On the effectiveness of nitrogen oxide reductions as a control over ammonium nitrate aerosol

oleh: S. E. Pusede, S. E. Pusede, K. C. Duffey, A. A. Shusterman, A. Saleh, J. L. Laughner, P. J. Wooldridge, Q. Zhang, C. L. Parworth, H. Kim, S. L. Capps, L. C. Valin, C. D. Cappa, A. Fried, J. Walega, J. B. Nowak, A. J. Weinheimer, R. M. Hoff, T. A. Berkoff, A. J. Beyersdorf, J. Olson, J. H. Crawford, R. C. Cohen, R. C. Cohen

Format: Article
Diterbitkan: Copernicus Publications 2016-03-01

Deskripsi

Nitrogen oxides (NO<sub><i>x</i></sub>) have fallen steadily across the US over the last 15 years. At the same time, NO<sub><i>x</i></sub> concentrations decrease on weekends relative to weekdays, largely without co-occurring changes in other gas-phase emissions, due to patterns of diesel truck activities. These trends taken together provide two independent constraints on the role of NO<sub><i>x</i></sub> in the nonlinear chemistry of atmospheric oxidation. In this context, we interpret interannual trends in wintertime ammonium nitrate (NH<sub>4</sub>NO<sub>3</sub>) in the San Joaquin Valley of California, a location with the worst aerosol pollution in the US and where a large portion of aerosol mass is NH<sub>4</sub>NO<sub>3</sub>. Here, we show that NO<sub><i>x</i></sub> reductions have simultaneously decreased nighttime and increased daytime NH<sub>4</sub>NO<sub>3</sub> production over the last decade. We find a substantial decrease in NH<sub>4</sub>NO<sub>3</sub> since 2000 and conclude that this decrease is due to reduced nitrate radical-initiated production at night in residual layers that are decoupled from fresh emissions at the surface. Further reductions in NO<sub><i>x</i></sub> are imminent in California, and nationwide, and we make a quantitative prediction of the response of NH<sub>4</sub>NO<sub>3</sub>. We show that the combination of rapid chemical production and efficient NH<sub>4</sub>NO<sub>3</sub> loss via deposition of gas-phase nitric acid implies that high aerosol days in cities in the San Joaquin Valley air basin are responsive to local changes in NO<sub><i>x</i></sub> within those individual cities. Our calculations indicate that large decreases in NO<sub><i>x</i></sub> in the future will not only lower wintertime NH<sub>4</sub>NO<sub>3</sub> concentrations but also cause a transition in the dominant NH<sub>4</sub>NO<sub>3</sub> source from nighttime to daytime chemistry.