The Total Carbon Column Observing Network (TCCON) is a ground-based network of Fourier Transform Spectrometer (FTS) sites around the globe, where the column abundances of CO₂, CH₄, N₂O, CO and O₂ are measured. CO₂ is constrained with a precision better than 0.25% (1-σ). To achieve a similarly high accuracy, calibration to World Meteorological Organization (WMO) standards is required. This paper introduces the first aircraft calibration campaign of five European TCCON sites and a mobile FTS instrument. A series of WMO standards in-situ profiles were obtained over European TCCON sites via aircraft and compared with retrievals of CO₂ column amounts from the TCCON instruments. The results of the campaign show that the FTS measurements are consistently biased 1.1% ± 0.2% low with respect to WMO standards, in agreement with previous TCCON calibration campaigns. The standard a priori profile for the TCCON FTS retrievals is shown to not add a bias. The same calibration factor is generated using aircraft profiles as a priori and with the TCCON standard a priori. With a calibration to WMO standards, the highly precise TCCON CO₂ measurements of total column concentrations provide a suitable database for the calibration and validation of nadir-viewing satellites.

The Laptev and East Siberian Seas have been proposed as a substantial source of methane (CH₄) to the atmosphere. During summer 2014, we made unique high‐resolution simultaneous measurements of CH₄ in the atmosphere above, and surface waters of, the Laptev and East Siberian Seas. Turbulence‐driven sea‐air fluxes along the ship's track were derived from these observations; an average diffusive flux of 2.99 mg m⁻² d⁻¹ was calculated for the Laptev Sea and for the ice‐free portions of the western East Siberian Sea, 3.80 mg m⁻² d⁻¹. Although seafloor bubble plumes were observed at two locations in the study area, our calculations suggest that regionally, turbulence‐driven diffusive flux alone accounts for the observed atmospheric CH₄ enhancements, with only a local, limited role for bubble fluxes, in contrast to earlier reports. CH₄ in subice seawater in certain areas suggests that a short‐lived flux also occurs annually at ice‐out.

Coastal ecosystems can efficiently remove carbon dioxide (CO₂) from the atmosphere and are thus promoted for nature-based climate change mitigation. Natural methane (CH₄) emissions from these ecosystems may counterbalance atmospheric CO₂ uptake. Still, knowledge of mechanisms sustaining such CH₄ emissions and their contribution to net radiative forcing remains scarce for globally prevalent macroalgae, mixed vegetation, and surrounding depositional sediment habitats. Here we show that these habitats emit CH₄ in the range of 0.1 – 2.9 mg CH₄ m⁻² d⁻¹ to the atmosphere, revealing in situ CH₄ emissions from macroalgae that were sustained by divergent methanogenic archaea in anoxic microsites. Over an annual cycle, CO₂-equivalent CH₄ emissions offset 28 and 35% of the carbon sink capacity attributed to atmospheric CO₂ uptake in the macroalgae and mixed vegetation habitats, respectively, and augment net CO₂ release of unvegetated sediments by 57%. Accounting for CH₄ alongside CO₂ sea-air fluxes and identifying the mechanisms controlling these emissions is crucial to constrain the potential of coastal ecosystems as net atmospheric carbon sinks and develop informed climate mitigation strategies.

In September/October 2009, six European ground-based Fourier Transform Spectrometers (FTS) of the Total Carbon Column Observation Network (TCCON) were calibrated for the first time using aircraft measurements. The campaign was part of the Infrastructure for Measurement of the European Carbon Cycle (IMECC) project. During this campaign, altitude profiles of several trace gases and meteorological parameters were taken close to the FTS sites (typically within 1–2 km distance for flight altitudes below 5000 m). Profiles of CO₂, CH₄, CO and H₂O were measured continuously. N₂O, H₂, and SF₆ were later derived from flask measurements. The aircraft data had a vertical coverage ranging from approximately 300 to 13 000 m, corresponding to ~80% of the total atmospheric column seen by the FTS. This study summarizes the calibration results for CH₄. The resulting calibration factor of 0.978 ± 0.002 (±1 σ) from the IMECC campaign agreed very well with the results that Wunch et al. (2010) had derived for TCCON instruments in North America, Australia, New Zealand, and Japan using similar methods. By combining our results with the data of Wunch et al. (2010), the uncertainty of the calibration factor could be reduced by a factor of three (compared to using only IMECC or only Wunch et al. (2010) data). A careful analysis of the calibration method used by Wunch et al. (2010) revealed that the incomplete vertical coverage of the aircraft profiles can lead to a bias in the calibration factor. This bias can be compensated with a new iterative approach that we developed. Using this improved method, we derived a significantly lower calibration factor of 0.974 ± 0.002 (±1 σ). This corresponds to a correction of all TCCON CH₄ measurements by roughly −7 ppb.

The Arctic Ocean is an important sink for atmospheric CO₂. The impact of decreasing sea ice extent and expanding marginal ice zones on Arctic air‐sea CO₂ exchange depends on the rate of gas transfer in the presence of sea ice. Sea ice acts to limit air‐sea gas exchange by reducing contact between air and water but is also hypothesized to enhance gas transfer rates across surrounding open‐water surfaces through physical processes such as increased surface‐ocean turbulence from ice‐water shear and ice‐edge form drag. Here we present the first direct determination of the CO₂ air‐sea gas transfer velocity in a wide range of Arctic sea ice conditions. We show that the gas transfer velocity increases near linearly with decreasing sea ice concentration. We also show that previous modeling approaches overestimate gas transfer rates in sea ice regions.

This article introduces a new fully automated FTIR system that is part of the Total Carbon Column Observing Network (TCCON). It will provide continuous ground-based measurements of column-averaged volume mixing ratio for CO₂, CH₄ and several other greenhouse gases in the tropics. Housed in a 20-foot shipping container it was developed as a transportable system that could be deployed almost anywhere in the world. We describe the automation concept which relies on three autonomous subsystems and their interaction. Crucial components like a sturdy and reliable solar tracker dome are described in detail. The automation software employs a new approach relying on multiple processes, database logging and web-based remote control. First results of total column measurements at Jena, Germany show that the instrument works well and can provide parts of the diurnal as well as seasonal cycle for CO₂. Instrument line shape measurements with an HCl cell suggest that the instrument stays well-aligned over several months. After a short test campaign for side by side intercomaprison with an existing TCCON instrument in Australia, the system will be transported to its final destination Ascension Island.