Published in

European Geosciences Union, Atmospheric Chemistry and Physics, 9(15), p. 5161-5179, 2015

DOI: 10.5194/acp-15-5161-2015

European Geosciences Union, Atmospheric Chemistry and Physics Discussions, 23(14), p. 32583-32627

DOI: 10.5194/acpd-14-32583-2014

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Origin of springtime ozone enhancements in the lower troposphere over Beijing: in situ measurements and model analysis

This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Abstract

Ozone (O 3 ) concentrations in the lower troposphere (LT) over Beijing have significantly increased over the past 2 decades as a result of rapid industrialization in China, with important implications for regional air quality and the photochemistry of the background troposphere. We characterize the vertical distribution of lower-tropospheric (0–6 km) O 3 over Beijing using observations from 16 ozonesonde soundings during a field campaign in April–May 2005 and MOZAIC (Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft) over 13 days in the same period. We focus on the origin of LT O 3 enhancements observed over Beijing, particularly in May. We use a global 3-D chemistry and transport model (GEOS-Chem CTM; GEOS – Goddard Earth Observing System) driven by assimilated meteorological fields to examine the transport pathways for O 3 pollution and to quantify the sources contributing to O 3 and its enhancements in the springtime LT over Beijing. Output from the Global Modeling Initiative (GMI) CTM is also used. High O 3 concentrations (up to 94.7 ppbv) were frequently observed at the altitude of ~ 1.5–2 km. The CTMs captured the timing of the occurrences but significantly underestimated their magnitude. GEOS-Chem simulations and a case study showed that O 3 produced in the Asian troposphere (especially from Asian anthropogenic pollution) made major contributions to the observed O 3 enhancements. Contributions from anthropogenic pollution in the European and North American troposphere were reduced during these events, in contrast with days without O 3 enhancements when contributions from Europe and North America were substantial. The O 3 enhancements typically occurred under southerly wind and warmer conditions. It is suggested that an earlier onset of the Asian summer monsoon would cause more O 3 enhancement events in the LT over the North China Plain in late spring and early summer.