Clouds play a key role in Earth’s radiation budget, and aerosols serve as the seeds upon which cloud droplets form. Anthropogenic activity has led to an increase in aerosol particle concentrations globally and an increase in those particles that act as cloud condensation nuclei (CCN) and ice nucleating particles (INP). The effect of an increase in aerosols on cloud optical properties, and associated radiative forcing, is the most uncertain component of historical radiative forcing of Earth’s climate caused by greenhouse gases (GHGs) and aerosols. The Intergovernmental Panel on Climate Change (IPCC) AR5 assessment of climate forcing factors (Fig. S1) ascribes “high” confidence to the estimate of direct aerosol radiative forcing (mean