Simulating Droplet-Resolved Haze and Cloud Chemistry Forming Secondary Organic Aerosols in Turbulent Conditions...

Most models do not explicitly simulate droplet-resolved cloud chemistry and the interactions between turbulence and cloud chemistry due to large associated computational costs. Here, we incorporate the formation of isoprene epoxydiol secondary organic aerosol (IEPOX-SOA) in individual droplets within a one-dimensional explicit mixing parcel model (EMPM-Chem). We apply EMPM-Chem to simulate turbulence and droplet-resolved IEPOX-SOA formation using a laboratory cloud chamber configuration. We find that the dissolution of IEPOX gases is weighted more toward larger cloud droplets due to their large liquid water content (compared to smaller droplets), while the conversion of dissolved IEPOX to IEPOX-SOA is much greater within smaller deliquesced haze particles due to their higher acidity and ionic strengths compared to cloud droplets. We also apply the EMPM-Chem model to simulate how IEPOX-SOA formation evolves in individual cloud droplets within rising cloudy parcels in the atmosphere. We find that as subsaturated air is entrained into and turbulently mixed with the cloud parcel, evaporation causes a reduction in droplet sizes, which leads to corresponding increases in per droplet ionic strength and acidity. Increased droplet acidity, in turn, greatly accelerates the kinetics of IEPOX-SOA formation. Our results provide key insights into single cloud-droplet chemistry, suggesting that entrainment mixing may be an important process that increases SOA formation in the real atmosphere.