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Understanding the sources and evolution of aerosols is crucial forconstraining the impacts that aerosols have on a global scale. An unansweredquestion in atmospheric science is the source and evolution of the Antarcticaerosol population. Previous work over the continent has primarily utilizedlow temporal resolution aerosol filters to answer questions about thechemical composition of Antarctic aerosols. Bulk aerosol sampling has beenuseful in identifying seasonal cycles in the aerosol populations, especiallyin populations that have been attributed to Southern Ocean phytoplanktonemissions. However, real-time, high-resolution chemical composition data arenecessary to identify the mechanisms and exact timing of changes in theAntarctic aerosol. The recent 2ODIAC (2-Season Ozone Depletion andInteraction with Aerosols Campaign) field campaign saw the first everdeployment of a real-time, high-resolution aerosol mass spectrometer (SP-AMS– soot particle aerosol mass spectrometer – or AMS) to the continent. Data obtained from the AMS, and a suite of otheraerosol, gas-phase, and meteorological instruments, are presented here. Inparticular, this paper focuses on the aerosol population over coastalAntarctica and the evolution of that population in austral spring. Resultsindicate that there exists a sulfate mode in Antarctica that is externallymixed with a mass mode vacuum aerodynamic diameter of 250 nm. Springtimeincreases in sulfate aerosol are observed and attributed to biogenic sources,in agreement with previous research identifying phytoplankton activity as thesource of the aerosol. Furthermore, the total Antarctic aerosol population isshown to undergo three distinct phases during the winter to summertransition. The first phase is dominated by highly aged sulfate particlescomprising the majority of the aerosol mass at low wind speed. The secondphase, previously unidentified, is the generation of a sub-250 nm aerosolpopulation of unknown composition. The second phase appears as a transitionalphase during the extended polar sunrise. The third phase is marked by anincreased importance of biogenically derived sulfate to the total aerosolpopulation (photolysis of dimethyl sulfate and methanesulfonic acid (DMS andMSA)). The increased importance of MSA is identified both through the direct,real-time measurement of aerosol MSA and through the use of positive matrixfactorization on the sulfur-containing ions in the high-resolution mass-spectral data. Given the importance of sub-250 nm particles, theaforementioned second phase suggests that early austral spring is the seasonwhere new particle formation mechanisms are likely to have the largestcontribution to the aerosol population in Antarctica

A missing source of aerosols in Antarctica – beyond long-range transport, phytoplankton, and photochemistry