Knowledge of cloud and precipitation formation processes remains incomplete, yet global precipitation is predominantly produced by clouds containing the ice phase. Ice first forms in clouds warmer than −36°C on particles termed ice nuclei. We combine observations from field studies over a 14-year period, from a variety of locations around the globe, to show that the concentrations of ice nuclei active in mixed-phase cloud conditions can be related to temperature and the number concentrations of particles larger than 0.5 μm in diameter. This new relationship reduces unexplained variability in ice nuclei concentrations at a given temperature from ∼10 3 to less than a factor of 10, with the remaining variability apparently due to variations in aerosol chemical composition or other factors. When implemented in a global climate model, the new parameterization strongly alters cloud liquid and ice water distributions compared to the simple, temperature-only parameterizations currently widely used. The revised treatment indicates a global net cloud radiative forcing increase of ∼1 W m −2 for each order of magnitude increase in ice nuclei concentrations, demonstrating the strong sensitivity of climate simulations to assumptions regarding the initiation of cloud glaciation.aerosol indirect effects | climate forcing | ice nucleation T he formation of ice in clouds is of vital importance to life on Earth, as ice formation is one of the key processes initiating precipitation. In addition, since ice nucleation is tied to the action of specific aerosol particles, natural and human impacts on ice nucleation in the atmosphere can lead to alteration of the energy and hydrological cycles (1). Ice nucleation in clouds occurs via two primary pathways: homogeneous freezing of liquid particles below about −36°C and heterogeneous ice nucleation, triggered by "ice nuclei" that possess surface properties favorable to lowering the energy barrier to crystallization. Once ice is formed, some circumstances may favor generation of ice from preexisting ice particles, or secondary ice formation (2). Heterogeneous ice nucleation remains an enigmatic topic involving multiple mechanistic processes (3) that sometimes defy ready investigation or description. Despite the lack of a complete understanding of heterogeneous ice formation processes, a variety of techniques have been developed and used to detect the presence of and quantify the number concentrations of atmospheric ice nuclei as a function of temperature (4). These measurements show that, although generally representing only 1 in 10 5 of ambient particles in the free troposphere (5), ice nuclei (IN) can nevertheless exert an influence on cold cloud microphysical processes that is disproportionate to their low number concentrations. For example, the concentrations of IN needed to explain observed precipitation rates range from as small as 10 −3 per standard liter at −10°C (6) to more typical estimates of a few IN per standard liter at −20°C (7).The sensitivity of precipitation initiation fro...

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Aerosols influence cloud and precipitation development in complex ways due to myriad feedbacks at a variety of scales from individual clouds through entire storm systems. This paper describes the implementation, testing, and results of a newly modified bulk microphysical parameterization with explicit cloud droplet nucleation and ice activation by aerosols. Idealized tests and a high-resolution, convection-permitting, continental-scale, 72-h simulation with five sensitivity experiments showed that increased aerosol number concentration results in more numerous cloud droplets of overall smaller size and delays precipitation development. Furthermore, the smaller droplet sizes cause the expected increased cloud albedo effect and more subtle longwave radiation effects. Although increased aerosols generally hindered the warm-rain processes, regions of mixed-phase clouds were impacted in slightly unexpected ways with more precipitation falling north of a synoptic-scale warm front. Aerosol impacts to regions of light precipitation, less than approximately 2.5 mm h−1, were far greater than impacts to regions with higher precipitation rates. Comparisons of model forecasts with five different aerosol states versus surface precipitation measurements revealed that even a large-scale storm system with nearly a thousand observing locations did not indicate which experiment produced a more correct final forecast, indicating a need for far longer-duration simulations due to the magnitude of both model forecast error and observational uncertainty. Last, since aerosols affect cloud and precipitation phase and amount, there are resulting implications to a variety of end-user applications such as surface sensible weather and aircraft icing.

Many soil‐derived particles dominated by insoluble material, including Saharan dusts, are known to act as ice nuclei. If, however, dust particles can compete with other atmospheric particle types to form liquid cloud droplets, they have a greater potential to change climate through indirect effects on cloud radiative properties and to affect the hydrological cycle through precipitation changes. By directly collecting and analyzing the residual nuclei of small cloud droplets, we demonstrate that Saharan dust particles do commonly act as cloud condensation nuclei (CCN) in the eastern North Atlantic. Droplet activation calculations support the measurements by showing that due to its slightly hygroscopic nature, even submicron dust can be important as CCN. Given the dual nature of Saharan dust particles as CCN and ice nuclei, this infusion of dust is expected to impact not only droplet size and albedo in small clouds, but ice formation in deep convective clouds.