Atmospheric aerosols are an important component of the Earth system, with substantial impacts on biogeochemistry, human health, clouds, and radiation. Because these aerosols interact with clouds and radiation, uncertainties in aerosol forcing remain a significant contributor to the uncertainties associated with climate change projections. Among all aerosols, the light-absorbing aerosols are critical to understanding the aerosol forcing on climate, because they can warm the atmosphere and offset the cooling effects by non-absorbing aerosols. Despite the importance of absorbing aerosols, climate models fail to accurately represent their properties, distributions, and their associated large-scale environments. In this seminar, I will focus on dust and smoke aerosols because they account for the majority of the absorbing aerosols in the atmosphere. I will explore how the large-scale aerosol environment complicates the attribution of aerosol-cloud interactions over the southeast Atlantic, where the most extensive above-cloud smoke occurs. I will also explore the representation of small-scale dust properties in climate models and how newly-developed observational constraints on dust size distribution expose the discrepancies in these models and the associated bias in the simulated dust impacts on the global climate.