Characterizing the impact of water uptake on light absorption by aerosol particles
Absorbing aerosols (AA) have an important impact on the global radiation budget. The composition and properties of AA can vary substantially throughout the atmosphere, depending on the particle source and the influence of chemical aging. Uncertainties associated with the radiative effects of AA remain substantial. A key contributor to this uncertainty is understanding the extent to which water uptake alters absorption by AA particles and how this depends on particle composition. We have used new and existing experimental tools to systematically characterize the relationship(s) between AA chemical and physical characteristics, relative humidity, and mixing of AA with other aerosol components through a combination of laboratory and field measurements. We have developed fundamental understanding through laboratory experiments that will enable interpretation of field observations at DOE ARM sites and facilitate process-based improvements in the simulation of absorption by carbonaceous aerosols in climate models. In the laboratory experiments we have considered a variety of different AA types, including fullerene soot (a surrogate for refractory black carbon, or BC) and nigrosine (a surrogate for partially soluble brown carbon, or BrC). By examining a range of AA types we will develop insight into how the chemical and physical properties of AA particles (e.g. whether they are refractory or soluble) impact the influence of water uptake on absorption. These AA particles will also be mixed—both internally and externally—with compounds having a wide range of hygroscopic properties to establish how the impact of water uptake on absorption will vary with photochemical processing. These laboratory observations have been compared with commonly used theoretical models, enabling development of empirical models that will facilitate improved representation of absorption by AA particles in regional and global climate models. Overall, our study has contributed to the mission of the Atmospheric System Research program by quantifying how interactions between aerosols and radiation depend on relative humidity. Through this, our work will improve understanding and model representation of aerosol processes as they affect the Earth’s radiation budget.