The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol−cloud interactions at everincreasing levels of detail, but these models lack the resolution to represent clouds and aerosol−cloud interactions adequately. There is a dearth of observational constraints on aerosol−cloud interactions. We develop a conceptual approach to systematically constrain the aerosol−cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surfacebased shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol−cloud radiation system.T he climate system, with its couplings between land surface, vegetation, ocean, cryosphere, and atmosphere, is an extraordinarily complex system that is under intensive scrutiny for the purposes of climate analysis and prediction. The atmospheric aerosol and its interaction with clouds is a poorly quantified component of the climate system and is the focus of the current study. The aerosol comprises suspended particles that derive from the oceans, land surface, volcanoes, and anthropogenic activities. The difficulty in quantifying climate forcing by the aerosol emanates partly from the complexity in the aerosol itself, and partly from the fact that its influence on clouds requires detailed understanding of clouds and cloud feedbacks at a range of spatiotemporal scales. Untangling the multiple cloud responses that occur as a result of aerosol perturbations is particularly difficult (1). As one example, consider the influence of the aerosol on clouds and precipitation. Assuming no change in condensed water, the aerosol, by acting as nucleation sites for droplets, might generate smaller droplets, more reflective clouds (2), and reduced precipitation (3). However, through a multitude of complex and contingent pathways, aerosol-perturbed clouds sometimes appear to have similar reflectance because brightening is offset by reductions in cloud water, a fundamental property controlling cloud reflectance. On short timescales (hours), the aerosol tends to reduce precipitation in shallow, liquid-only clouds, but this may be offset over longer periods (multiple days) (4). Deep, mixed-phase convective clouds present even more complex pathways for generation of precipitation, and even more contingencies. The aerosol appears to change the distribution and intensity of surface rain from deep c...