Recent developments in our understanding of atmospheric organic particulate matter formation have been used to develop a state-of-the-art organic aerosol module for regional chemical transport models (CTMs). The module has been added to the regional CTM, PMCAMx, and has been evaluated against observations in the eastern U.S. The new module uses the volatility basis set framework to simulate primary organic aerosol (POA) partitioning between the gas and particulate phases and the gas-phase oxidation of the corresponding vapors. The formation and chemical aging of secondary organic aerosol (SOA) are modeled using the same volatility distribution approach. The module uses recent results from smog chamber studies for the formation of SOA from anthropogenic and biogenic hydrocarbons. Hourly organic aerosol predictions are evaluated using data from the Pittsburgh Air Quality Study (PAQS), and daily averaged predictions for July 2001 are compared to ambient measurements from the EPA Speciated Trends Network (STN) and the Interagency Monitoring of Protected Visual Environments (IMPROVE). The model reproduces both the absolute organic aerosol concentrations in urban and rural locations as well as the high degree of oxidation of these compounds. The chemical aging of anthropogenic SOA is consistent with the ambient organic aerosol concentration field and has a significant impact on the absolute ground-level concentrations of these compounds.

Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM/OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM/OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH > SRH led to increased SOA concentrations,· particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties· such as the OM/OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were highly water soluble and expected to contribute to water-soluble organic carbon (WSOC). Organic aerosol and SOA precursors were abundant at night, but additional improvements in daytime organic aerosol are needed to close the model–measurement gap. When taking into account deviations from ideality, including both inorganic (when RH > SRH) and organic water in the organic partitioning medium reduced the mean bias in SOA for routine monitoring networks and improved model performance compared to observations from SOAS. Property updates from this work will be released in CMAQ v5.2.

The Arctic region is vulnerable to climate change and able to affect global climate. The summertime Arctic atmosphere is pristine and strongly influenced by natural regional emissions, which have poorly understood climate impacts related to atmospheric particles and clouds. Here we show that ammonia from seabird-colony guano is a key factor contributing to bursts of newly formed particles, which are observed every summer in the near-surface atmosphere at Alert, Nunavut, Canada. Our chemical-transport model simulations indicate that the pan-Arctic seabird-influenced particles can grow by sulfuric acid and organic vapour condensation to diameters sufficiently large to promote pan-Arctic cloud-droplet formation in the clean Arctic summertime. We calculate that the resultant cooling tendencies could be large (about −0.5 W m−2 pan-Arctic-mean cooling), exceeding −1 W m−2 near the largest seabird colonies due to the effects of seabird-influenced particles on cloud albedo. These coupled ecological–chemical processes may be susceptible to Arctic warming and industrialization.