1Center for Spatial Information Science and Systems, George Mason University, Fairfax, VA, USA
2National Oceanic and Atmospheric Administration (NOAA), Air Resource Laboratory, College Park, Maryland, USA
Received: 12 Jul 2013 – Discussion started: 23 Aug 2013
Abstract. As precursors to tropospheric ozone and nitrate, nitrogen oxide (NOx) in the present atmosphere and its transformation in response to emission and climate perturbations are studied by using the CAM-Chem model and air quality measurements from the National Emissions Inventory (NEI), Clean Air Status and Trends Network (CASTNET), and Environmental Protection Agency Air Quality System (EPA AQS). It is found that NOx transformations in present atmospheric conditions show different sensitivities over industrial and non-industrial regions. As a result, the surface ozone and nitrate formations can be divided into several regimes associated with the dominant emission types and relative levels of NOx and volatile organic compounds (VOC). Ozone production in industrial regions (the main NOx emission source areas) increases in warmer conditions and slightly decreases following an increase in NOx emissions due to NOx titration, which is opposite to the response in non-industrial regions. The ozone decrease following a temperature increase in non-industrial regions indicates that ozone production in regions that lack NOx emission sources may be sensitive to NOx transformation in remote source regions. The increase in NO2 from NOx titration over industrial regions results in an increase rate of total nitrate that remains higher than the increase rate of NOx emissions. The presented findings indicate that a change in the ozone concentration is more directly affected by changes in climate and precursor emissions, while a change in the nitrate concentration is affected by local ozone production types and their seasonal transfer. The sensitivity to temperature perturbations shows that a warmer climate accelerates the decomposition of odd nitrogen (NOy) during the night. As a result, the transformation rate of NOx to nitrate decreases. Examinations of the historical emissions and air quality records of a typical NOx-limited area, such as Atlanta and a VOC-limited area, such as Los Angeles further confirm the conclusions drawn from the modeling experiments.
Revised: 01 Jan 2014 – Accepted: 03 Jan 2014 – Published: 05 Feb 2014
Lei, H. and Wang, J. X. L.: Sensitivities of NOx transformation and the effects on surface ozone and nitrate, Atmos. Chem. Phys., 14, 1385-1396, doi:10.5194/acp-14-1385-2014, 2014.