FTIR Measurements of Greenhouse Gases over Thessaloniki, Greece in the Framework of COCCON and Comparison with S5P/TROPOMI Observations

In this work, column-averaged dry-air mole fractions of carbon dioxide (XCO2), methane (XCH4) and carbon monoxide (XCO) are presented for the first time at a mid-latitude urban station, Thessaloniki, Greece, using the Bruker EM27/SUN ground-based low-resolution Fourier Transform spectrometer operated according to the requirements of the Collaborative Carbon Column Observing Network (COCCON). Two years of measurements are presented and examined for seasonal variability. The observed XCO2 levels show the expected seasonal cycle (spring maximum, late summer minimum) with a peak-to-peak amplitude of 12 ppm, with maximum values reported for winter 2021 exceeding 416 ppm. The XCH4 values are shown to increase in the second half of the year, with autumn showing the highest mean value of 1.878 ± 0.01 ppm. The XCO levels, following anthropogenic sources, show high winter and low summer values, exhibiting a rise again in August and September with a maximum value of 114 ± 3 ppb and a minimum in summer 2020 of 76 ± 3 ppb. Additionally, methane and carbon monoxide products obtained from the TROPOspheric Monitoring Instrument (TROPOMI), Sentinel-5P space borne sensor, are compared with the ground-based measurements. We report a good agreement between products. The relative mean bias for methane and carbon monoxide are −0.073 ± 0.647% and 3.064 ± 5.566%, respectively. Furthermore, a 15-day running average is subtracted from the original daily mean values to provide ΔXCO2, ΔXCO and ΔXCH4 residuals, so as to identify local sources at a synoptic scale. ΔXCO and ΔXCO2 show the best correlation in the winter (R2 = 0.898, slope = 0.007) season due to anthropogenic emissions in this period of the year (combustion of fossil fuels or industrial activities), while in summer no correlation is found. ΔXCO and ΔXCH4 variations are similar through both years of measurements and have a very good correlation in all seasons including winter (R2 = 0.804, slope = 1.209). The investigation of the X-gases comparison is of primary importance in order to identify local sources and quantify the impact of these trace gases to the deregulation of earth-climate system balance

The added value of satellite observations of methane for understanding the contemporary methane budget

Surface observations have recorded large and incompletely understood changes to atmospheric methane (CH(4)) this century. However, their ability to reveal the responsible surface sources and sinks is limited by their geographical distribution, which is biased towards the northern midlatitudes. Data from Earth-orbiting satellites designed specifically to measure atmospheric CH(4) have been available since 2009 with the launch of the Japanese Greenhouse gases Observing SATellite (GOSAT). We assess the added value of GOSAT to data collected by the US National Oceanic and Atmospheric Administration (NOAA), which have been the lynchpin for knowledge about atmospheric CH(4) since the 1980s. To achieve that we use the GEOS-Chem atmospheric chemistry transport model and an inverse method to infer a posteriori flux estimates from the NOAA and GOSAT data using common a priori emission inventories. We find the main benefit of GOSAT data is from its additional coverage over the tropics where we report large increases since the 2014/2016 El Niño, driven by biomass burning, biogenic emissions and energy production. We use data from the European TROPOspheric Monitoring Instrument to show how better spatial coverage and resolution measurements allow us to quantify previously unattainable diffuse sources of CH(4), thereby opening up a new research frontier. This article is part of a discussion meeting issue ‘Rising methane: is warming feeding warming? (part 1)’

First data set of H<sub>2</sub>O/HDO columns from the Tropospheric Monitoring Instrument (TROPOMI)

Global measurements of atmospheric water vapour isotopologues aid to better understand the hydrological cycle and improve global circulation models. This paper presents a new data set of vertical column densities of H2O and HDO retrieved from short-wave infrared (2.3 µm) reflectance measurements by the Tropospheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor satellite. TROPOMI features daily global coverage with a spatial resolution of up to 7 km×7 km. The retrieval utilises a profile-scaling approach. The forward model neglects scattering, and strict cloud filtering is therefore necessary. For validation, recent ground-based water vapour isotopologue measurements by the Total Carbon Column Observing Network (TCCON) are employed. A comparison of TCCON δD with ground-based measurements by the Multi-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA) project for data prior to 2014 (where MUSICA data are available) shows a bias in TCCON δD estimates. As TCCON HDO is currently not validated, an overall correction of recent TCCON HDO data is derived based on this finding. The agreement between the corrected TCCON measurements and co-located TROPOMI observations is good with an average bias of (−0.2±3)×10$^{21}$ molec cm$^{-2}$ ((1.1±7.2) %) in H$_{2}$O and (−2±7)×10$^{17}$ molec cm$^{-2}$ ((−1.1±7.3) %) in HDO, which corresponds to a mean bias of (−14±17) ‰ in a posteriori δD. The bias is lower at low- and mid-latitude stations and higher at high-latitude stations. The use of the data set is demonstrated with a case study of a blocking anticyclone in northwestern Europe in July 2018 using single-overpass data

Shipborne measurements of XCO2_{2}, XCH4_{4}, and XCO above the Pacific Ocean and comparison to CAMS atmospheric analyses and S5P/TROPOMI

Measurements of atmospheric column-averaged dry-air mole fractions of carbon dioxide (XCO2), methane (XCH4), and carbon monoxide (XCO) have been collected across the Pacific Ocean during the Measuring Ocean REferences 2 (MORE-2) campaign in June 2019. We deployed a shipborne variant of the EM27/SUN Fourier transform spectrometer (FTS) on board the German RN Sonne which, during MORE-2, crossed the Pacific Ocean from Vancouver, Canada, to Singapore. Equipped with a specially manufactured fast solar tracker, the FTS operated in direct-sun viewing geometry during the ship cruise reliably delivering solar absorption spectra in the shortwave infrared spectral range (4000 to 11000 cm(-1)). After filtering and bias correcting the dataset, we report on XCO2, XCH4, and XCO measurements for 22 d along a trajectory that largely aligns with 30 degrees N of latitude between 140 degrees W and 120 degrees E of longitude. The dataset has been scaled to the Total Carbon Column Observing Network (TCCON) station in Karlsruhe, Germany, before and after the MORE-2 campaign through side-by-side measurements. The la repeatability of hourly means of XCO2, XCH4, and XCO is found to be 0.24 ppm, 1.1 ppb, and 0.75 ppb, respectively. The Copernicus Atmosphere Monitoring Service (CAMS) models gridded concentration fields of the atmospheric composition using assimilated satellite observations, which show excellent agreement of 0.52 +/- 0.31 ppm for XCO2, 0.9 +/- 4.1 ppb for XCH4, and 3.2 +/- 3.4 ppb for XCO (mean difference +/- SD, standard deviation, of differences for entire record) with our observations. Likewise, we find excellent agreement to within 2.2 +/- 6.6 ppb with the XCO observations of the TROPOspheric MOnitoring Instrument (TROPOMI) on the Sentinel-5 Precursor satellite (S5P). The shipborne measurements are accessible at https://doi.org/10.1594/PANGAEA.917240 (Knapp et al., 2020)

Intercomparison of arctic XH2_{2}O observations from three ground-based Fourier transform infrared networks and application for satellite validation

In this paper, we compare column-averaged dry-air mole fractions of water vapor (XH$_{2}$O) retrievals from the COllaborative Carbon Column Observing Network (COCCON) with retrievals from two co-located high-resolution Fourier transform infrared (FTIR) spectrometers as references at two boreal sites, Kiruna, Sweden, and Sodankylä, Finland, from 6 March 2017 to 20 September 2019. In the framework of the Network for the Detection of Atmospheric Composition Change (NDACC), an FTIR spectrometer is operated at Kiruna. The H$_{2}$O product derived from these observations has been generated with the MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA) processor. In Sodankylä, a Total Carbon Column Observing Network (TCCON) spectrometer is operated, and the official XH$_{2}$O data as provided by TCCON are used for this study. The datasets are in good overall agreement, with COCCON data showing a wet bias of (49.20±58.61) ppm ((3.33±3.37) %, R$^{2}$=0.9992) compared with MUSICA NDACC and (56.32±45.63) ppm ((3.44±1.77) %, R$^{2}$=0.9997) compared with TCCON. Furthermore, the a priori H$_{2}$O volume mixing ratio (VMR) profiles (MAP) used as a priori information in the TCCON retrievals (also adopted for COCCON retrievals) are evaluated with respect to radiosonde (Vaisala RS41) profiles at Sodankylä. The MAP and radiosonde profiles show similar shapes and a good linear correlation of integrated XH$_{2}$O, indicating that MAP is a reasonable approximation of the true atmospheric state and an appropriate choice for the scaling retrieval methods as applied by COCCON and TCCON. COCCON shows a reduced dry bias (−14.96 %) in comparison with TCCON (−19.08 %) with respect to radiosonde XH$_{2}$O. Finally, we investigate the quality of satellite data at high latitudes. For this purpose, the COCCON XH$_{2}$O is compared with retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) generated with the MUSICA processor (MUSICA IASI) and with retrievals from the TROPOspheric Monitoring Instrument (TROPOMI). Both paired datasets generally show good agreement and similar correlations at the two sites. COCCON measures 4.64 % less XH2O at Kiruna and 3.36 % less at Sodankylä with respect to MUSICA IASI, whereas COCCON measures 9.71 % more XH$_{2}$O at Kiruna and 7.75 % more at Sodankylä compared with TROPOMI. Our study supports the assumption that COCCON also delivers a well-characterized XH$_{2}$O data product. This emphasizes that this approach might complement the TCCON network with respect to satellite validation efforts. This is the first published study where COCCON XH$_{2}$O has been compared with MUSICA NDACC and TCCON retrievals and has been used for MUSICA IASI and TROPOMI validation

Intercomparison of atmospheric CO2 and CH4 abundances on regional scales in boreal areas using Copernicus Atmosphere Monitoring Service (CAMS) analysis, COllaborative Carbon Column Observing Network (COCCON) spectrometers, and Sentinel-5 Precursor satellite observations

We compare the atmospheric column-averaged dry-air mole fractions of carbon dioxide (XCO$_{2}$) and methane (XCH$_{4}$) measured with a pair of COllaborative Carbon Column Observing Network (COCCON) spectrometers at Kiruna and Sodankylä (boreal areas). We compare model data provided by the Copernicus Atmosphere Monitoring Service (CAMS) between 2017 and 2019 with XCH$_{4}$ data from the recently launched Sentinel-5 Precursor (S5P) satellite between 2018 and 2019. In addition, measured and modeled gradients of XCO$_{2}$ and XCH$_{4}$ (ΔXCO$_{2}$ and ΔXCH$_{4}$) on regional scales are investigated. Both sites show a similar and very good correlation between COCCON retrievals and the modeled CAMS XCO$_{2}$ data, while CAMS data are biased high with respect to COCCON by 3.72 ppm (±1.80 ppm) in Kiruna and 3.46 ppm (±1.73 ppm) in Sodankylä on average. For XCH$_{4}$, CAMS values are higher than the COCCON observations by 0.33 ppb (±11.93 ppb) in Kiruna and 7.39 ppb (±10.92 ppb) in Sodankylä. In contrast, the S5P satellite generally measures lower atmospheric XCH$_{4}$ than the COCCON spectrometers, with a mean difference of 9.69 ppb (±20.51 ppb) in Kiruna and 3.36 ppb (±17.05 ppb) in Sodankylä. We compare the gradients of XCO$_{2}$ and XCH$_{4}$ (ΔXCO$_{2}$ and ΔXCH$_{4}$) between Kiruna and Sodankylä derived from CAMS analysis and COCCON and S5P measurements to study the capability of detecting sources and sinks on regional scales. The correlations in ΔXCO$_{2}$ and ΔXCH$_{4}$ between the different datasets are generally smaller than the correlations in XCO$_{2}$ and XCH$_{4}$ between the datasets at either site. The ΔXCO$_{2}$ values predicted by CAMS are generally higher than those observed with COCCON with a slope of 0.51. The ΔXCH$_{4}$ values predicted by CAMS are mostly higher than those observed with COCCON with a slope of 0.65, covering a larger dataset than the comparison between S5P and COCCON. When comparing CAMS ΔXCH$_{4}$ with COCCON ΔXCH$_{4}$ only in S5P overpass days (slope = 0.53), the correlation is close to that between S5P and COCCON (slope = 0.51). CAMS, COCCON, and S5P predict gradients in reasonable agreement. However, the small number of observations coinciding with S5P limits our ability to verify the performance of this spaceborne sensor. We detect no significant impact of ground albedo and viewing zenith angle on the S5P results. Both sites show similar situations with the average ratios of XCH$_{4}$ (S5P/COCCON) of 0.9949±0.0118 in Kiruna and 0.9953±0.0089 in Sodankylä. Overall, the results indicate that the COCCON instruments have the capability of measuring greenhouse gas (GHG) gradients on regional scales, and observations performed with the portable spectrometers can contribute to inferring sources and sinks and to validating spaceborne greenhouse gas sensors. To our knowledge, this is the first published study using COCCON spectrometers for the validation of XCH$_{4}$ measurements collected by S5P