 in remote marine boundary layer regions and are generally in good agreement with observations. Modelled continental CN concentrations are lower than observed, which may be due to lack of some primary aerosol sources or the neglect of nucleation mechanisms other than binary homogeneous nucleation of sulfuric acidwater particles. Remote marine CN concentrations increase to around 2000-10 000 cm −3 (at standard temperature and pressure) in the upper troposphere, which agrees with typical observed vertical profiles. Cloud condensation nuclei (CCN) at 0.2% supersaturation vary between about 1000 cm −3 in polluted regions and between 10 and 500 cm −3 in the remote marine boundary layer. New particle formation through sulfuric acid-water binary nucleation occurs predominantly in the upper troposphere, but the model results show that these particles contribute greatly to aerosol concentrations in the marine boundary layer. For this sulfur-sea salt system it is estimated that sea spray emissions account for only ∼10% of CCN in the tropical marine boundary layer, but between 20 and 75% in the mid-latitude Southern Ocean. In a run with only natural sulfate and sea salt emissions the global mean surface CN concentration is more than 60% of that from a run Correspondence to: D. V. Spracklen (dominick@env.leeds.ac.uk) with 1985 anthropogenic sulfur emissions, although the natural emissions comprise only 27% of total sulfur emissions. Southern hemisphere marine boundary layer CN are more than 90% natural in origin, while polluted continental CN are more than 90% anthropogenic in origin, although these numbers will change when other anthropogenic CN sources are included in the model.

Abstract. Cloud condensation nuclei (CCN) are derived from particles emitted directly into the atmosphere (primary emissions) or from the growth of nanometer-sized particles nucleated in the atmosphere. It is important to separate these two sources because they respond in different ways to gas and particle emission control strategies and environmental changes. Here, we use a global aerosol microphysics model to quantify the contribution of primary and nucleated particles to global CCN. The model considers primary emissions of sea spray, sulfate and carbonaceous particles, and nucleation processes appropriate for the free troposphere and boundary layer. We estimate that 45% of global low-level cloud CCN at 0.2% supersaturation are secondary aerosol derived from nucleation (ranging between 31–49% taking into account uncertainties primary emissions and nucleation rates), the remainder being directly emitted as primary aerosol. The model suggests that 35% of CCN (0.2%) in low-level clouds were created in the free and upper troposphere. In the marine boundary layer 55% of CCN (0.2%) are from nucleation, 45% being entrained from the free troposphere. Both in global and marine boundary layer 10% of CCN (0.2%) is nucleated in the boundary layer. Combinations of model runs show that primary and nucleated CCN are non-linearly coupled. In particular, boundary layer nucleated CCN are strongly suppressed by both primary emissions and entrainment of particles nucleated in the free troposphere. Elimination of all primary emissions reduces global CCN (0.2%) by only 20% and elimination of upper tropospheric nucleation reduces CCN (0.2%) by only 12% because of increased impact of boundary layer nucleation on CCN.

Abstract. Polar stratospheric clouds (PSCs) of type 1a or 1a-enh containing high number densities of nitric acid trihydrate (NAT) particles, can act as mother clouds for extremely large NAT particles, termed NAT-rocks, provided the air below the clouds is supersaturated with respect to NAT. Individual NAT particles at the cloud base fall into undepleted gas phase and rapidly accelerate due to a positive feedback between their growth and sedimentation. The resulting reduction in number density is further enhanced by the strong HNO 3 depletion within a thin layer below the mother cloud, which delays subsequent particles. This paper introduces the basic microphysical principles behind this mother cloud/NAT-rock mechanism, which produces 10 −4 cm −3 NAT-rocks with radii around 10 µm some kilometers below the mother cloud. The mechanism does not require selective nucleation and works even for a monodisperse particle size distribution in the mother cloud.

Abstract. Convective cloud systems in the maritime tropics play a critical role in global climate, but accurately representing aerosol interactions within these clouds persists as a major challenge for weather and climate modelling. We quantify the effect of ice-nucleating particles (INPs) on the radiative properties of a complex tropical Atlantic deep convective cloud field using a regional model with an advanced double-moment microphysics scheme. Our results show that the domain-mean daylight outgoing radiation varies by up to 18 W m−2 depending on the chosen INP parameterisation. The key distinction between different INP parameterisations is the temperature dependence of ice formation, which alters the vertical distribution of cloud microphysical processes. The controlling effect of the INP temperature dependence is substantial even in the presence of Hallett–Mossop secondary ice production, and the effects of secondary ice formation depend strongly on the chosen INP parameterisation. Our results have implications for climate model simulations of tropical clouds and radiation, which currently do not consider a link between INP particle type and ice water content. The results also provide a challenge to the INP measurement community, as we demonstrate that INP concentration measurements are required over the full mixed-phase temperature regime, which covers around 10 orders of magnitude.