Arctic fog chemistry induces the unexpected growth of Aitken mode particles to CCN-active particles

New particle formation (NPF) and early growth are efficient processes producing high concentrations of cloud condensation nuclei (CCNs) precursors in the Arctic marine boundary layer (AMBL). However, due to short lifetime and lack of condensable vapors, newly formed particles do often not grow beyond 50 nm and cause low CCN particle concentrations in the AMBL. Thus, even the smallest amount of Aitken mode particle growth is capable to significantly increase the CCN budget. However, the growth mechanism of Aitken-mode particles from NPF into CCN range in the Arctic is still rather unclear and was therefore investigated during the cruise campaign PASCAL in 2017.

During PASCAL, aerosol particles measurements were performed and an unexpected rapid growth of Aitken mode particles was observed right after fog episodes. Combined field data analyses and detailed multiphase chemistry box model simulations with the CAPRAM mechanism were performed to study the underlying processes. Resulting, a new mechanism is proposed explaining how particles with d < 50 nm are able to grow into CCN size range in the Arctic without requiring high water vapor supersaturation (SS). The investigations demonstrated that the rapid post-fog particle growth of Aitken mode is related to chemical processes within the Arctic fog. The redistribution of semi-volatile acidic (e.g., methanesulfonic acid) and basic (e.g., ammonia) compounds from processed CCN-active particles to smaller CCN-inactive particles can cause a rapid particle growth of Aitken mode particles after fog evaporation enabling them to grow towards CCN size. Comparisons of the model results with Berner impactor measurements supports the proposed growth mechanism.

Overall, this study provided new insights on how the increasing frequency of NPF and fog-related particle processing can increase in the number of CCNs and cloud droplets leading to an increased albedo of Arctic clouds and thus affect the radiative balance in the Arctic. Since fogs will occur more frequently in the Arctic as a result of climate change, this growth mechanism and a deeper knowledge on its feedbacks can be essential to understand Arctic warming.