Rapid growth of Aitken-mode particles during Arctic summer by fog chemical processing and its implication.

ABSTRACT

In the Arctic, new particle formation (NPF) and subsequent growth processes are the keys to produce Aitken-mode particles, which under certain conditions can act as cloud condensation nuclei (CCNs). The activation of Aitken-mode particles increases the CCN budget of Arctic low-level clouds and, accordingly, affects Arctic climate forcing. However, the growth mechanism of Aitken-mode particles from NPF into CCN range in the summertime Arctic boundary layer remains a subject of current research. In this combined Arctic cruise field and modeling study, we investigated Aitken-mode particle growth to sizes above 80 nm. A mechanism is suggested that explains how Aitken-mode particles can become CCN without requiring high water vapor supersaturation. Model simulations suggest the formation of semivolatile compounds, such as methanesulfonic acid (MSA) in fog droplets. When the fog droplets evaporate, these compounds repartition from CCNs into the gas phase and into the condensed phase of nonactivated Aitken-mode particles. For MSA, a mass increase factor of 18 is modeled. The postfog redistribution mechanism of semivolatile acidic and basic compounds could explain the observed growth of >20 nm h-1 for 60-nm particles to sizes above 100 nm. Overall, this study implies that the increasing frequency of NPF and fog-related particle processing can affect Arctic cloud properties in the summertime boundary layer.