Boreal forest fire impacts on lower troposphere carbon monoxide and ozone levels at the regional to hemispheric scales

Tropospheric ozone (O3) and carbon monoxide (CO) pollution in the Northern Hemisphere is commonly thought to be of anthropogenic origin. While this is true in most cases, copious quantities of pollutants are emitted by fires in boreal regions, and the impact of these fires on CO has been shown to significantly exceed the impact of urban and industrial sources during large fire years. The impact of boreal fires on ozone is still poorly quantified, and large uncertainties exist in the estimates of the fire-released nitrogen oxides (NO x ), a critical factor in ozone production. As boreal fire activity is predicted to increase in the future due to its strong dependence on weather conditions, it is necessary to understand how these fires affect atmospheric composition. To determine the scale of boreal fire impacts on ozone and its precursors, this work combined statistical analysis of ground-based measurements downwind of fires, satellite data analysis, transport modeling and the results of chemical model simulations. The first part of this work focused on determining boreal fire impact on ozone levels downwind of fires, using analysis of observations in several-days-old fire plumes intercepted at the Pico Mountain station (Azores). The results of this study revealed that fires significantly increase midlatitude summertime ozone background during high fire years, implying that predicted future increases in boreal wildfires may affect ozone levels over large regions in the Northern Hemisphere. To improve current estimates of NOx emissions from boreal fires, we further analyzed ΔNOy /ΔCO enhancement ratios in the observed fire plumes together with transport modeling of fire emission estimates. The results of this analysis revealed the presence of a considerable seasonal trend in the fire NOx /CO emission ratio due to the late-summer changes in burning properties. This finding implies that the constant NOx /CO emission ratio currently used in atmospheric modeling is unrealistic, and is likely to introduce a significant bias in the estimated ozone production. Finally, satellite observations were used to determine the impact of fires on atmospheric burdens of nitrogen dioxide (NO2 ) and formaldehyde (HCHO) in the North American boreal region. This analysis demonstrated that fires dominated the HCHO burden over the fires and in plumes up to two days old. This finding provides insights into the magnitude of secondary HCHO production and further enhances scientific understanding of the atmospheric impacts of boreal fires

Assessment of source contributions to seasonal vegetative exposure to ozone in the U.S.

W126 is a cumulative ozone exposure index based on sigmoidally weighted daytime ozone concentrations used to evaluate the impacts of ozone on vegetation. We quantify W126 in the U.S. in the absence of North American anthropogenic emissions (North American background or “NAB”) using three regional or global chemical transport models for May–July 2010. All models overestimate W126 in the eastern U.S. due to a persistent bias in daytime ozone, while the models are relatively unbiased in California and the Intermountain West. Substantial difference in the magnitude and spatial and temporal variability of the estimates of W126 NAB between models supports the need for a multimodel approach. While the average NAB contribution to daytime ozone in the Intermountain West is 64–78%, the average W126 NAB is only 9–27% of current levels, owing to the weight given to high O3 concentrations in W126. Based on a three-model mean, NAB explains ~30% of the daily variability in the W126 daily index in the Intermountain West. Adjoint sensitivity analysis shows that nationwide W126 is influenced most by NOx emissions from anthropogenic (58% of the total sensitivity) and natural (25%) sources followed by nonmethane volatile organic compounds (10%) and CO (7%). Most of the influence of anthropogenic NOx comes from the U.S. (80%), followed by Canada (9%), Mexico (4%), and China (3%). Thus, long-range transport of pollution has a relatively small impact on W126 in the U.S., and domestic emissions control should be effective for reducing W126 levels

Assessing source characteristics of PM \u3c inf\u3e 2.5 in the eastern united states using positive matrix factorization

Fine aerosol (PM2.5) measurements obtained from the first year of operation of the nationwide network of PM25 monitors were studied with the factor analysis technique of positive matrix factorization (PMF). PM2.5 mass concentration data were extracted from the Atmospheric Information Retrieval System (AIRS) database of the U.S. Environmental Protection Agency (EPA). PMF was applied to measurements at more than 350 monitoring locations in the eastern half of the United States. Data consisted of PM2.5 24-hr averaged concentrations measured every third day from April through December 1999. The PMF model suggested six factors representing source influences to the PM2.5 mass concentrations at measurement sites. Factor 5, covering much of the Appalachian states, exhibited significant seasonal behavior. © 2004 Air & Waste Management Association