[1] Many prior studies clearly document episodic Asian pollution in the western U.S. free troposphere. Here, we examine the mechanisms involved in the transport of Asian pollution plumes into western U.S. surface air through an integrated analysis of in situ and satellite measurements in May-June 2010 with a new global high-resolution ($50 Â 50 km 2 ) chemistry-climate model (GFDL AM3). We find that AM3 with full stratosphere-troposphere chemistry nudged to reanalysis winds successfully reproduces observed sharp ozone gradients above California, including the interleaving and mixing of Asian pollution and stratospheric air associated with complex interactions of midlatitude cyclone air streams. Asian pollution descends isentropically behind cold fronts; at $800 hPa a maximum enhancement to ozone occurs over the southwestern U.S., including the densely populated Los Angeles Basin. During strong episodes, Asian emissions can contribute 8-15 ppbv ozone in the model on days when observed daily maximum 8-h average ozone (MDA8 O 3 ) exceeds 60 ppbv. We find that in the absence of Asian anthropogenic emissions, 20% of MDA8 O 3 exceedances of 60 ppbv in the model would not have occurred in the southwestern USA. For a 75 ppbv threshold, that statistic increases to 53%. Our analysis indicates the potential for Asian emissions to contribute to high-O 3 episodes over the high-elevation western USA, with implications for attaining more stringent ozone standards in this region. We further demonstrate a proof-of-concept approach using satellite CO column measurements as a qualitative early warning indicator to forecast Asian ozone pollution events in the western U.S. with lead times of 1-3 days. Citation: Lin, M., et al. (2012), Transport of Asian ozone pollution into surface air over the western United States in spring,
[1] Airborne and ground-based measurements during the CalNex (California Research at the Nexus of Air Quality and Climate Change) field study in May/June 2010 show a weekend effect in ozone in the South Coast Air Basin (SoCAB) consistent with previous observations. The well-known and much-studied weekend ozone effect has been attributed to weekend reductions in nitrogen oxide (NO x = NO + NO 2 ) emissions, which affect ozone levels via two processes: (1) reduced ozone loss by titration and (2) enhanced photochemical production of ozone due to an increased ratio of non-methane volatile organic compounds (VOCs) to NO x . In accord with previous assessments, the 2010 airborne and ground-based data show an average decrease in NO x of 46 AE 11% and 34 AE 4%, respectively, and an average increase in VOC/NO x ratio of 48 AE 8% and 43 AE 22%, respectively, on weekends. This work extends current understanding of the weekend ozone effect in the SoCAB by identifying its major causes and quantifying their relative importance from the available CalNex data. Increased weekend production of a VOC-NO x oxidation product, peroxyacetyl nitrate, compared to a radical termination product, nitric acid, indicates a significant contribution from increased photochemical production on weekends. Weekday-to-weekend differences in the products of NO x oxidation show 45 AE 13% and 42 AE 12% more extensive photochemical processing and, when compared with odd oxygen (O x = O 3 + NO 2 ), 51 AE 14% and 22 AE 17% greater ozone production efficiency on weekends in the airborne and ground-based data, respectively, indicating that both contribute to higher weekend ozone levels in the SoCAB.
Abstract. As part of the North Atlantic Regional Experiment (NARE), instrumentation for the measurement of O 3 and CO was included on research flights conducted by the National Oceanic and Atmospheric Administration WP-3D Orion aircraft from St. John' s, Newfoundland, Canada, and Kefiavik, Iceland, from February 2 to 25, 1999. These flights sampled the lower troposphere over the western North Atlantic Ocean. One significant feature observed during these flights was the close proximity of air masses with contrasting source signatures: high levels of anthropogenic pollution immediately adjacent to elevated O3 of stratospheric origin. Here we present a case study showing the most pronounced example of this proximity, which was associated with a frontal passage across North America and out into the North Atlantic region. Trajectory analyses and satellite imagery are used to investigate the transport mechanisms that create the interleaving of air masses from the different sources. One important chemical feature was noted: in air masses with differing amounts of anthropogenic pollution admixed, O3 was negatively correlated with CO, which indicates that emissions from surface anthropogenic sources had reduced O3 in this wintertime period, even in air masses transported into the free troposphere.
Ozone, carbon monoxide, aerosol extinction coefficient, acetonitrile, nitric acid and relative humidity measured from the NOAA P3 aircraft during the Tex-AQS/GoMACCS 2006 experiment, indicate mixing between a biomass burning plume and a stratospheric intrusion in the free troposphere above eastern Texas. Lagrangianbased transport analysis and satellite imagery are used to investigate the transport mechanisms that bring together the tropopause fold and the biomass burning plume originating in southern California, which may affect the chemical budget of tropospheric trace gases.
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