期刊
ATMOSPHERIC CHEMISTRY AND PHYSICS
卷 17, 期 17, 页码 10269-10290出版社
COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-17-10269-2017
关键词
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资金
- Australian Government's Australian Antarctic science grant program [FoRCES 4012]
- Australian Research Council's Centre of Excellence for Climate System Science [CE110001028]
- Commonwealth Department of the Environment ozone summer scholar program
- Australian Government Research Training Program (RTP) Scholarship
Stratosphere-to-troposphere transport (STT) provides an important natural source of ozone to the upper troposphere, but the characteristics of STT events in the Southern Hemisphere extratropics and their contribution to the regional tropospheric ozone budget remain poorly constrained. Here, we develop a quantitative method to identify STT events from ozonesonde profiles. Using this method we estimate the seasonality of STT events and quantify the ozone transported across the tropopause over Davis (69 degrees S, 20062013), Macquarie Island (54 degrees S, 2004-2013), and Melbourne (38 degrees S, 2004-2013). STT seasonality is determined by two distinct methods: a Fourier bandpass filter of the vertical ozone profile and an analysis of the Brunt-Vaisala frequency. Using a bandpass filter on 7-9 years of ozone profiles from each site provides clear detection of STT events, with maximum occurrences during summer and minimum during winter for all three sites. The majority of tropospheric ozone enhancements owing to STT events occur within 2.5 and 3 km of the tropopause at Davis and Macquarie Island respectively. Events are more spread out at Melbourne, occurring frequently up to 6 km from the tropopause. The mean fraction of total tropospheric ozone attributed to STT during STT events is similar to 1.0-3.5% at each site; however, during individual events, over 10% of tropospheric ozone may be directly transported from the stratosphere. The cause of STTs is determined to be largely due to synoptic low-pressure frontal systems, determined using coincident ERA-Interim reanalysis meteorological data. Ozone enhancements can also be caused by biomass burning plumes transported from Africa and South America, which are apparent during austral winter and spring and are determined using satellite measurements of CO. To provide regional context for the ozonesonde observations, we use the GEOS-Chem chemical transport model, which is too coarsely resolved to distinguish STT events but is able to accurately simulate the seasonal cycle of tropospheric ozone columns over the three southern hemispheric sites. Combining the ozonesonde-derived STT event characteristics with the simulated tropospheric ozone columns from GEOS-Chem, we estimate STT ozone flux near the three sites and see austral summer dominated yearly amounts of between 5.7 and 8.7 x 10(17) molecules cm(-2) a(-1).
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