Experimental Assessment of Collection Efficiency of Submicron Aerosol Particles by Cloud Droplets

The interplay between aerosol particles and water droplets in the atmosphere, especially in clouds, influences both aerosol and cloud properties. The major uncertainty in our understanding of climate arises in the indirect effect of aerosol and their ability to impact cloud formation and consequently alter the global radiative balance. The collision between a water droplet and aerosol particles that results in coalescence is termed “collection” or “coagulation”. Coagulation can lead to aerosol removal from the atmosphere or induce ice nucleation via contact freezing. There is a theoretical collection efficiency minimum of particles with diameter between 0.1-2 µm, called the “Greenfield Gap”. Experimental effort, however, was limited to drizzle and rain drops until recently, and has not constrained parameters that describe particle collection efficiency by cloud droplets. Collection efficiency is also an important parameter for assessing contact freezing, the least known ice nucleation mechanism today. Experimentally assessing collection efficiency can prove the existence of the “Greenfield Gap” and lay the foundation for studying contact freezing.

We recently constructed the MIT-Contact Freezing Chamber (MIT-CFC) to study coagulation experimentally. A stream of 40 µm cloud droplets fall freely into the chamber and collide with aerosol particles with known size and concentration. The outflow goes through a series of dryers before entering the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument for chemical composition analysis. PALMS is a true single-particle instrument and gives information on the size and the chemical composition of each particle. Coagulated particles from the MIT-CFC have mass spectral signatures of both the aerosol particles and the droplet residuals, while the droplet residual contains no signature of the aerosol particles. To our knowledge, this is the first time coagulation has been seen on a single-particle basis. We will present the collection efficiency data by the 40 µm droplets of polystyrene latex spheres (PSLs) with well-defined sizes (50-950 nm) and concentrations (10-100 #/cc) under atmospherically relevant temperatures and relative humidity conditions. The data are in line with the Greenfield Gap.