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Fossil fuel CO2 (CO2ff) is the major contributor\udof anthropogenic CO2 in the atmosphere, and accurate quantification is\udessential to better understand the carbon cycle. Since October 2012, we have\udbeen continuously measuring the mixing ratios of CO, CO2, CH4, and\udH2O at five different heights at the Beromünster tall tower,\udSwitzerland. Air samples for radiocarbon (Δ14CO2) analysis\udhave also been collected from the highest sampling inlet (212.5 m) of the\udtower on a biweekly basis. A correction was applied for 14CO2\udemissions from nearby nuclear power plants (NPPs), which have been simulated\udwith the Lagrangian transport model FLEXPART-COSMO. The 14CO2\udemissions from NPPs offset the depletion in 14C by fossil fuel\udemissions, resulting in an underestimation of the fossil fuel component in atmospheric\udCO2 by about 16 %. An average observed ratio (RCO) of 13.4 ± 1.3 mmol mol−1\udwas calculated from the enhancements in CO mixing ratios\udrelative to the clean-air reference site Jungfraujoch (ΔCO) and the\udradiocarbon-based fossil fuel CO2 mole fractions. The wintertime\udRCO estimate of 12.5 ± 3.3 is about 30 % higher than the\udwintertime ratio between in situ measured CO and CO2 enhancements at\udBeromünster over the Jungfraujoch background (8.7 mmol mol−1) corrected for\udnon-fossil contributions due to strong biospheric contribution despite the\udstrong correlation between ΔCO and ΔCO2 in winter. By\udcombining the ratio derived using the radiocarbon measurements and the\udin situ measured CO mixing ratios, a high-resolution time series of\udCO2ff was calculated exhibiting a clear seasonality driven by seasonal\udvariability in emissions and vertical mixing. By subtracting the fossil fuel\udcomponent and the large-scale background, we have determined the regional\udbiospheric CO2 component that is characterized by seasonal variations\udranging between −15 and +30 ppm. A pronounced diurnal variation was observed\udduring summer modulated by biospheric exchange and vertical mixing, while no\udconsistent pattern was found during winter

atmospheric chemistry and physics

Estimation of the fossil fuel component in atmospheric CO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; based on radiocarbon measurements at the Beromünster tall tower, Switzerland