In situ characterization of cloud condensation nuclei, interstitial, and background particles using the single particle mass spectrometer, SPLAT II.

The aerosol indirect effect remains the most uncertain aspect of climate change modeling, calling for characterization of individual particles sizes and compositions with high spatial and temporal resolution. We present the first deployment of our single particle mass spectrometer (SPLAT II) operated in dual data acquisition mode to simultaneously measure particle number concentrations, density, asphericity, and individual particle size and quantitative composition, with temporal resolution better than 60 s, thus yielding all the required properties to definitively characterize the aerosol-cloud interaction in this exemplary case. We find that particles are composed of oxygenated organics, many mixed with sulfates, biomass burning particles, some with sulfates, and processed sea-salt. Cloud residuals are found to contain more sulfates than background particles, explaining their higher efficiency to serve as cloud condensation nuclei (CCN). Additionally, CCN sulfate content increased with time due to in-cloud droplet processing. A comparison between the size distributions of background, CCN, and interstitial particles shows that while nearly all CCN particles are larger than 100 nm, over 80% of interstitial particles are smaller than 100 nm. We conclude that for this cloud, particle size is the controlling factor on aerosol activation into cloud-droplets, with higher sulfate content playing a secondary role.