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 XCO 2 and 0.9 ppbv for XCH 4 , which is within the 1σ precision of the comparison, 0.6 ppmv for XCO 2 and 4.3 ppbv for XCH 4 . The bias between the two data sets is 3.9 ppmv for XCO 2 and 13.0 ppbv for XCH 4 . 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 XCO 2 and 0.2 ppbv for XCH 4 per year, with 1σ precisions of 0.4 ppmv for XCO 2 and 1.4 ppbv for XCH 4 , respectively. The bias between the two data sets is 0.6 ppmv for XCO 2 and 0.5 ppbv for XCH 4 . 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 COC-CON 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 XCO 2 is 0.20 ppmv, while it is 0.8 ppbv for XCH 4 . The average standard deviation of the ensemble is 0.13 ppmv for XCO 2 and 0.6 ppbv for XCH 4 . 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 XCO 2 and 2.2 ppbv for XCH 4 . 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.

Abstract. The portable FTIR (Fourier transform infrared) spectrometer EM27/SUN, dedicated to the precise and accurate observation of column-averaged abundances of methane and carbon dioxide, has been equipped with a second detector channel, which allows the detection of additional species, especially carbon monoxide. This allows an improved characterisation of observed carbon dioxide enhancements and makes the extended spectrometer especially suitable as a validation tool of ESA's Sentinel 5 Precursor mission, as it now covers the same spectral region as used by the infrared channel of the TROPOMI (TROPOspheric Monitoring Instrument) sensor. The extension presented here does not rely on a dichroic, but instead a fraction of the solar beam is decoupled near the aperture stop of the spectrometer using a small plane mirror. This approach allows maintaining the camera-controlled solar tracker set-up, which is referenced to the field stop in front of the primary detector. Moreover, the upgrade of existing instruments can be performed without alterating the optical set-up of the primary channel and resulting changes of the instrumental characteristics of the original instrument.

Abstract. Sulfur dioxide emissions from the Popocatépetl volcano in central Mexico were measured during the MI-LAGRO field campaign in March 2006. A stationary scanning DOAS (Differential Optical Absorption Spectrometer) was used to monitor the SO 2 emissions from the volcano and the results were compared with traverses done with a COSPEC from the ground and a DOAS instrument on board an ultra-light aircraft. Daytime evolutions as well as day-today variation of the SO 2 emissions are reported. A value of 2.45±1.39 Gg/day of SO 2 is reported from all the daily averages obtained during the month of March 2006, with large variation in maximum and minimum daily averages of 5.97 and 0.56 Gg/day, respectively. The large short-term fluctuations in the SO 2 emissions obtained could be confirmed through 2-D visualizations of the SO 2 plume measured with a scanning imaging infrared spectrometer. This instrument, based on the passive detection of thermal radiation from the volcanic gas and analysis with FTIR spectrometry, is used for the first time for plume visualization of a specific volcanic gas. A 48-h forward trajectory analysis indicates that the volcanic plume was predominantly directed towards the Puebla/Tlaxcala region (63%), followed by the Mexico City and Cuernavaca/Cuautla regions with 19 and 18% occurrences, respectively. 25% of the modeled trajectories going towards the Puebla region reached altitudes lower than 4000 m a.s.l. but all trajectories remained over this altitude for the other two regions.

Abstract. In a 3.5 year long study, the long term performance of a mobile Bruker EM27/SUN spectrometer, used for greenhouse gases 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, qualifying it as an useful supplement for the existing TCCON network in remote areas. For achieving consistent performance, such an extension requires careful testing of any spectrometers involved by application of common quality assurance 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 in XCO 2 is 0.20 ppm, while it is 0.8 ppb for XCH 4 . As indicated by the executed long-term study on one device presented here, the remaining empirical calibration factor deduced for 5 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 raw residual bias reported above.

Abstract. The composition and emission rates of volcanic gas plumes provide insight of the geologic internal activity, atmospheric chemistry, aerosol formation and radiative processes around it. Observations are necessary for public security and the aviation industry. Ground-based thermal emission infrared spectroscopy, which uses the radiation of the volcanic gas itself, allows for continuously monitoring during day and night from a safe distance. We present measurements on Popocatépetl volcano based on thermal emission spectroscopy during different campaigns between 2006-2009 using a Scanning Infrared Gas Imaging System (SIGIS). The experimental set-up, measurement geometries and analytical algorithms are described. The equipment was operated from a safe distance of 12 km from the volcano at two different spectral resolutions: 0.5 and 4 cm −1 . The 2-dimensional scanning capability of the instrument allows for an on-line visualization of the volcanic SO 2 plume and its animation. SiF 4 was also identified in the infrared spectra recorded at both resolutions. The SiF 4 /SO 2 molecular ratio can be calculated from each image and used as a highly useful parameter to follow changes in volcanic activity. A small Vulcanian eruption was monitored during the night of 16 to 17 November 2008 and strong ash emission together with a pronounced SO 2 cloud was registered around 01:00 a.m. LST (Local Standard Time). Enhanced SiF 4 /SO 2 ratios were observed before and after the eruption. A validation of the results from thermal emission measurements with those from absorption spectra of the moon taken at the same time, as well as an error analysis, are presented. The inferred propagation speed from sequential images is used in a subsequent paper (Part 2) to calculate the emission rates at different distances from the crater.