Abstract

We examine the ozone production efficiency in transpacific Asian pollution plumes, and the implications for ozone air quality in California, by using aircraft and surface observations in April–May 2002 from the Intercontinental Transport and Chemical Transformation 2002 (ITCT 2K2) campaign off the California coast and the Pacific Exploration of Asian Continental Emission–B (PEACE‐B) campaign over the northwest Pacific. The observations are interpreted with a global three‐dimensional chemical transport model (GEOS‐CHEM). The model reproduces the mean features observed for CO, reactive nitrogen oxides (NOy), and ozone but underestimates the strong (∼20 ppbv) stratospheric contribution to ozone in the middle troposphere. The ITCT 2K2 aircraft sampled two major transpacific Asian pollution plumes, one on 5 May at 5–8 km altitude with CO up to 275 ppbv but no elevated ozone and one on 17 May at 2.5–4 km altitude with CO up to 225 ppbv and ozone up to 90 ppbv. We show that the elevated ozone in the latter plume is consistent with production from peroxyacetylnitrate (PAN) decomposition during subsidence of the plume over the northeast Pacific. This production is particularly efficient because of the strong radiation and low humidity of the subsiding environment. We argue that such PAN decomposition represents a major and possibly dominant component of the ozone enhancement in transpacific Asian pollution plumes. Strong dilution of Asian pollution plumes takes place during entrainment in the U.S. boundary layer, greatly reducing their impact at U.S. surface sites. California mountain sites are more sensitive to Asian pollution because of their exposure to the free troposphere. Model results indicate a mean Asian pollution enhancement of 7 ppbv ozone at Sequoia National Park in May 2002 on those days when the 8‐hour average ozone concentration exceeded 80 ppbv.

Highlights

  • Troposphere—constituent transport and chemistry; 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); KEYWORDS: ozone, Asian pollution, ITCT 2K2, Pacific Exploration of Asian Continental Emission–B (PEACE-B), transpacific transport

  • The PHOBEA aircraft campaigns over the NW coast of the United States observed a number of transpacific Asian pollution plumes with elevated carbon monoxide (CO) and dust, and with variable enhancements of ozone [Jaffe et al, 1999, 2003a, 2003b; Price et al, 2003, 2004; Bertschi et al, 2004]

  • [4] A critical issue in relating NOx emissions to global ozone production is the fraction of emitted NOx that is ventilated out of the continental boundary layer [Jacob et al, 1993]

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Summary

Introduction

[2] Rapid industrialization of the Asian continent may have important implications for global tropospheric ozone [Berntsen et al, 1997; Gupta et al, 1998; Wild and Akimoto, 2001] and surface ozone air quality in the United. [19] Figure 5 compares simulated and observed mean vertical concentration profiles of CO, NOy components, and ozone along the ITCT 2K2 aircraft flight tracks In this comparison we have excluded data from transit flights, flights targeted at local ship and urban plumes (flights 7, 10, and 13), observations in the continental boundary layer (CBL) over land, fresh combustion plumes (diagnosed by aerosol concentrations higher than 2000 cmÀ3 and either NO or NO2 greater than 500 pptv), and stratospheric air (diagnosed by O3 > 100 ppbv and CO < 100 ppbv). 75% of the observed ozonesonde profiles show high-ozone layers (enhancements > 10 ppbv) at 1– 5 km altitude, and the majority of these layers appear to originate from the stratosphere (based on low humidity, back-trajectories, and potential vorticity)

Ozone Production in Transpacific Pollution Plumes
Findings
Conclusions
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