Abstract

Atmospheric aerosols and their interaction with clouds are the largest uncertainty in the human forcing of the climate system. Anthropogenic emissions have increased aerosol concentrations, increasing the concentration of cloud droplets and leading to reductions in droplet size and increases in cloud reflectivity (a negative radiative forcing). Central to this climate impact is the susceptibility of cloud droplet number to aerosol. This susceptibility varies widely with the method and data used to estimate it and within global climate models, explaining much of the variation in estimates of the radiative forcing from aerosol-cloud interactions (RFaci). Better constraints on the susceptibility have been a key target for recent observation-based constraints on the aerosol forcing.                                                                                                                                                 Previous work has shown that the aerosol burden of the clean, pre-industrial atmosphere has been demonstrated as a key uncertainty for the aerosol forcing. Here we show that the behaviour of clouds under these clean conditions is of equal importance for understanding the spread in radiative forcing estimates between models and observations. This means that the uncertainty in the aerosol impact on clouds is, counterintuitively, driven by situations with little aerosol. Removing these clean conditions from observational estimates of the susceptibility produces a close agreement between different model and observational estimates of the cloud response to aerosol, but does not provide a strong constraint on the RFaci. If we are to produce tighter constraints on the radiative forcing from aerosol-cloud interactions, better constraints on the behaviour of cloud in keen conditions are vital.

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