Abstract. Tropospheric ozone results from in situ chemical formation and stratosphere–troposphere exchange (STE), with the latter being more important in the middle and upper troposphere than in the lower troposphere. Ozone photochemical formation is nonlinear and results from the oxidation of methane and non-methane hydrocarbons (NMHCs) in the presence of nitrogen oxide (NOx=NO+NO2). Previous studies showed that O3 short- and long-term trends are nonlinearly controlled by near-surface anthropogenic emissions of carbon monoxide (CO), volatile organic compounds (VOCs), and nitrogen oxides, which may also be impacted by the long-range transport (LRT) of O3 and its precursors. In addition, several studies have demonstrated the important role of STE in enhancing ozone levels, especially in the midlatitudes. In this article, we investigate tropospheric ozone spatial variability and trends from 2005 to 2019 and relate those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone (TrC-O3) and its precursors, nitrogen dioxide (TrC-NO2), formaldehyde (TrC-HCHO), and total column CO (TC-CO), as well as ozonesonde data and model simulations. Our results indicate a complex relationship between tropospheric ozone column levels, surface ozone levels, and ozone precursors. While the increasing trends of near-surface ozone concentrations can largely be explained by variations in VOC and NOx concentration under different regimes, TrC-O3 may also be affected by other variables such as tropopause height and STE as well as LRT. Decreasing or increasing trends in TrC-NO2 have varying effects on TrC-O3, which is related to the different local chemistry in each region. We also shed light on the contribution of NOx lightning and soil NO and nitrous acid (HONO) emissions to trends of tropospheric ozone on regional and global scales.
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Local and Regional Contributions to Tropospheric Ozone Concentrations
The Wasatch Front in Utah, USA is currently a non-attainment area for ozone according to the Environmental Protection Agency’s (EPA) National Ambient Air Quality Standards (NAAQS). Nitrogen oxides (NOx = NO2 + NO) and volatile organic compounds (VOCs) in the presence of sunlight lead to ozone formation in the troposphere. When the rate of oxidant production, defined as the sum of O3 and NO2, is faster than the rate of NOx production, a region is said to be NOx-limited and ozone formation will be limited by the concentration of NOx species in the region. The inverse of this situation makes the region VOC-limited. Knowing if a region is NOx-limited or VOC-limited can aid in generating effective mitigation strategies. Understanding the background or regional contributions to ozone in a region, whether it be from the transport of precursors or of ozone, provides information about the lower limit for ozone concentrations that a region can obtain with regulation of local precursors. In this paper, measured oxidant and NOx concentrations are analyzed from 14 counties in the state of Utah to calculate the regional and local contributions to ozone for each region. This analysis is used to determine the nature of the atmosphere in each county by determining if the region is VOC- or NOx-limited. Furthermore, this analysis is performed for each county for the years 2012 and 2022 to determine if there has been a change in the oxidative nature and quantify the regional and local contributions to ozone over a 10-year period. All studied counties—except for Washington County—in Utah were found to be VOC-limited in 2012. This shifted in 2022 to most counties being either in a transitional state or being NOx-limited. Local contributions to ozone increased in two major counties, Cache and Salt Lake Counties, but decreased in Carbon, Davis, Duchesne, Uinta, Utah, Washington, and Weber Counties. Generally, the regional contributions to oxidant concentrations decreased across the state. A summertime spike in both regional and local contributions to oxidants was seen. Smoke from wildfires was seen to increase the regional contributions to oxidants and shift the local regime to be more NOx-limited.
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- Award ID(s):
- 2114655
- PAR ID:
- 10553099
- Publisher / Repository:
- MDPI
- Date Published:
- Journal Name:
- Atmosphere
- Volume:
- 14
- Issue:
- 8
- ISSN:
- 2073-4433
- Page Range / eLocation ID:
- 1262
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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