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In the last two IPCC assessments aerosol radiative forcing have been given the largest uncertainty range of all forcing agents assessed. This forcing range is really a diversity of simulated forcing in different models. An essential step towards reducing model uncertainty is to quantify and attribute the sources of uncertainty at the process level. Here, we use statistical emulation techniques to quantify uncertainty in simulated concentrations of July-mean cloud condensation nuclei (CCN) from a complex global aerosol microphysics model. CCN was chosen because it is the aerosol property that controls cloud drop concentrations, and therefore the aerosol indirect radiative forcing effect.We use Gaussian process emulation to perform a full variancebased sensitivity analysis and quantify, for each model grid box, the uncertainty in simulated CCN that results from 8 uncertain model parameters. We produce global maps of absolute and relative CCN sensitivities to the 8 model parameter ranges and derive probability density functions for simulated CCN. The approach also allows us to include the uncertainty from interactions between these parameters, which cannot be quantified in traditional one-at-a-time sensitivity tests. The key findings from our analysis are that model CCN in polluted regions and the Southern Ocean are mostly only sensitive to uncertainties in emissions parameters but in all other regions CCN uncertainty is driven almost exclusively by uncertainties in parameters associated with model processes. For example, in marine regions between 30° S and 30° N model CCN uncertainty is driven mainly by parameters associated with cloud processing of Aitken-sized particles whereas in Polar Regions uncertainties in scavenging parameters dominate. In these two regions a single parameter dominates but in other regions up to 50% of the variance can be due to interaction effects between different parameters. Our analysis provides direct quantification of the reduction in variance that would result if a parameter could be specified precisely. When extended to all process parameters the approach presented here will therefore provide a clear global picture of how improved knowledge of aerosol processes would translate into reduced model uncertainty. [ABSTRACT FROM AUTHOR]

Empirical relationships that link cloud droplet number (CDN) to aerosol number or mass are commonly used to calculate global fields of CDN for climate forcing assessments. In this work we use a sectional global model of sulfate and sea-salt aerosol coupled to a mechanistic aerosol activation scheme to explore the limitations of this approach. We find that a given aerosol number concentration produces a wide range of CDN concentrations due to variations in the shape of the aerosol size distribution. On a global scale, the dependence of CDN on the size distribution results in regional biases in predicted CDN (for a given aerosol number). Empirical relationships between aerosol number and CDN are often derived from regional data but applied to the entire globe. In an analogous process, we derive regional "correlation-relations" between aerosol number and CDN and apply these regional relations to calculations of CDN on the global scale. The global mean percentage error in CDN caused by using regionally derived CDN-aerosol relations is 20 to 26%, which is about half the global mean percentage change in CDN caused by doubling the updraft velocity. However, the error is as much as 25-75% in the Southern Ocean, the Arctic and regions of persistent stratocumulus when an aerosol-CDN correlation relation from the North Atlantic is used. These regions produce much higher CDN concentrations (for a given aerosol number) than predicted by the globally uniform empirical relations. CDN aerosol number relations from different regions also show very different sensitivity to changing aerosol. The magnitude of the rate of change of CDN with particle number, a measure of the aerosol efficacy, varies by a factor 4. CDN in cloud processed regions of persistent stratocumulus is particularly sensitive to changing aerosol number. It is therefore likely that the indirect effect will be underestimated in these important regions. [ABSTRACT FROM AUTHOR]