X. Liu, Y. Zhang, L. G. Huey, RJ Yokelson, Y. Wang, J. L. Jimenez, P Campuzano-Jost, AJ Beyersdorf, DR Blake, Y Choi, and others. 2016. “
Agricultural Fires in the Southeastern US during SEAC4RS: Emissions of Trace Gases and Particles and Evolution of Ozone, Reactive Nitrogen, and Organic Aerosol.” Journal of Geophysical Research: Atmospheres.
Publisher's VersionAbstractEmissions from 15 agricultural fires in the southeastern U.S. were measured from the NASA DC-8 research aircraft during the summer 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. This study reports a detailed set of emission factors (EFs) for 25 trace gases and 6 fine particle species. The chemical evolution of the primary emissions in seven plumes was examined in detail for ~1.2 h. A Lagrangian plume cross-section model was used to simulate the evolution of ozone (O3), reactive nitrogen species, and organic aerosol (OA). Observed EFs are generally consistent with previous measurements of crop residue burning, but the fires studied here emitted high amounts of SO2 and fine particles, especially primary OA and chloride. Filter-based measurements of aerosol light absorption implied that brown carbon (BrC) was ubiquitous in the plumes. In aged plumes, rapid production of O3, peroxyacetyl nitrate (PAN), and nitrate was observed with ΔO3/ΔCO, ΔPAN/ΔNOy, and Δnitrate/ΔNOy reaching ~0.1, ~0.3, and ~0.3. For five selected cases, the model reasonably simulated O3 formation but underestimated PAN formation. No significant evolution of OA mass or BrC absorption was observed. However, a consistent increase in oxygen-to-carbon (O/C) ratios of OA indicated that OA oxidation in the agricultural fire plumes was much faster than in urban and forest fire plumes. Finally, total annual SO2, NOx, and CO emissions from agricultural fires in Arkansas, Louisiana, Mississippi, and Missouri were estimated (within a factor of ~2) to be equivalent to ~2% SO2 from coal combustion and ~1% NOx and ~9% CO from mobile sources.
Yuzhong Zhang and Yuhang Wang. 2016. “
Climate-driven ground-level ozone extreme in the fall over the Southeast United States.” Proceedings of the National Academy of Sciences, Pp. 201602563.
Publisher's VersionAbstract

Ground-level ozone is adverse to human and vegetation health. High ground-level ozone concentrations usually occur over the United States in the summer, often referred to as the ozone season. However, observed monthly mean ozone concentrations in the southeastern United States were higher in October than July in 2010. The October ozone average in 2010 reached that of July in the past three decades (1980–2010). Our analysis shows that this extreme October ozone in 2010 over the Southeast is due in part to a dry and warm weather condition, which enhances photochemical production, air stagnation, and fire emissions. Observational evidence and modeling analysis also indicate that another significant contributor is enhanced emissions of biogenic isoprene, a major ozone precursor, from water-stressed plants under a dry and warm condition. The latter finding is corroborated by recent laboratory and field studies. This climate-induced biogenic control also explains the puzzling fact that the two extremes of high October ozone both occurred in the 2000s when anthropogenic emissions were lower than the 1980s and 1990s, in contrast to the observed decreasing trend of July ozone in the region. The occurrences of a drying and warming fall, projected by climate models, will likely lead to more active photochemistry, enhanced biogenic isoprene and fire emissions, an extension of the ozone season from summer to fall, and an increase of secondary organic aerosols in the Southeast, posing challenges to regional air quality management.
Dasa Gu, Yuhang Wang, Ran Yin, Yuzhong Zhang, and Charles Smeltzer. 2016. “
Inverse modelling of NO x emissions over eastern China: uncertainties due to chemical non-linearity.” Atmospheric Measurement Techniques, 9, 10, Pp. 5193.
Publisher's VersionAbstractSatellite observations of nitrogen dioxide (NO2) have often been used to derive nitrogen oxides (NOx = NO + NO2) emissions. A widely used inversion method was developed by Martin et al. (2003). Refinements of this method were subsequently developed. In the context of this inversion method, we show that the local derivative (of a first-order Taylor expansion) is more appropriate than the “bulk ratio” (ratio of emission to column) used in the original formulation for polluted regions. Using the bulk ratio can lead to biases in regions of high NOx emissions such as eastern China due to chemical non-linearity. Inverse modelling using the local derivative method is applied to both GOME-2 and OMI satellite measurements to estimate anthropogenic NOx emissions over eastern China. Compared with the traditional method using bulk ratio, the local derivative method produces more consistent NOx emission estimates between the inversion results using GOME-2 and OMI measurements. The results also show significant changes in the spatial distribution of NOx emissions, especially over high emission regions of eastern China. We further discuss a potential pitfall of using the difference of two satellite measurements to derive NOx emissions. Our analysis suggests that chemical non-linearity needs to be accounted for and that a careful bias analysis is required in order to use the satellite differential method in inverse modelling of NOx emissions.
Yuzhong Zhang, Yuhang Wang, Gao Chen, Charles Smeltzer, James Crawford, Jennifer Olson, James Szykman, Andrew J Weinheimer, David J Knapp, Denise D Montzka, and others. 2016. “
Large vertical gradient of reactive nitrogen oxides in the boundary layer: Modeling analysis of DISCOVER-AQ 2011 observations.” Journal of Geophysical Research: Atmospheres.
Publisher's VersionAbstract

An often used assumption in air pollution studies is a well-mixed boundary layer (BL), where pollutants are evenly distributed. Because of the difficulty in obtaining vertically resolved measurements, the validity of the assumption has not been thoroughly evaluated. In this study, we use more than 200 vertical profiles observed in the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) aircraft campaign in July 2011 to examine the vertical distributions of pollutants over the Washington-Baltimore area. While many long-lived species are well mixed in daytime, the observed average vertical profile of NOx shows a large negative gradient with increasing altitude in the BL. Our analysis suggests that the magnitude of the NOxgradient is highly sensitive to atmospheric stability. We investigate how parameterizations of the BL and land-surface processes impact vertical profiles in a 1-D chemical transport model, using three BL schemes (Asymmetric Convective Model version 2 (ACM2), Yonsei University (YSU), and Mellor-Yamada-Janjic (MYJ)) and two land-surface schemes (Noah and Rapid Update Cycle (RUC)). The model reasonably reproduces the median vertical profiles of NOx under different BL stability conditions within 30% of observations, classified based on potential temperature gradient and BL height. Comparisons with NOx observations for individual vertical profiles reveal that while YSU performs better in the turbulent and deep BL case, in general, ACM2 (RMSE = 2.0 ppbv) outperforms YSU (RMSE = 2.5 ppbv) and MYJ (RMSE = 2.2 ppbv). Results also indicate that the land-surface schemes in the Weather Research and Forecasting (WRF) model have a small impact on the NOx gradient. Using model simulations, we analyze the impact of BL NOx gradient on the calculation of the ozone production rate and satellite NO2retrieval. We show that using surface measurements and the well-mixed BL assumption causes a ~45% high bias in the estimated BL ozone production rate and that the variability of NO2 vertical profiles is responsible for 5–10% variability in the retrieved NO2 tropospheric vertical columns.