Sharp rises in the atmospheric abundance of ethane (C 2 H 6 ) have been detected from 2009 onwards in the Northern Hemisphere as a result of the unprecedented growth in the exploitation of shale gas and tight oil reservoirs in North America. Using time series of C 2 H 6 total columns derived from groundbased Fourier transform infrared (FTIR) observations made at five selected Network for the Detection of Atmospheric Composition Change sites, we characterize the recent C 2 H 6 evolution and determine growth rates of ∼5% yr −1 at mid-latitudes and of ∼3% yr −1 at remote sites. Results from CAM-chem simulations with the Hemispheric Transport of Air Pollutants, Phase II bottom-up inventory for anthropogenic emissions are found to greatly underestimate the current C 2 H 6 abundances. Doubling global emissions is required to reconcile the simulations and the observations prior to 2009. We further estimate that North American anthropogenic C 2 H 6 emissions have increased from 1.6 Tg yr −1 in 2008 to 2.8 Tg yr −1 in 2014, i.e. by 75% over these six years. We also completed a second simulation with new top-down emissions of C 2 H 6 from North American oil and gas activities, biofuel consumption and biomass burning, inferred from space-borne observations of methane (CH 4 ) from Greenhouse Gases Observing SATellite. In this simulation, GEOS-Chem is able to reproduce FTIR measurements at the mid-latitudinal sites, underscoring the impact of the North American oil and gas development on the current C 2 H 6 abundance. Finally we estimate that the North American oil and gas emissions of CH 4 , a major greenhouse gas, grew from 20 to 35 Tg yr −1 over the period 2008-2014, in association with the recent C 2 H 6 rise.
Abstract. As an ubiquitous product of the oxidation of many volatile organic compounds (VOCs), formaldehyde (HCHO) plays a key role as a short-lived and reactive intermediate in the atmospheric photo-oxidation pathways leading to the formation of tropospheric ozone and secondary organic aerosols. In this study, HCHO profiles have been successfully retrieved from ground-based Fourier transform infrared (FTIR) solar spectra and UV-visible Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) scans recorded during the July 2010–December 2012 time period at the Jungfraujoch station (Swiss Alps, 46.5° N, 8.0° E, 3580 m a.s.l.). Analysis of the retrieved products has revealed different vertical sensitivity between both remote sensing techniques. Furthermore, HCHO amounts simulated by two state-of-the-art chemical transport models (CTMs), GEOS-Chem and IMAGES v2, have been compared to FTIR total columns and MAX-DOAS 3.6–8 km partial columns, accounting for the respective vertical resolution of each ground-based instrument. Using the CTM outputs as the intermediate, FTIR and MAX-DOAS retrievals have shown consistent seasonal modulations of HCHO throughout the investigated period, characterized by summertime maximum and wintertime minimum. Such comparisons have also highlighted that FTIR and MAX-DOAS provide complementary products for the HCHO retrieval above the Jungfraujoch station. Finally, tests have revealed that the updated IR parameters from the HITRAN 2012 database have a cumulative effect and significantly decrease the retrieved HCHO columns with respect to the use of the HITRAN 2008 compilation.
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