In a 3.5-year long study, the long-term performance of a mobile, solar absorption Bruker EM27/SUN spectrometer, used for greenhouse gas observations, is checked with respect to a co-located reference Bruker IFS 125HR spectrometer, which is part of the Total Carbon Column Observing Network (TCCON). We find that the EM27/SUN is stable on timescales of several years; the drift per year between the EM27/SUN and the official TCCON product is 0.02 ppmv for XCO₂ and 0.9 ppbv for XCH₄, which is within the 1σ precision of the comparison, 0.6 ppmv for XCO₂ and 4.3 ppbv for XCH₄. The bias between the two data sets is 3.9 ppmv for XCO₂ and 13.0 ppbv for XCH₄. In order to avoid sensitivity-dependent artifacts, the EM27/SUN is also compared to a truncated IFS 125HR data set derived from full-resolution TCCON interferograms. The drift is 0.02 ppmv for XCO₂ and 0.2 ppbv for XCH₄ per year, with 1σ precisions of 0.4 ppmv for XCO₂ and 1.4 ppbv for XCH₄, respectively. The bias between the two data sets is 0.6 ppmv for XCO₂ and 0.5 ppbv for XCH₄. With the presented long-term stability, the EM27/SUN qualifies as an useful supplement to the existing TCCON network in remote areas. To achieve consistent performance, such an extension requires careful testing of any spectrometers involved by application of common quality assurance measures. One major aim of the COllaborative Carbon Column Observing Network (COCCON) infrastructure is to provide these services to all EM27/SUN operators. In the framework of COCCON development, the performance of an ensemble of 30 EM27/SUN spectrometers was tested and found to be very uniform, enhanced by the centralized inspection performed at the Karlsruhe Institute of Technology prior to deployment. Taking into account measured instrumental line shape parameters for each spectrometer, the resulting average bias across the ensemble with respect to the reference EM27/SUN used in the long-term study in XCO₂ is 0.20 ppmv, while it is 0.8 ppbv for XCH₄. The average standard deviation of the ensemble is 0.13 ppmv for XCO₂ and 0.6 ppbv for XCH₄. In addition to the robust metric based on absolute differences, we calculate the standard deviation among the empirical calibration factors. The resulting 2σ uncertainty is 0.6 ppmv for XCO₂ and 2.2 ppbv for XCH₄. As indicated by the executed long-term study on one device presented here, the remaining empirical calibration factor deduced for each individual instrument can be assumed constant over time. Therefore the application of these empirical factors is expected to further improve the EM27/SUN network conformity beyond the scatter among the empirical calibration factors reported above.

We demonstrate the use of compact solar-tracking Fourier transform spectrometers (Bruker EM27/SUN) for differential measurements of the column-averaged dry-air mole fractions of CH₄ and CO₂ within urban areas. Using Allan variance analysis, we show that the differential column measurement has a precision of 0.01 % for X_CO2 and X_CH4 with an optimum integration time of 10 min, corresponding to Allan deviations of 0.04 ppm and 0.2 ppb, respectively. The sensor system is very stable over time and after relocation across the continent. We report tests of the differential column measurement, and its sensitivity to emission sources, by measuring the downwind-minus-upwind column difference ΔX_CH4 across dairy farms in the Chino area, California, and using the data to verify emissions reported in the literature. Ratios of spatial column differences ΔX_CH4∕ΔX_CO2 were observed across Pasadena within the Los Angeles basin, indicating values consistent with regional emission ratios from the literature. Our precise, rapid measurements allow us to determine significant short-term variations (5–10 min) of X_CO2 and X_CH4 and to show that they represent atmospheric phenomena. Overall, this study helps establish a range of new applications for compact solar-viewing Fourier transform spectrometers. By accurately measuring the small differences in integrated column amounts across local and regional sources, we directly observe the mass loading of the atmosphere due to the influence of emissions in the intervening locale. The inference of the source strength is much more direct than inversion modeling using only surface concentrations and less subject to errors associated with small-scale transport phenomena.

Methane (CH₄) emissions from coal production amount to roughly one-third of European anthropogenic CH₄ emissions in the atmosphere. Poland is the largest hard coal producer in the European Union with the Polish side of the Upper Silesian Coal Basin (USCB) as the main part of it. Emission estimates for CH₄ from the USCB for individual coal mine ventilation shafts range between 0.03 and 20 kt a⁻¹, amounting to a basin total of roughly 440 kt a⁻¹ according to the European Pollutant Release and Transfer Register (E-PRTR, http://prtr.ec.europa.eu/, 2014). We mounted a ground-based, portable, sun-viewing FTS (Fourier transform spectrometer) on a truck for sampling coal mine ventilation plumes by driving cross-sectional stop-and-go patterns at 1 to 3 km from the exhaust shafts. Several of these transects allowed for estimation of CH₄ emissions based on the observed enhancements of the column-averaged dry-air mole fractions of methane (XCH₄) using a mass balance approach. Our resulting emission estimates range from 6±1 kt a⁻¹ for a single shaft up to 109±33 kt a⁻¹ for a subregion of the USCB, which is in broad agreement with the E-PRTR reports. Three wind lidars were deployed in the larger USCB region providing ancillary information about spatial and temporal variability of wind and turbulence in the atmospheric boundary layer. Sensitivity studies show that, despite drawing from the three wind lidars, the uncertainty of the local wind dominates the uncertainty of the emission estimates, by far exceeding errors related to the XCH₄ measurements themselves. Wind-related relative errors on the emission estimates typically amount to 20 %.

In order to mitigate climate change, it is crucial to understand urban greenhouse gas (GHG) emissions precisely, as more than two-thirds of the anthropogenic GHG emissions worldwide originate from cities. Nowadays, urban emission estimates are mainly based on bottom-up calculation approaches with high uncertainties. A reliable and long-term top-down measurement approach could reduce the uncertainty of these emission inventories significantly. We present the Munich Urban Carbon Column network (MUCCnet), the world's first urban sensor network, which has been permanently measuring GHGs, based on the principle of differential column measurements (DCMs), since summer 2019. These column measurements and column concentration differences are relatively insensitive to vertical redistribution of tracer masses and surface fluxes upwind of the city, making them a favorable input for an inversion framework and, therefore, a well-suited candidate for the quantification of GHG emissions. However, setting up such a stationary sensor network requires an automated measurement principle. We developed our own fully automated enclosure systems for measuring column-averaged CO₂, CH₄ and CO concentrations with a solar-tracking Fourier transform spectrometer (EM27/SUN) in a fully automated and long-term manner. This also includes software that starts and stops the measurements autonomously and can be used independently from the enclosure system. Furthermore, we demonstrate the novel applications of such a sensor network by presenting the measurement results of our five sensor systems that are deployed in and around Munich. These results include the seasonal cycle of CO₂ since 2015, as well as concentration gradients between sites upwind and downwind of the city. Thanks to the automation, we were also able to continue taking measurements during the COVID-19 lockdown in spring 2020. By correlating the CO₂ column concentration gradients to the traffic amount, we demonstrate that our network is capable of detecting variations in urban emissions. The measurements from our unique sensor network will be combined with an inverse modeling framework that we are currently developing in order to monitor urban GHG emissions over years, identify unknown emission sources and assess how effective the current mitigation strategies are. In summary, our achievements in automating column measurements of GHGs will allow researchers all over the world to establish this approach for long-term greenhouse gas monitoring in urban areas.

In this study, an extension on the previously reported status of the COllaborative Carbon Column Observing Network's (COCCON) calibration procedures incorporating refined methods is presented. COCCON is a global network of portable Bruker EM27/SUN FTIR spectrometers for deriving column-averaged atmospheric abundances of greenhouse gases. The original laboratory open-path lamp measurements for deriving the instrumental line shape (ILS) of the spectrometer from water vapour lines have been refined and extended to the secondary detector channel incorporated in the EM27/SUN spectrometer for detection of carbon monoxide (CO). The refinements encompass improved spectroscopic line lists for the relevant water lines and a revision of the laboratory pressure measurements used for the analysis of the spectra. The new results are found to be in good agreement with those reported by Frey et al. (2019) and discussed in detail. In addition, a new calibration cell for ILS measurements was designed, constructed and put into service. Spectrometers calibrated since January 2020 were tested using both methods for ILS characterization, open-path (OP) and cell measurements. We demonstrate that both methods can detect the small variations in ILS characteristics between different spectrometers, but the results of the cell method indicate a systematic bias of the OP method. Finally, a revision and extension of the COCCON network instrument-to-instrument calibration factors for XCO₂, XCO and XCH₄ is presented, incorporating 47 new spectrometers (of 83 in total by now). This calibration is based on the reference EM27/SUN spectrometer operated by the Karlsruhe Institute of Technology (KIT) and spectra collected by the collocated TCCON station Karlsruhe. Variations in the instrumental characteristics of the reference EM27/SUN from 2014 to 2017 were detected, probably arising from realignment and the dual-channel upgrade performed in early 2018. These variations are considered in the evaluation of the instrument-specific calibration factors in order to keep all tabulated calibration results consistent.