Closure analysis of aerosol-cloud composition in tropical maritime warm convection
Authors: Crosbie Ewan , Ziemba Luke D. , Shook Michael A. , Robinson Claire E. , Winstead Edward L. , Thornhill K. Lee , Braun Rachel A. , MacDonald Alexander B. , Stahl Connor , Sorooshian Armin , van den Heever Susan C. , DiGangi Joshua P. , Diskin Glenn S. , Woods Sarah , Bañaga Paola , Brown Matthew D. , Gallo Francesca , Hilario Miguel Ricardo A. , Jordan Carolyn E. , Leung Gabrielle R. , Moore Richard H. , Sanchez Kevin J. , Shingler Taylor J. , Wiggins Elizabeth B. 
Published: May 2022

Abstract. Cloud droplet composition is a key observable quantity that can aid understanding of how aerosols and clouds interact. As part of the Clouds, Aerosols and Monsoon Processes – Philippines Experiment (CAMP2Ex), three case studies were analyzed involving collocated airborne sampling of relevant clear and cloudy airmasses associated with maritime warm convection. Two of the cases represented a polluted marine background, with signatures of transported East Asian regional pollution, aged over water for several days, while the third case comprised a major smoke transport event from Kalimantan fires. Sea salt was a dominant component of cloud droplet composition, in spite of fine particulate enhancement from regional anthropogenic sources. Furthermore, the proportion of sea salt was enhanced relative to sulfate in rainwater and may indicate both a propensity for sea salt to aid warm rain production and an increased collection efficiency of large sea salt particles by rain in subsaturated environments. Amongst cases, as precipitation became more significant, so too did the variability in the sea salt to (non-sea salt) sulfate ratio. Across cases, nitrate and ammonium were fractionally greater in cloud water than fine-mode aerosol particles; however, a strong co-variability in cloud water nitrate and sea salt was suggestive of prior uptake of nitrate on large salt particles. A mass-based closure analysis of non-sea salt sulfate compared the cloud water air-equivalent mass concentration to the concentration of aerosol particles serving as cloud condensation nuclei for droplet activation. While sulfate found in cloud was generally constrained by the sub-cloud aerosol concentration, there was significant intra-cloud variability that was attributed to entrainment – causing evaporation of sulfate containing droplets – and losses due to precipitation. In addition, precipitation tended to promote mesoscale variability in the sub-cloud aerosol through a combination of removal, convective downdrafts, and through dynamically-driven convergence. Physical mechanisms exerted such strong control over the cloud water compositional budget that it was not possible to isolate any signature of chemical production/loss using in-cloud observations. The cloud-free environment surrounding the non-precipitating, smoke case indicated sulfate enhancement compared to convective mixing quantified by a stable gas tracer; however, this was not observed in the cloud water (either through use of ratios or the mass closure) perhaps implying that the warm convective cloud time scale was too short for chemical production to be a leading-order budgetary term. Closure of other species was truncated by incomplete characterization of coarse aerosol (e.g., it was found that only 10-50% of sea salt mass found in cloud was captured during clear air sampling) and unmeasured gas phase abundances affecting closure of semi-volatile aerosol species (e.g., ammonium, nitrate and organic aerosols) and soluble volatile organic compound contributions to total organic carbon in cloud water.