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Abstract. Mercury (Hg) is a global atmospheric pollutant. In its oxidized form (HgII), it can readily deposit to ecosystems, where it may bioaccumulate and cause severe health effects. High HgII concentrations are reported in the free troposphere, but spatiotemporal data coverage is limited. Underestimation of HgII by commercially available measurement systems hinders quantification of Hg cycling and fate. During spring–summer 2021 and 2022, we measured elemental (Hg0) and oxidized Hg using a calibrated dual-channel system alongside trace gases, aerosol properties, and meteorology at the high-elevation Storm Peak Laboratory (SPL) above Steamboat Springs, Colorado. Oxidized Hg concentrations displayed diel and episodic behavior similar to previous work at SPL but were approximately 3 times higher in magnitude due to improved measurement accuracy. We identified 18 multi-day events of elevated HgII (mean enhancement of 36 pg m−3) that occurred in dry air (mean ± SD of relative humidity = 32 ± 16 %). Lagrangian particle dispersion model (HYSPLIT–STILT, Hybrid Single-Particle Lagrangian Integrated Trajectory–Stochastic Time-Inverted Lagrangian Transport) 10 d back trajectories showed that the majority of transport prior to events occurred in the low to middle free troposphere. Oxidized Hg was anticorrelated with Hg0 during events, with an average (± SD) slope of −0.39 ± 0.14. We posit that event HgII resulted from upwind oxidation followed by deposition or cloud uptake during transport. Meanwhile, sulfur dioxide measurements verified that three upwind coal-fired power plants did not influence ambient Hg at SPL. Principal component analysis showed HgII consistently inversely related to Hg0 and generally not associated with combustion tracers, confirming oxidation in the clean, dry free troposphere as its primary origin. 

Abstract. New particle formation (NPF) events are defined as asudden burst of aerosols followed by growth and can impact climate bygrowing to larger sizes and under proper conditions, potentially formingcloud condensation nuclei (CCN). Field measurements relating NPF and CCN arecrucial in expanding regional understanding of how aerosols impactclimate. To quantify the possible impact of NPF on CCN formation, it isimportant to not only maintain consistency when classifying NPF events butalso consider the proper timeframe for particle growth to CCN-relevantsizes. Here, we analyze 15 years of direct measurements of both aerosol sizedistributions and CCN concentrations and combine them with novel methods toquantify the impact of NPF on CCN formation at Storm Peak Laboratory (SPL),a remote, mountaintop observatory in Colorado. Using the new automaticmethod to classify NPF, we find that NPF occurs on 50 % of all daysconsidered in the study from 2006 to 2021, demonstrating consistency withprevious work at SPL. NPF significantly enhances CCN during the winter by afactor of 1.36 and during the spring by a factor of 1.54, which, when combined withprevious work at SPL, suggests the enhancement of CCN by NPF occurs on aregional scale. We confirm that events with persistent growth are common inthe spring and winter, while burst events are more common in the summer andfall. A visual validation of the automatic method was performed in thestudy. For the first time, results clearly demonstrate the significantimpact of NPF on CCN in montane North American regions and the potential forwidespread impact of NPF on CCN.