Characterizing ultrafine particle growth at a pine forest site influenced by anthropogenic pollution during BEACHON-RoMBAS-2011

Representing the formation and growth of ultrafine particles in chemistry and climate models is challenging due to the complexity of processes involved, which leads to uncertainties in aerosol size distributions and their effects on Cloud Condensation Nuclei (CCN). The Rocky Mountain Biogenic Aerosol Study (RoMBAS) was an intensive measurement campaign as part of the broader BEACHON (Bio-hydro-atmosphere interactions of Energy Aerosols, Carbon, H2O, Organics and Nitrogen) project. This took place during July - August 2011 at the Manitou Experimental Forest Observatory. The location is situated in the rural-urban interface along the Colorado Front Range and allows us to study the effects of aerosol formation and other atmospheric chemistry phenomenon in a forested region with periodic urban influences. Surface measurements of gases, aerosols and meteorological parameters from this campaign were used to examine the formation and growth processes leading to observed Aiken-mode Particle burst Events (APEs), and to quantify their effects on aerosol properties and cloud condensation nuclei CCN concentrations. Results suggest that APEs were observed at the forest site in the early afternoon associated with the arrival of anthropogenic plumes from Denver and Colorado Springs. Mean number concentrations of ultrafine particles (4-30nm) typically exceeded 5000 cm-3 during APEs and these elevated concentrations were correlated with elevated SO2. The Weather Research and Forecasting model with on-line Chemistry (WRF-Chem) was used to model APEs during BEACHON-RoMBAS. The model was updated to include an activation nucleation (AN) scheme with an empirical representation of aerosol nucleation rate, and subsequent growth due to the condensation of organic and inorganic vapors. Comparisons with ground measurements show that the updated model reasonably captures aerosol number concentrations and size distribution during APEs, as well as CN and CCN concentrations. Model results suggest that anthropogenic SO2 trigger APEs, and that the condensation of monoterpene oxidation products onto freshly nucleated particles drives their growth. The simulated growth rate is 1.2 nm/hr which is comparable with 2 nm/hr in the measurement. Comparing with a sensitivity test excluding nucleation process in the model, model calculations with AN show the presence of APEs in the forest area tends to modify the composition of small aerosols (<100nm), leading to 2.3 times higher values of sulfate aerosols.Therefore, the predicted volume-averaged hygroscopicity parameter and CCN concentration are significantly influenced.