On the correlation between hygroscopic properties and chemical composition of cloud condensation nuclei obtained from the chemical aging of soot particles with O₃ and SO₂

Soot particles released in the atmosphere have long been investigated for their ability to affect the radiative forcing. Although freshly emitted soot particles are generally considered to yield only positive contributions to the radiative forcing, atmospheric aging can activate them into efficient cloud condensation or ice nuclei, which can trigger the formation of persistent clouds and ultimately provide a negative contribution to the radiative forcing. Depending on their residence time in the atmosphere, soot particles can undergo several physical and chemical aging processes that affect their chemical composition, particle size distribution and morphology, and ultimately their optical and hygroscopic properties. The impact of the physical-chemical aging on the properties of soot particles is still difficult to quantify, as well as their effect on the radiative forcing of the atmosphere.This work investigates the hygroscopic properties of chemically aged soot particles obtained from the combustion of aviation fuel, and in particular the interplay between aging mechanisms initiated by two widespread atmospheric oxidizers (O-3 and SO2). Activation is measured in water supersaturation conditions using a cloud condensation nuclei counter. Once particle morphology and size distribution are taken into account, the hygroscopicity parameter kappa is derived using kappa-K & ouml;hler theory and correlated to the change of the chemical composition of the particles aged in a simulation chamber. While fresh soot particles are poor cloud condensation nuclei (kappa < 10(-4)) and are not significantly affected by either O-3 or SO2 at the timescale of the experiments, rapid activation is observed when they are simultaneously exposed to both oxidizers. Activated particles become efficient cloud condensation nuclei, comparable to the highly hygroscopic particulate matter typically found in the atmosphere (kappa = 0.2-0.6 at RH = 20 %). Statistical analysis reveals a correlation between the activation and sulfur-containing ions detected on the chemically aged particles that are absent from the fresh particles.