Airborne and ground-based observations of ammonium-nitrate-dominated aerosols in a shallow boundary layer during intense winter pollution episodes in northern Utah

摘要

Airborne and ground-based measurements of aerosol concentrations, chemical composition, and gas-phase precursors were obtained in three valleys in northern Utah (USA). The measurements were part of the Utah Winter Fine Particulate Study (UWFPS) that took place in January–February 2017. Total aerosol mass concentrations of PM1 were measured from a Twin Otter aircraft, with an aerosol mass spectrometer (AMS). PM1 concentrations ranged from less than 2μgm?3 during clean periods to over 100μgm?3 during the most polluted episodes, consistent with PM2.5 total mass concentrations measured concurrently at ground sites. Across the entire region, increases in total aerosol mass above ～2μgm?3 were associated with increases in the ammonium nitrate mass fraction, clearly indicating that the highest aerosol mass loadings in the region were predominantly attributable to an increase in ammonium nitrate. The chemical composition was regionally homogenous for total aerosol mass concentrations above 17.5μgm?3, with 74±5% (average±standard deviation) ammonium nitrate, 18±3% organic material, 6±3% ammonium sulfate, and 2±2% ammonium chloride. Vertical profiles of aerosol mass and volume in the region showed variable concentrations with height in the polluted boundary layer. Higher average mass concentrations were observed within the first few hundred meters above ground level in all three valleys during pollution episodes. Gas-phase measurements of nitric acid (HNO3) and ammonia (NH3) during the pollution episodes revealed that in the Cache and Utah valleys, partitioning of inorganic semi-volatiles to the aerosol phase was usually limited by the amount of gas-phase nitric acid, with NH3 being in excess. The inorganic species were compared with the ISORROPIA thermodynamic model. Total inorganic aerosol mass concentrations were calculated for various decreases in total nitrate and total ammonium. For pollution episodes, our simulations of a 50% decrease in total nitrate lead to a 46±3% decrease in total PM1 mass. A simulated 50% decrease in total ammonium leads to a 36±17%μgm?3 decrease in total PM1 mass, over the entire area of the study. Despite some differences among locations, our results showed a higher sensitivity to decreasing nitric acid concentrations and the importance of ammonia at the lowest total nitrate conditions. In the Salt Lake Valley, both HNO3 and NH3 concentrations controlled aerosol formation.