The chemical complexity of atmospheric organic aerosol (OA) has caused substantial uncertainties in understanding its origins and environmental impacts. Here, we provide constraints on OA origins through compositional characterization with molecular-level details. Our results suggest that secondary OA (SOA) from monoterpene oxidation accounts for approximately half of summertime fine OA in Centreville, AL, a forested area in the southeastern United States influenced by anthropogenic pollution. We find that different chemical processes involving nitrogen oxides, during days and nights, play a central role in determining the mass of monoterpene SOA produced. These findings elucidate the strong anthropogenic-biogenic interaction affecting ambient aerosol in the southeastern United States and point out the importance of reducing anthropogenic emissions, especially under a changing climate, where biogenic emissions will likely keep increasing.

Secondary organic aerosol (SOA) can affect the atmospheric radiation balance through absorbing light at shorter visible and UV wavelengths. However, the composition and optical properties of light-absorbing SOA is poorly understood. In this work, SOA filter samples were collected during individual chamber experiments conducted with three biogenic and eight aromatic volatile organic compound (VOC) precursors in the presence of NO and HO. Compared with the SOA generated using the aromatic precursors, biogenic SOA generally exhibits negligible light absorption above 350 nm; the aromatic SOA generated in the presence of NO shows stronger light absorption than that generated with HO. Fifteen nitroaromatic compound (NAC) chemical formulas were identified and quantified in SOA samples. Their contributions to the light absorption of sample extracts were also estimated. On average, the m-cresol/NO SOA sample has the highest mass contribution from NACs (10.4 ± 6.74%, w/w), followed by naphthalene/NO (6.41 ± 2.08%) and benzene/NO (5.81 ± 3.82%) SOA. The average contributions of NACs to total light absorption were at least two times greater than their average mass contributions at 365 and 400 nm, revealing the potential use of chromophoric NACs as brown carbon (BrC) tracers in source apportionment and air quality modeling studies.

Air quality impacts from wildfires have been dramatic in recent years, with millions of people exposed to elevated and sometimes hazardous fine particulate matter (PM 2.5) concentrations for extended periods. Fires emit particulate matter (PM) and gaseous compounds that can negatively impact human health and reduce visibility. While the overall trend in U.S. air quality has been improving for decades, largely due to implementation of the Clean Air Act, seasonal wildfires threaten to undo this in some regions of the United States. Our understanding of the health effects of smoke is growing with regard to respiratory and cardiovascular consequences and mortality. The costs of these health outcomes can exceed the billions already spent on wildfire suppression. In this critical review, we examine each of the processes that influence wildland fires and the effects of fires, including the natural role of wildland fire, forest management, ignitions, emissions, transport, chemistry, and human health impacts. We highlight key data gaps and examine the complexity and scope and scale of fire occurrence, estimated emissions, and resulting effects on regional air quality across the United States. The goal is to clarify which areas are well understood and which need more study. We conclude with a set of recommendations for future research. Implications: In the recent decade the area of wildfires in the United States has increased dramatically and the resulting smoke has exposed millions of people to unhealthy air quality. In this critical review we examine the key factors and impacts from fires including natural role of wildland fire, forest management, ignitions, emissions, transport, chemistry and human health.

Light-absorbing organic carbon (OC), also termed brown carbon (BrC), from laboratory-based biomass burning (BB) has been studied intensively to understand the contribution of BB to radiative forcing. However, relatively few measurements have been conducted on field-based BB and even fewer measurements have examined BrC from anthropogenic combustion sources like motor vehicle emissions. In this work, the light absorption of methanol-extractable OC from prescribed and laboratory BB and gasoline vehicle emissions was examined using spectrophotometry. The light absorption of methanol extracts showed a strong wavelength dependence for both BB and gasoline vehicle emissions. The mass absorption coefficients at 365 nm (MAC365, m2 g−1C) – used as a measurement proxy for BrC – were significantly correlated (p < 0.05) to the elemental carbon (EC)/OC ratios when examined by each BB fuel type. No significant correlation was observed when pooling fuels, indicating that both burn conditions and fuel types may impact BB BrC characteristics. The average MAC365 of gasoline vehicle emission samples is 0.62 ± 0.76 m2 g−1C, which is similar in magnitude to the BB samples (1.27 ± 0.76 m2 g−1C). These results suggest that in addition to BB, gasoline vehicle emissions may also be an important BrC source in urban areas.