Continuous isotopic composition measurements of tropospheric CO2 at Jungfraujoch (3580 m a.s.l.), Switzerland: real-time observation of regional pollution events

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Abstract
A quantum cascade laser based absorption spectrometer (QCLAS) is applied for the first time to perform in situ, continuous and high precision isotope ratio measurements of CO2 in the free troposphere. Time series of the three main CO2 isotopologue mixing ratios (12C16CO2, 13C16CO2 and 12C18O16O) have simultaneously been measured at one second time resolution over two years (from August 2008 to present) at the High Altitude Research Station Jungfraujoch (3580 m a.s.l., Switzerland). This work focuses on periods in February 2009 only, when sudden and pronounced enhancements in the tropospheric CO2 were observed. These short-term changes were closely correlated with variations in CO mixing ratios measured at the same site, indicating combustion related emissions as potential source. The analytical precision of 0.046‰ (at 50 s integration time) for both δ13C and δ18O and the high temporal resolution allowed the application of the Keeling plot method for source signature identification. The spatial origin of these CO2 emission sources was then determined by backward Lagrangian particle dispersion simulations.
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