Direct observation of wintertime secondary formation of sulfate in ambient aerosols in Fairbanks, Alaska

Sulfate comprises an average of 20% of the ambient PM2.5 mass during the winter months in Fairbanks, as indicated by 24-hour average filter measurements. During ALPACA 2022 field campaign (Jan 15th-Feb28th of 2022), we deployed two aerosol mass spectrometers (AMS) and one aerosol chemical speciation monitor (ACSM) at three urban sites, combined with Scanning Mobility Particle Sizer (SMPS), to examine the evolution of aerosol composition and size distribution at a sub-hourly time scale. During an intense pollution episode (ambient temperature is between -25 and -35 °C), all three instruments (two AMS and one ACSM) exhibit a sharp increase in sulfate mass within a matter of hours, while organic aerosols, black carbon and SO2 concentrations remain relatively stable. This notable increase in sulfate mass contributes to approximately half of the observed change in ambient PM2.5. The abrupt rise in sulfate mass is concurrent with a substantial increase in particle number density within the accumulation mode (100-1000 nm), suggesting the secondary formation of sulfate onto pre-existing aerosols. We further investigate possible mechanisms and have ruled out the possible role of cloud chemistry and transition metal ion. The rapid formation of sulfate seems to be linked to the ambient level of nitrogen oxides and, possibly, sunlight. Further investigation is underway to elucidate the intricate connections underlying this rapid sulfate formation.