The uptake of methanesulfonic acid (MSA) on existing particles is a major route of the particulate MSA formation, however, MSA uptake on different particles is still lacking in knowledge. Characteristics of MSA uptake on different aerosol particles were investigated in polynya (an area of open sea water surrounded by ice) regions of the Ross Sea, Antarctica. Particulate MSA mass concentrations, as well as aerosol population and size distribution, were observed simultaneously for the first time to access the uptake of MSA on different particles. The results show that MSA mass concentration does not always reflect MSA particle population in the marine atmosphere. MSA uptake on aerosol particle increases the particle size and changes aerosol chemical composition, but it does not increase the particle population. The uptake rate of MSA on particles is significantly influenced by aerosol chemical properties. Sea salt particles are beneficial for MSA uptake, as MSA-Na and MSA-Mg particles are abundant in the Na and Mg particles, accounting for 0.43±0.21 and 0.41±0.20 of the total Na and Mg particles, respectively. However, acidic and hydrophobic particles suppress the uptake of MSA, as MSA-EC (elemental carbon) and MSA-${\mathrm{SO}}_{\mathrm{4}}^{\mathrm{2}-}$ particles account for only 0.24±0.68 and 0.26±0.47 of the total EC and ${\mathrm{SO}}_{\mathrm{4}}^{\mathrm{2}-}$ particles, respectively. The results extend the knowledge of the formation and environmental behavior of MSA in the marine atmosphere.

Atmospheric particles can impact cloud formation and play a critical role in regulating cloud properties. However, particle characteristics at the single-particle level and their ability to act as ice-nucleating particles (INPs) over the marine atmosphere are poorly understood. In this study, we present micro-spectroscopic characterizations and ice nucleation properties of particles collected during a cruise from South Korea to Antarctica in 2019. Most of the samples were dominated by fresh sea salt, aged sea salt, and sea salt mixed with sulfate particles, with total number percentages ranging from 48 % to 99 % over the western Pacific and the Southern Ocean. The mixing-state index of the particle population ranged from 50 % to 95 % over the Northern Hemisphere and Southern Hemisphere. Multiphase processes on sea salt particles resulted in chlorine deficiency. This selective aging process made the marine particle population more externally mixed. Ice nucleation onset conditions primarily for the deposition mode were measured and the investigated particles showed diverse ice nucleation abilities. The fresh sea salt particles with organic coatings exhibited the highest ice nucleation ability at a relative humidity with respect to ice as low as 121 %. The sea salt mixed sulfate particle was enriched in INPs by a factor of 1.9. Aging processes affected both the mixing state of the particles and their ice nucleation abilities. Our analysis shows that assuming an internally mixed particle population in the marine atmosphere can lead to errors of several orders of magnitude in predicting ice nucleation rates.