Quantifying CH4_{4} emissions in hard coal mines from TROPOMI and IASI observations using the wind-assigned anomaly method

In this study, we use satellite-based total column-averaged dry-air mole fraction of CH4 (XCH4) from the TROPOspheric Monitoring Instrument (TROPOMI) and tropospheric XCH$_{4}$ (TXCH$_{4}$) from the Infrared Atmospheric Sounding Interferometer (IASI). In addition, the high-resolution model forecasts, XCH$_{4}$ and TXCH$_{4}$, from the Copernicus Atmosphere Monitoring Service (CAMS) are used to estimate the CH$_{4}$ emission rate averaged over 3 years (November 2017–December 2020) in the USCB region (49.3–50.8$^\circ$ N and 18–20$^\circ$ E). The wind-assigned anomaly method is first validated using the CAMS forecast data (XCH$_{4}$ and TXCH$_{4}$), showing a good agreement with the CAMS GLOBal ANThropogenic emission (CAMS-GLOB-ANT) inventory. It indicates that the wind-assigned method works well. This wind-assigned method is further applied to the TROPOMI XCH$_{4}$ and TROPOMI + IASI TXCH$_{4}$ by using the Carbon dioxide and Methane (CoMet) inventory derived for the year 2018. The calculated averaged total CH$_{4}$ emissions over the USCB region is about 496 kt yr$^{-1}$ (5.9×10$^{26}$ molec. s$^{-1}$) for TROPOMI XCH$_{4}$ and 437 kt yr$^{-1}$ (5.2×10$^{26}$ molec. s$^{-1}$) for TROPOMI + IASI TXCH$_{4}$. These values are very close to the ones given in the E-PRTR inventory (448 kt yr$^{-1}$) and the ones in the CoMet inventory (555 kt yr$^{-1}$), and are thus in agreement with these inventories. The similar estimates of XCH$_{4}$ and TXCH$_{4}$ also imply that for a strong source, the dynamically induced variations of the CH$_{4}$ mixing ratio in the upper troposphere and lower stratosphere region are of secondary importance. Uncertainties from different error sources (background removal and noise in the data, vertical wind shear, wind field segmentation, and angle of the emission cone) are approximately 14.8 % for TROPOMI XCH$_{4}$ and 11.4 % for TROPOMI + IASI TXCH$_{4}$. These results suggest that our wind-assigned method is quite robust and might also serve as a simple method to estimate CH$_{4}$ or CO$_{2}$ emissions for other regions

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

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

Estimation of NO2 emission strengths over Riyadh and Madrid from space from a combination of wind-assigned anomalies and machine learning technique

Nitrogen dioxide (NO2) air pollution provides valuable information for quantifying NOx emissions and exposures. This study presents a comprehensive method to estimate average tropospheric NO2 emission strengths derived from three-year (April 2018 – March 2021) TROPOMI observations by combining a wind-assigned anomaly approach and a Machine Learning (ML) method, the so-called Gradient Descent. This combined approach is firstly applied to the Saudi Arabian capital city Riyadh, as a test site, and yields a total emission rate of 1.04×1026 molec./s. The ML-trained anomalies fit very well with the wind-assigned anomalies with an R2 value of 1.0 and a slope of 0.99. Hotspots of NO2 emissions are apparent at several sites where the cement plant and power plants are located and over areas along the highways. Using the same approach, an emission rate of 1.80×1025 molec./s is estimated in the Madrid metropolitan area, Spain. Both the estimate and spatial pattern are comparable to the CAMS inventory.We also acknowledge the project of Joint R&D and Talents Program funded by the Qingdao Sino-German Institute of Intelligent Technologies (kh0100020213319) and the project of Transnational Interoperability Rules and Solution Patterns in Collaborative Production Networks based on IDS and GAIA-X funded by Ministry of Science and Technology, PRC (SQ2021YFE010470)

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 (XCO2) and methane (XCH4) measured with a pair of COllaborative Carbon Column Observing Network (COCCON) spectrometers at Kiruna and Sodankyla (boreal areas). We compare model data provided by the Copernicus Atmosphere Monitoring Service (CAMS) between 2017 and 2019 with XCH4 data from the recently launched Sentinel-5 Precursor (S5P) satellite between 2018 and 2019. In addition, measured and modeled gradients of XCO2 and XCH4 (Delta XCO2 and Delta XCH4) on regional scales are investigated. Both sites show a similar and very good correlation between COCCON retrievals and the modeled CAMS XCO2 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 Sodankyla on average. For XCH4, 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 Sodankyla. In contrast, the S5P satellite generally measures lower atmospheric XCH4 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 So-dankyla. We compare the gradients of XCO2 and XCH4 (Delta XCO2 and Delta XCH4) between Kiruna and Sodankyla derived from CAMS analysis and COCCON and S5P measurements to study the capability of detecting sources and sinks on regional scales. The correlations in Delta XCO2 and Delta XCH4 between the different datasets are generally smaller than the correlations in XCO2 and XCH4 between the datasets at either site. The Delta XCO2 values predicted by CAMS are generally higher than those observed with COCCON with a slope of 0.51. The Delta XCH4 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 Delta XCH4 with COCCON Delta XCH4 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 XCH4 (S5P/COCCON) of 0.9949 +/- 0.0118 in Kiruna and 0.9953 +/- 0.0089 in Sodankyla. 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 XCH4 measurements collected by S5P

Estimation of NO2_{2} emission strengths over Riyadh and Madrid from space from a combination of wind-assigned anomalies and a machine learning technique

Nitrogen dioxide (NO$_{2}$) air pollution provides valuable information for quantifying NOx (NOx = NO +NO$_{2}$) emissions and exposures. This study presents a comprehensive method to estimate average tropospheric NO$_{2}$emission strengths derived from 4-year (May 2018–June 2022) TROPOspheric Monitoring Instrument (TROPOMI) observations by combining a wind-assigned anomaly approach and a machine learning (ML) method, the so-called gradient descent algorithm. This combined approach is firstly applied to the Saudi Arabian capital city of Riyadh, as a test site, and yields a total emission rate of 1.09×1026 molec. s−1. The ML-trained anomalies fit very well with the wind-assigned anomalies, with an R2 value of 1.0 and a slope of 0.99. Hotspots of NO2 emissions are apparent at several sites: over a cement plant and power plants as well as over areas along highways. Using the same approach, an emission rate of 1.99×1025 molec. s−1 is estimated in the Madrid metropolitan area, Spain. Both the estimate and spatial pattern are comparable with the Copernicus Atmosphere Monitoring Service (CAMS) inventory. Weekly variations in NO$_{2}$emission are highly related to anthropogenic activities, such as the transport sector. The NO$_{2}$emissions were reduced by 16 % at weekends in Riyadh, and high reductions were found near the city center and in areas along the highway. An average weekend reduction estimate of 28 % was found in Madrid. The regions with dominant sources are located in the east of Madrid, where residential areas and the Madrid-Barajas airport are located. Additionally, due to the COVID-19 lockdowns, the NO$_{2}$emissions decreased by 21 % in March–June 2020 in Riyadh compared with the same period in 2019. A much higher reduction (62 %) is estimated for Madrid, where a very strict lockdown policy was implemented. The high emission strengths during lockdown only persist in the residential areas, and they cover smaller areas on weekdays compared with weekends. The spatial patterns of NO$_{2}$emission strengths during lockdown are similar to those observed at weekends in both cities. Although our analysis is limited to two cities as test examples, the method has proven to provide reliable and consistent results. It is expected to be suitable for other trace gases and other target regions. However, it might become challenging in some areas with complicated emission sources and topography, and specific NO$_{2}$decay times in different regions and seasons should be taken into account. These impacting factors should be considered in the future model to further reduce the uncertainty budget

Estimation of NO2 emission strengths over Riyadh and Madrid from space from a combination of wind-assigned anomalies and a machine learning technique

Nitrogen dioxide (NO2) air pollution provides valuable information for quantifying NOx (NOx = NO + NO2) emissions and exposures. This study presents a comprehensive method to estimate average tropospheric NO2 emission strengths derived from 4-year (May 2018–June 2022) TROPOspheric Monitoring Instrument (TROPOMI) observations by combining a wind-assigned anomaly approach and a machine learning (ML) method, the so-called gradient descent algorithm. This combined approach is firstly applied to the Saudi Arabian capital city of Riyadh, as a test site, and yields a total emission rate of 1.09×1026 molec. s−1. The ML-trained anomalies fit very well with the wind-assigned anomalies, with an R2 value of 1.0 and a slope of 0.99. Hotspots of NO2 emissions are apparent at several sites: over a cement plant and power plants as well as over areas along highways. Using the same approach, an emission rate of 1.99×1025 molec. s−1 is estimated in the Madrid metropolitan area, Spain. Both the estimate and spatial pattern are comparable with the Copernicus Atmosphere Monitoring Service (CAMS) inventory.We wish to acknowledge the Joint R&D and Talents Program project, funded by the Qingdao Sino-German Institute of Intelligent Technologies (grant no. kh0100020213319); the Deutsche Forschungsgemeinschaft; and the Open Access Publishing Fund of the Karlsruhe Institute of Technology for their support

Quality controls, bias, and seasonality of CO2columns in the boreal forest with Orbiting Carbon Observatory-2, Total Carbon Column Observing Network, and EM27/SUN measurements

Seasonal CO$_{2}$ exchange in the boreal forest plays an important role in the global carbon budget and in driving interannual variability in seasonal cycles of atmospheric CO$_{2}$. Satellite-based observations from polar orbiting satellites like the Orbiting Carbon Observatory-2 (OCO-2) offer an opportunity to characterize boreal forest seasonal cycles across longitudes with a spatially and temporally rich data set, but data quality controls and biases still require vetting at high latitudes. With the objective of improving data availability at northern, terrestrial high latitudes, this study evaluates quality control methods and biases of OCO-2 retrievals of atmospheric column-averaged dry air mole fractions of CO$_{2}$ (X$_{CO2}$) in boreal forest regions. In addition to the standard quality control (QC) filters recommended for the Atmospheric Carbon Observations from Space (ACOS) B8 (B8 QC) and ACOS B9 (B9 QC) OCO-2 retrievals, a third set of quality control filters were specifically tailored to boreal forest observations (boreal QC) with the goal of increasing data availability at high latitudes without sacrificing data quality. Ground-based reference measurements of X$_{CO2}$ include observations from two sites in the Total Carbon Column Observing Network (TCCON) at East Trout Lake, Saskatchewan, Canada, and Sodankylä, Finland. OCO-2 retrievals were also compared to ground-based observations from two Bruker EM27/SUN Fourier transform infrared spectrometers (FTSs) at Fairbanks, Alaska, USA. The EM27/SUN spectrometers that were deployed in Fairbanks were carefully monitored for instrument performance and were bias corrected to TCCON using observations at the Caltech TCCON site. The B9 QC were found to pass approximately twice as many OCO-2 retrievals over land north of 50° N than the B8 QC, and the boreal QC were found to pass approximately twice as many retrievals in May, August, and September as the B9 QC. While boreal QC results in a substantial increase in passable retrievals, this is accompanied by increases in the standard deviations in biases at boreal forest sites from ∼1.4 parts per million (ppm) with B9 QC to ∼1.6 ppm with boreal QC. Total average biases for coincident OCO-2 retrievals at the three sites considered did not consistently increase or decrease with different QC methods, and instead, responses to changes in QC varied according to site and satellite viewing geometries. Regardless of the quality control method used, seasonal variability in biases was observed, and this variability was more pronounced at Sodankylä and East Trout Lake than at Fairbanks. Long-term coincident observations from TCCON, EM27/SUN, and satellites from multiple locations would be necessary to determine whether the reduced seasonal variability in bias at Fairbanks is due to geography or instrumentation. Monthly average biases generally varied between −1 and +1 ppm at the three sites considered, with more negative biases in spring (March, April, and May – MAM) and autumn (September and October – SO) but more positive biases in the summer months (June, July, and August – JJA). Monthly standard deviations in biases ranged from approximately 1.0 to 2.0 ppm and did not exhibit strong seasonal dependence, apart from exceptionally high standard deviation observed with all three QC methods at Sodankylä in June. There was no evidence found to suggest that seasonal variability in bias is a direct result of air mass dependence in ground-based retrievals or of proximity bias from coincidence criteria, but there were a number of retrieval parameters used as quality control filters that exhibit seasonality and could contribute to seasonal dependence in OCO-2 bias. Furthermore, it was found that OCO-2 retrievals of X$_{CO2}$ without the standard OCO-2 bias correction exhibit almost no perceptible seasonal dependence in average monthly bias at these boreal forest sites, suggesting that seasonal variability in bias is introduced by the bias correction. Overall, we found that modified quality controls can allow for significant increases in passable OCO-2 retrievals with only marginal compromises in data quality, but seasonal dependence in biases still warrants further exploration