Impact of Cloud Process in the Mixing State and Microphysical Properties of Soot Particles: Implications in Light Absorption Enhancement.

The radiative forcing of soot is dependent on the morphology, mixing state and structure. Cloud processing has been predicted to affect their mixing properties but little is known about the resulting light absorption properties. We collected ambient particles in the pre‐cloud period, the cloud residues and interstitials in the in‐cloud period at Mt. Tianjing (southern China). The morphology parameters of soot aggregates with varying mixing materials [sulfate (S) and organics (OM)] and mixing structures were investigated by a transmission electron microscope, and their absorption cross section were calculated based on discrete dipole approximation. We found that the number contribution of soot‐S decreased from 45% in the pre‐cloud period to 32% in the in‐cloud period, and that of soot‐OM increased from 44% to 60%. Moreover, the number proportion of soot‐OM with fully embedded structure increased remarkably in the in‐cloud period (29%), compared with that in the pre‐cloud period (3%). In addition, the soot‐S aggregates became denser after in‐cloud aqueous process. However, for soot‐OM aggregates, the morphology remained relatively constant. The distinctly different change of soot‐S and soot‐OM in morphology highlights the chemically resolved reconstruction of soot morphology. Theoretical calculation further shows that the changes of soot particles in the mixing state and morphological characteristics by the cloud process resulted in the light absorption enhancement increase from 1.57 to 2.01. This study highlights that the evolution of microphysical properties upon cloud processing should also be considered in climate models to more accurately evaluate the impacts of soot particles. Plain Language Summary: While soot particles are the main component of aerosols that produce positive radiative forcing in clouds, the impact of in‐cloud processes on key factors (mixing state and microphysical property) for evaluating the optical properties of soot particles is unclear. Here, we report the detailed information on several parameters required to calculate the optical properties of soot particles, throughout the cloud events. And we found that changes in the mixing state, mixing structure, and morphology of soot particles under the influence of in‐cloud processes lead to a significant light absorption enhancement. The results also highlight the role of in‐cloud aqueous formation of secondary compositions in reshaping the soot particles, which has substantial implications for the climate impact of soot particles. Given that ∼70% of the Earth's surface is covered by clouds, taking the mixing state and microphysical properties of soot particles into account in climate models may help constrain the contribution of soot particles to global radiative forcing. Key Points: Cloud processing contributes to the increase of organic coating on soot aggregates, especially for those with fully embedded structureThe sulfate coating causes more compaction of soot aggregates than the organic coating upon cloud processingChanges in the microphysical properties of soot particles driven by one cloud event increase their absorption enhancement by 1.29 times [ABSTRACT FROM AUTHOR]