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Methane (CH4) is an important anthropogenic greenhouse gas, and its rising concentration in the atmosphere contributes significantly to global warming. A comparatively small number of highly emitting persistent methane sources are responsible for a large share of global methane emissions. The identification and quantification of these sources, which often show large uncertainties regarding their emissions or locations, are important to support mitigating climate change. Daily global column-averaged dry air mole fractions of atmospheric methane (XCH4) are retrieved from radiance measurements of the TROPOspheric Monitoring Instrument (TROPOMI) on board on the Sentinel-5 Precursor (S5P) satellite with a moderately high spatial resolution, enabling the detection and quantification of localized methane sources. We developed a fully automated algorithm to detect regions with persistent methane enhancement and to quantify their emissions using a monthly TROPOMI XCH4 dataset from the years 2018–2021. We detect 217 potential persistent source regions (PPSRs), which account for approximately 20 % of the total bottom-up emissions. By comparing the PPSRs in a spatial analysis with anthropogenic and natural emission databases, we conclude that 7.8 % of the detected source regions are dominated by coal, 7.8 % by oil and gas, 30.4 % by other anthropogenic sources like landfills or agriculture, 7.3 % by wetlands, and 46.5 % by unknown sources. Many of the identified PPSRs are in well-known source regions, like the Permian Basin in the USA, which is a large production area for oil and gas; the Bowen Basin coal mining area in Australia; or the Pantanal Wetlands in Brazil. We perform a detailed analysis of the PPSRs with the 10 highest emission estimates, including the Sudd Wetland in South Sudan, an oil- and gas-dominated area on the west coast in Turkmenistan, and one of the largest coal production areas in the world, the Kuznetsk Basin in Russia. The calculated emission estimates of these source regions are in agreement within the uncertainties in results from other studies but are in most of the cases higher than the emissions reported by emission databases. We demonstrate that our algorithm is able to automatically detect and quantify persistent localized methane sources of different source type and shape, including larger-scale enhancements such as wetlands or extensive oil- and gas-production basins.

Global crude steel production is expected to continue to increase in the coming decades to meet the demands of the growing world population. Currently, the dominant steelmaking technology worldwide is the conventional highly CO2-intensive blast furnace–basic oxygen furnace production route (also known as the Linz–Donawitz process), which uses iron ore as raw material and coke as a reducing agent. As a result, large quantities of special gases that are rich in carbon monoxide (CO) are by-products of the various stages of the steelmaking process. Given the challenges associated with satellite-based estimates of carbon dioxide (CO2) emissions at the scale of emitting installations due to significant background levels, co-emitted CO may serve as a valuable indicator of the carbon footprint of steel plants. We show that regional CO release from steel production sites can be monitored from space using 5 years of measurements (2018–2022) from the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor satellite, benefiting from its relatively high spatial resolution and daily global coverage. We analyse all German steel plants with blast furnaces and basic oxygen furnaces and obtain associated CO emissions in the range of 50–400 kt yr−1 per site. A comparison with the respective CO2 emissions on the level of emitting installations available from emissions trading data of the European Union Emissions Trading System yields a linear relationship with a sector-specific CO/CO2 emission ratio for the analysed steelworks of 3.24 % [2.73–3.89; 1σ], suggesting the feasibility of using CO as a proxy for CO2 emissions from comparable steel production sites. An evaluation at other steel production sites indicates that the derived CO/CO2 emission ratio is also representative of other highly optimised state-of-the-art Linz–Donawitz steelworks outside Germany and that the emission ratio is potentially valuable for estimating sector-specific CO2 emissions from remotely sensed CO emissions, provided that the underlying CO emission estimate is not affected by other sources.

The Tropospheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor (S5P) satellite is part of the latest generation of trace gas monitoring satellites and provides a new level of spatio-temporal information with daily global coverage, which enables the calculation of daily globally averaged CH4 concentrations. To investigate changes in atmospheric methane, the background CH4 level (i.e. the CH4 concentration without seasonal and short-term variations) has to be determined. CH4 growth rates vary in a complex manner and high-latitude zonal averages may have gaps in the time series, and thus simple fitting methods do not produce reliable results. In this paper we present an approach based on fitting an ensemble of dynamic linear models (DLMs) to TROPOMI data, from which the best model is chosen with the help of cross-validation to prevent overfitting. This method is computationally fast and is not dependent on additional inputs, allowing for fast and continuous analysis of the most recent time series data. We present results of global annual methane increases (AMIs) for the first 4.5 years of S5P/TROPOMI data, which show good agreement with AMIs from other sources. Additionally, we investigated what information can be derived from zonal bands. Due to the fast meridional mixing within hemispheres, we use zonal growth rates instead of AMIs, since they provide a higher temporal resolution. Clear differences can be observed between Northern Hemisphere and Southern Hemisphere growth rates, especially during 2019 and 2022. The growth rates show similar patterns within the hemispheres and show no short-term variations during the years, indicating that air masses within a hemisphere are well-mixed during a year. Additionally, the growth rates derived from S5P/TROPOMI data are largely consistent with growth rates derived from Copernicus Atmospheric Monitoring Service (CAMS) global-inversion-optimized (CAMS/INV) data, which use surface observations. In 2019 a reduction in growth rates can be observed for the Southern Hemisphere, while growth rates in the Northern Hemisphere stay stable or increase. During 2020 a strong increase in Southern Hemisphere growth rates can be observed, which is in accordance with recently reported increases in Southern Hemisphere wetland emissions. In 2022 the reduction in the global AMI can be attributed to decreased growth rates in the Northern Hemisphere, while growth rates in the Southern Hemisphere remain high. Investigations of fluxes from CAMS/INV data support these observations and suggest that the Northern Hemisphere decrease is mainly due to the decrease in anthropogenic fluxes, while in the Southern Hemisphere, wetland fluxes continued to rise. While the continued increase in Southern Hemisphere wetland fluxes agrees with existing studies about the causes of observed methane trends, the difference between Northern Hemisphere and Southern Hemisphere methane increases in 2022 has not been discussed before and calls for further research.

Several ambient air quality records corroborate the severe and persistent degradation of air quality over northern India during the winter months, with evidence of a continued, increasing trend of pollution across the Indo-Gangetic Plain (IGP) over the past decade. A combination of atmospheric dynamics and uncertain emissions, including the post-monsoon agricultural stubble burning, make it challenging to resolve the role of each individual factor. Here we demonstrate the potential use of an atmospheric transport model, the Weather Research and Forecasting model coupled with chemistry (WRF–Chem) to identify and quantify the role of transport mechanisms and emissions on the occurrence of the pollution events. The investigation is based on the use of carbon monoxide (CO) observations from the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor satellite and the surface measurement network, as well as the WRF–Chem simulations, to investigate the factors contributing to CO enhancement over India during November 2018. We show that the simulated column-averaged dry air mole fraction (XCO) is largely consistent with TROPOMI observations, with a spatial correlation coefficient of 0.87. The surface-level CO concentrations show larger sensitivities to boundary layer dynamics, wind speed, and diverging source regions, leading to a complex concentration pattern and reducing the observation-model agreement with a correlation coefficient ranging from 0.41 to 0.60 for measurement locations across the IGP. We find that daily satellite observations can provide a first-order inference of the CO transport pathways during the enhanced burning period, and this transport pattern is reproduced well in the model. By using the observations and employing the model at a comparable resolution, we confirm the significant role of atmospheric dynamics and residential, industrial, and commercial emissions in the production of the exorbitant level of air pollutants in northern India. We find that biomass burning plays only a minimal role in both column and surface enhancements of CO, except for the state of Punjab during the high pollution episodes. While the model reproduces observations reasonably well, a better understanding of the factors controlling the model uncertainties is essential for relating the observed concentrations to the underlying emissions. Overall, our study emphasizes the importance of undertaking rigorous policy measures, mainly focusing on reducing residential, commercial, and industrial emissions in addition to actions already underway in the agricultural sectors.

The switch from the use of coal to natural gas or oil for energy generation potentially reduces greenhouse gas emissions and thus the impact on global warming and climate change because of the higher energy creation per CO2 molecule emitted. However, the climate benefit over coal is offset by methane (CH4) leakage from natural gas and petroleum systems, which reverses the climate impact mitigation if the rate of fugitive emissions exceeds the compensation point at which the global warming resulting from the leakage and the benefit from the reduction of coal combustion coincide. Consequently, an accurate quantification of CH4 emissions from the oil and gas industry is essential to evaluate the suitability of natural gas and petroleum as bridging fuels on the way to a carbon-neutral future. We show that regional CH4 release from large oil and gas fields can be monitored from space by using dense daily recurrent measurements of the TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor satellite to quantify emissions and leakage rates. The average emissions for the time period 2018/2019 from the five most productive basins in the United States, the Permian, Appalachian, Eagle Ford, Bakken, and Anadarko, are estimated to be 3.18±1.13, 2.36±0.88, 1.37±0.63, 0.89±0.56, and 2.74±0.74 Mt yr−1, respectively. This corresponds to CH4 leakage rates relative to the associated production between 1.2 % and 1.4 % for the first four production regions, which are consistent with bottom-up estimates and likely fall below the break-even leakage rate for immediate climate benefit. For the Anadarko Basin, the fugitive emission rate is larger and amounts to 3.9±1.1 %, which likely exceeds the break-even rate for immediate benefit and roughly corresponds to the break-even rate for a 20-year time horizon. The determined values are smaller than previously derived satellite-based leakage rates for the time period 2009–2011, which was an early phase of hydraulic fracturing, indicating that it is possible to improve the climate footprint of the oil and gas industry by adopting new technologies and that efforts to reduce methane emissions have been successful. For two of the world's largest natural gas fields, Galkynysh and Dauletabad in Turkmenistan, we find collective methane emissions of 3.26±1.17 Mt yr−1, which corresponds to a leakage rate of 4.1±1.5 %, suggesting that the Turkmen energy industry is not employing methane emission avoidance strategies and technologies as successfully as those currently widely used in the United States. The leakage rates in Turkmenistan and in the Anadarko Basin indicate that there is potential to reduce fugitive methane emissions from natural gas and petroleum systems worldwide. In particular, relatively newly developed oil and gas plays appear to have larger leakage rates compared to more mature production areas.

Due to proceeding climate change, some regions such as California face rising weather extremes with dry periods becoming warmer and drier, entailing the risk that wildfires and associated air pollution episodes will continue to increase. November 2018 turned into one of the most severe wildfire episodes on record in California, with two particularly destructive wildfires spreading concurrently through the north and the south of the state. Both fires ignited at the wildland–urban interface, causing many civilian fatalities and forcing the total evacuation of several cities and communities. Here we demonstrate that the inherent carbon monoxide (CO) emissions of the wildfires and subsequent transport can be observed from space by analysing radiance measurements of the TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor satellite in the shortwave infrared spectral range. From the determined CO distribution we assess the corresponding air quality burden in major Californian cities caused by the fires and discuss the associated uncertainties. As a result of the prevailing wind conditions, the largest CO load during the first days of the fires is found in Sacramento and San Francisco, with city area averages reaching boundary layer concentration anomalies of about 2.5 mg CO m−3. Even the most polluted city scenes likely comply with the national ambient air quality standards (10 mg CO m−3 with 8 h averaging time). This finding based on dense daily recurrent satellite monitoring is consistent with isolated ground-based air quality measurements.

Glyoxal (CHOCHO) and formaldehyde (HCHO) are intermediate products in the tropospheric oxidation of the majority of volatile organic compounds (VOCs). CHOCHO is also a precursor of secondary organic aerosol (SOA) in the atmosphere. CHOCHO and HCHO are released from biogenic, anthropogenic, and pyrogenic sources. CHOCHO and HCHO tropospheric lifetimes are typically considered to be short during the daytime at mid-latitudes (e.g. several hours), as they are rapidly removed from the atmosphere by their photolysis, oxidation by OH, and uptake on particles or deposition. At night and at high latitudes, tropospheric lifetimes increase to many hours or even days. Previous studies demonstrated that CHOCHO and HCHO vertical column densities (VCDs) are well retrieved from space-borne observations using differential optical absorption spectroscopy (DOAS). In this study, we present CHOCHO and HCHO VCDs retrieved from measurements by TROPOMI (TROPOspheric Monitoring Instrument), launched on the Sentinel-5 Precursor (S5P) platform in October 2017. We observe strongly elevated amounts of CHOCHO and HCHO during the 2018 fire season in British Columbia, Canada, where a large number of fires occurred in August. CHOCHO and HCHO plumes from individual fire hot spots are observed in air masses travelling over distances of up to 1500 km, i.e. much longer than expected for the relatively short tropospheric lifetime expected for CHOCHO and HCHO. Comparison with simulations by the particle dispersion model FLEXPART (FLEXible PARTicle dispersion model) indicates that effective lifetimes of 20 h and more are needed to explain the observations of CHOCHO and HCHO if they decay in an effective first-order process. FLEXPART used in the study calculates accurately the transport. In addition an exponential decay, in our case assumed to be photochemical, of a species along the trajectory is added. We have used this simple approach to test our assumption that CHOCHO and HCHO are created in the fires and then decay at a constant rate in the plume as it is transported. This is clearly not the case and we infer that CHOCHO and HCHO are either efficiently recycled during transport or continuously formed from the oxidation of longer-lived precursors present in the plume, or possibly a mixture of both. We consider the best explanation of the observed CHOCHO and HCHO VCD in the plumes of the fire is that they are produced by oxidation of longer-lived precursors, which were also released by the fire and present in the plume.

Despite its key role in climate change, large uncertainties persist in our knowledge of the anthropogenic emissions of carbon dioxide (CO2) and no global observing system exists that allows us to monitor emissions from localized CO2 sources with sufficient accuracy. The Orbiting Carbon Observatory-2 (OCO-2) satellite allows retrievals of the column-average dry-air mole fractions of CO2 (XCO2). However, regional column-average enhancements of individual point sources are usually small, compared to the background concentration and its natural variability, and often not much larger than the satellite's measurement noise. This makes the unambiguous identification and quantification of anthropogenic emission plume signals challenging. NO2 is co-emitted with CO2 when fossil fuels are combusted at high temperatures. It has a short lifetime on the order of hours so that NO2 columns often greatly exceed background and noise levels of modern satellite sensors near sources, which makes it a suitable tracer of recently emitted CO2. Based on six case studies (Moscow, Russia; Lipetsk, Russia; Baghdad, Iraq; Medupi and Matimba power plants, South Africa; Australian wildfires; and Nanjing, China), we demonstrate the usefulness of simultaneous satellite observations of NO2 and XCO2. For this purpose, we analyze co-located regional enhancements of XCO2 observed by OCO-2 and NO2 from the Sentinel-5 Precursor (S5P) satellite and estimate the CO2 plume's cross-sectional fluxes. We take advantage of the nearly simultaneous NO2 measurements with S5P's wide swath and small measurement noise by identifying the source of the observed XCO2 enhancements, excluding interference with remote upwind sources, allowing us to adjust the wind direction, and by constraining the shape of the CO2 plumes. We compare the inferred cross-sectional fluxes with the Emissions Database for Global Atmospheric Research (EDGAR), the Open-Data Inventory for Anthropogenic Carbon dioxide (ODIAC), and, in the case of the Australian wildfires, with the Global Fire Emissions Database (GFED). The inferred cross-sectional fluxes range from 31 MtCO2 a−1 to 153 MtCO2 a−1 with uncertainties (1σ) between 23 % and 72 %. For the majority of analyzed emission sources, the estimated cross-sectional fluxes agree, within their uncertainty, with either EDGAR or ODIAC or lie somewhere between them. We assess the contribution of multiple sources of uncertainty and find that the dominating contributions are related to the computation of the effective wind speed normal to the plume's cross section. The flux uncertainties are expected to be reduced by the planned European Copernicus anthropogenic CO2 monitoring mission (CO2M), which will provide not only precise measurements with high spatial resolution but also imaging capabilities with a wider swath of simultaneous XCO2 and NO2 observations. Such a mission, particularly if performed by a constellation of satellites, will deliver CO2 emission estimates from localized sources at an unprecedented frequency and level of accuracy.

The growth rate of atmospheric carbon dioxide (CO2) reflects the net effect of emissions and uptake resulting from anthropogenic and natural carbon sources and sinks. Annual mean CO2 growth rates have been determined from satellite retrievals of column-averaged dry-air mole fractions of CO2, i.e. XCO2, for the years 2003 to 2016. The XCO2 growth rates agree with National Oceanic and Atmospheric Administration (NOAA) growth rates from CO2 surface observations within the uncertainty of the satellite-derived growth rates (mean difference ± standard deviation: 0.0±0.3 ppm year−1; R: 0.82). This new and independent data set confirms record-large growth rates of around 3 ppm year−1 in 2015 and 2016, which are attributed to the 2015–2016 El Niño. Based on a comparison of the satellite-derived growth rates with human CO2 emissions from fossil fuel combustion and with El Niño Southern Oscillation (ENSO) indices, we estimate by how much the impact of ENSO dominates the impact of fossil-fuel-burning-related emissions in explaining the variance of the atmospheric CO2 growth rate. Our analysis shows that the ENSO impact on CO2 growth rate variations dominates that of human emissions throughout the period 2003–2016 but in particular during the period 2010–2016 due to strong La Niña and El Niño events. Using the derived growth rates and their uncertainties, we estimate the probability that the impact of ENSO on the variability is larger than the impact of human emissions to be 63 % for the time period 2003–2016. If the time period is restricted to 2010–2016, this probability increases to 94 %.

Methane is an important atmospheric greenhouse gas and an adequate understanding of its emission sources is needed for climate change assessments, predictions, and the development and verification of emission mitigation strategies. Satellite retrievals of near-surface-sensitive column-averaged dry-air mole fractions of atmospheric methane, i.e. XCH4, can be used to quantify methane emissions. Maps of time-averaged satellite-derived XCH4 show regionally elevated methane over several methane source regions. In order to obtain methane emissions of these source regions we use a simple and fast data-driven method to estimate annual methane emissions and corresponding 1σ uncertainties directly from maps of annually averaged satellite XCH4. From theoretical considerations we expect that our method tends to underestimate emissions. When applying our method to high-resolution atmospheric methane simulations, we typically find agreement within the uncertainty range of our method (often 100 %) but also find that our method tends to underestimate emissions by typically about 40 %. To what extent these findings are model dependent needs to be assessed. We apply our method to an ensemble of satellite XCH4 data products consisting of two products from SCIAMACHY/ENVISAT and two products from TANSO-FTS/GOSAT covering the time period 2003–2014. We obtain annual emissions of four source areas: Four Corners in the south-western USA, the southern part of Central Valley, California, Azerbaijan, and Turkmenistan. We find that our estimated emissions are in good agreement with independently derived estimates for Four Corners and Azerbaijan. For the Central Valley and Turkmenistan our estimated annual emissions are higher compared to the EDGAR v4.2 anthropogenic emission inventory. For Turkmenistan we find on average about 50 % higher emissions with our annual emission uncertainty estimates overlapping with the EDGAR emissions. For the region around Bakersfield in the Central Valley we find a factor of 5–8 higher emissions compared to EDGAR, albeit with large uncertainty. Major methane emission sources in this region are oil/gas and livestock. Our findings corroborate recently published studies based on aircraft and satellite measurements and new bottom-up estimates reporting significantly underestimated methane emissions of oil/gas and/or livestock in this area in EDGAR.

Wetlands are a major emission source of methane (CH4) globally. In this study, we evaluate wetland emission estimates derived using the UK community land surface model (JULES, the Joint UK Land Earth Simulator) against atmospheric observations of methane, including, for the first time, total methane columns derived from the SCIAMACHY instrument on board the ENVISAT satellite. Two JULES wetland emission estimates are investigated: (a) from an offline run driven with Climatic Research Unit–National Centers for Environmental Prediction (CRU-NCEP) meteorological data and (b) from the same offline run in which the modelled wetland fractions are replaced with those derived from the Global Inundation Extent from Multi-Satellites (GIEMS) remote sensing product. The mean annual emission assumed for each inventory (181 Tg CH4 per annum over the period 1999–2007) is in line with other recently published estimates. There are regional differences as the unconstrained JULES inventory gives significantly higher emissions in the Amazon (by ~36 Tg CH4 yr−1) and lower emissions in other regions (by up to 10 Tg CH4 yr−1) compared to the JULES estimates constrained with the GIEMS product. Using the UK Hadley Centre's Earth System model with atmospheric chemistry (HadGEM2), we evaluate these JULES wetland emissions against atmospheric observations of methane. We obtain improved agreement with the surface concentration measurements, especially at high northern latitudes, compared to previous HadGEM2 runs using the wetland emission data set of Fung et al. (1991). Although the modelled monthly atmospheric methane columns reproduce the large-scale patterns in the SCIAMACHY observations, they are biased low by 50 part per billion by volume (ppb). Replacing the HadGEM2 modelled concentrations above 300 hPa with HALOE–ACE assimilated TOMCAT output results in a significantly better agreement with the SCIAMACHY observations. The use of the GIEMS product to constrain the JULES-derived wetland fraction improves the representation of the wetland emissions in JULES and gives a good description of the seasonality observed at surface sites influenced by wetlands, especially at high latitudes. We find that the annual cycles observed in the SCIAMACHY measurements and at many of the surface sites influenced by non-wetland sources cannot be reproduced in these HadGEM2 runs. This suggests that the emissions over certain regions (e.g. India and China) are possibly too high and/or the monthly emission patterns for specific sectors are incorrect. The comparisons presented in this paper show that the performance of the JULES wetland scheme is comparable to that of other process-based land surface models. We identify areas for improvement in this and the atmospheric chemistry components of the HadGEM Earth System model. The Earth Observation data sets used here will be of continued value in future evaluations of JULES and the HadGEM family of models.

Current knowledge about the European terrestrial biospheric carbon sink, from the Atlantic to the Urals, relies upon bottom-up inventory and surface flux inverse model estimates (e.g. 0.27±0.16 GtC a−1 for 2000–2005 (Schulze et al., 2009), 0.17±0.44 GtC a−1 for 2001–2007 (Peters et al., 2010), 0.45±0.40 GtC a−1 for 2010 (Chevallier et al., 2014), 0.40±0.42 GtC a−1 for 2001–2004 (Peylin et al., 2013)). Inverse models assimilate in situ CO2 atmospheric concentrations measured by surface-based air sampling networks. The intrinsic sparseness of these networks is one reason for the relatively large flux uncertainties (Peters et al., 2010; Bruhwiler et al., 2011). Satellite-based CO2 measurements have the potential to reduce these uncertainties (Miller et al., 2007; Chevallier et al., 2007). Global inversion experiments using independent models and independent GOSAT satellite data products consistently derived a considerably larger European sink (1.0–1.3 GtC a−1 for 09/2009–08/2010 (Basu et al., 2013), 1.2–1.8 GtC a−1 in 2010 (Chevallier et al., 2014)). However, these results have been considered unrealistic due to potential retrieval biases and/or transport errors (Chevallier et al., 2014) or have not been discussed at all (Basu et al., 2013; Takagi et al., 2014). Our analysis comprises a regional inversion approach using STILT (Gerbig et al., 2003; Lin et al., 2003) short-range (days) particle dispersion modelling, rendering it insensitive to large-scale retrieval biases and less sensitive to long-range transport errors. We show that the satellite-derived European terrestrial carbon sink is indeed much larger (1.02±0.30 GtC a−1 in 2010) than previously expected. This is qualitatively consistent among an ensemble of five different inversion set-ups and five independent satellite retrievals (BESD (Reuter et al., 2011) 2003–2010, ACOS (O’Dell et al., 2012) 2010, UoL-FP (Cogan et al., 2012) 2010, RemoTeC (Butz et al., 2011) 2010, and NIES (Yoshida et al., 2013) 2010) using data from two different instruments (SCIAMACHY (Bovensmann et al., 1999) and GOSAT (Kuze et al., 2009)). The difference to in situ based inversions (Peylin et al., 2013), whilst large with respect to the mean reported European carbon sink (0.4 GtC a−1 for 2001–2004), is similar in magnitude to the reported uncertainty (0.42 GtC a−1). The highest gain in information is obtained during the growing season when satellite observation conditions are advantageous, a priori uncertainties are largest, and the surface sink maximises; during the dormant season, the results are dominated by the a priori. Our results provide evidence that the current understanding of the European carbon sink has to be revisited.

The terrestrial biosphere is currently acting as a net carbon sink on the global scale, exhibiting significant interannual variability in strength. To reliably predict the future strength of the land sink and its role in atmospheric CO2 growth, the underlying biogeochemical processes and their response to a changing climate need to be well understood. In particular, better knowledge of the impact of key climate variables such as temperature or precipitation on the biospheric carbon reservoir is essential. It is demonstrated using nearly a decade of SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) nadir measurements that years with higher temperatures during the growing season can be robustly associated with larger growth rates in atmospheric CO2 and smaller seasonal cycle amplitudes for northern mid-latitudes. We find linear relationships between warming and CO2 growth as well as seasonal cycle amplitude at the 98% significance level. This suggests that the terrestrial carbon sink is less efficient at higher temperatures during the analysed time period. Unless the biosphere has the ability to adapt its carbon storage under warming conditions in the longer term, such a temperature response entails the risk of potential future sink saturation via a positive carbon-climate feedback. Quantitatively, the covariation between the annual CO2 growth rates derived from SCIAMACHY data and warm season surface temperature anomaly amounts to 1.25 ± 0.32 ppm yr−1 K−1 for the Northern Hemisphere, where the bulk of the terrestrial carbon sink is located. In comparison, this relationship is less pronounced in the Southern Hemisphere. The covariation of the seasonal cycle amplitudes retrieved from satellite measurements and temperature anomaly is −1.30 ± 0.31 ppm K−1 for the north temperate zone. These estimates are consistent with those from the CarbonTracker data assimilated CO2 data product, indicating that the temperature dependence of the model surface fluxes is realistic.

Urban areas, which are home to the majority of today's world population, are responsible for more than two-thirds of the global energy-related carbon dioxide emissions. Given the ongoing demographic growth and rising energy consumption in metropolitan regions particularly in the developing world, urban-based emissions are expected to further increase in the future. As a consequence, monitoring and independent verification of reported anthropogenic emissions is becoming more and more important. It is demonstrated using SCIAMACHY nadir measurements that anthropogenic CO2 emissions can be detected from space and that emission trends might be tracked using satellite observations. This is promising with regard to future satellite missions with high spatial resolution and wide swath imaging capability aiming at constraining anthropogenic emissions down to the point-source scale. By subtracting retrieved background values from those retrieved over urban areas we find significant CO2 enhancements for several anthropogenic source regions, namely 1.3 ± 0.7 ppm for the Rhine-Ruhr metropolitan region and the Benelux, 1.1 ± 0.5 ppm for the East Coast of the United States, and 2.4 ± 0.9 ppm for the Yangtze River Delta. The order of magnitude of the enhancements is in agreement with what is expected for anthropogenic CO2 signals. The larger standard deviation of the retrieved Yangtze River Delta enhancement is due to a distinct positive trend of 0.3 ± 0.2 ppm yr−1, which is quantitatively consistent with anthropogenic emissions from the Emission Database for Global Atmospheric Research (EDGAR) in terms of percentual increase per year. Potential contributions to the retrieved CO2 enhancement by several error sources, e.g. aerosols, albedo, and residual biospheric signals due to heterogeneous seasonal sampling, are discussed and can be ruled out to a large extent.

We analyze an ensemble of seven XCO2 retrieval algorithms for SCIAMACHY (scanning imaging absorption spectrometer of atmospheric chartography) and GOSAT (greenhouse gases observing satellite). The ensemble spread can be interpreted as regional uncertainty and can help to identify locations for new TCCON (total carbon column observing network) validation sites. Additionally, we introduce the ensemble median algorithm EMMA combining individual soundings of the seven algorithms into one new data set. The ensemble takes advantage of the algorithms' independent developments. We find ensemble spreads being often < 1 ppm but rising up to 2 ppm especially in the tropics and East Asia. On the basis of gridded monthly averages, we compare EMMA and all individual algorithms with TCCON and CarbonTracker model results (potential outliers, north/south gradient, seasonal (peak-to-peak) amplitude, standard deviation of the difference). Our findings show that EMMA is a promising candidate for inverse modeling studies. Compared to CarbonTracker, the satellite retrievals find consistently larger north/south gradients (by 0.3–0.9 ppm) and seasonal amplitudes (by 1.5–2.0 ppm).

SCIAMACHY onboard ENVISAT (launched in 2002) enables the retrieval of global long-term column-averaged dry air mole fractions of the two most important anthropogenic greenhouse gases carbon dioxide and methane (denoted XCO2 and XCH4). In order to assess the quality of the greenhouse gas data obtained with the recently introduced v2 of the scientific retrieval algorithm WFM-DOAS, we present validations with ground-based Fourier Transform Spectrometer (FTS) measurements and comparisons with model results at eight Total Carbon Column Observing Network (TCCON) sites providing realistic error estimates of the satellite data. Such validation is a prerequisite to assess the suitability of data sets for their use in inverse modelling. It is shown that there are generally no significant differences between the carbon dioxide annual increases of SCIAMACHY and the assimilation system CarbonTracker (2.00 &pm; 0.16 ppm yr−1 compared to 1.94 &pm; 0.03 ppm yr−1 on global average). The XCO2 seasonal cycle amplitudes derived from SCIAMACHY are typically larger than those from TCCON which are in turn larger than those from CarbonTracker. The absolute values of the northern hemispheric TCCON seasonal cycle amplitudes are closer to SCIAMACHY than to CarbonTracker and the corresponding differences are not significant when compared with SCIAMACHY, whereas they can be significant for a subset of the analysed TCCON sites when compared with CarbonTracker. At Darwin we find discrepancies of the seasonal cycle derived from SCIAMACHY compared to the other data sets which can probably be ascribed to occurrences of undetected thin clouds. Based on the comparison with the reference data, we conclude that the carbon dioxide data set can be characterised by a regional relative precision (mean standard deviation of the differences) of about 2.2 ppm and a relative accuracy (standard deviation of the mean differences) of 1.1–1.2 ppm for monthly average composites within a radius of 500 km. For methane, prior to November 2005, the regional relative precision amounts to 12 ppb and the relative accuracy is about 3 ppb for monthly composite averages within the same radius. The loss of some spectral detector pixels results in a degradation of performance thereafter in the spectral range currently used for the methane column retrieval. This leads to larger scatter and lower XCH4 values are retrieved in the tropics for the subsequent time period degrading the relative accuracy. As a result, the overall relative precision is estimated to be 17 ppb and the relative accuracy is in the range of about 10–20 ppb for monthly averages within a radius of 500 km. The derived estimates show that the SCIAMACHY XCH4 data set before November 2005 is suitable for regional source/sink determination and regional-scale flux uncertainty reduction via inverse modelling worldwide. In addition, the XCO2 monthly data potentially provide valuable information in continental regions, where there is sparse sampling by surface flask measurements.

Carbon dioxide (CO2) and methane (CH4) are the two most important anthropogenic greenhouse gases contributing to global climate change. SCIAMACHY onboard ENVISAT (launch 2002) was the first and is now with TANSO onboard GOSAT (launch 2009) one of only two satellite instruments currently in space whose measurements are sensitive to CO2 and CH4 concentration changes in the lowest atmospheric layers where the variability due to sources and sinks is largest. We present long-term SCIAMACHY retrievals (2003–2009) of column-averaged dry air mole fractions of both gases (denoted XCO2 and XCH4) derived from absorption bands in the near-infrared/shortwave-infrared (NIR/SWIR) spectral region focusing on large-scale features. The results are obtained using an upgraded version (v2) of the retrieval algorithm WFM-DOAS including several improvements, while simultaneously maintaining its high processing speed. The retrieved mole fractions are compared to global model simulations (CarbonTracker XCO2 and TM5 XCH4) being optimised by assimilating highly accurate surface measurements from the NOAA/ESRL network and taking the SCIAMACHY averaging kernels into account. The comparisons address seasonal variations and long-term characteristics. The steady increase of atmospheric carbon dioxide primarily caused by the burning of fossil fuels can be clearly observed with SCIAMACHY globally. The retrieved global annual mean XCO2 increase agrees with CarbonTracker within the error bars (1.80±0.13 ppm yr−1 compared to 1.81±0.09 ppm yr−1). The amplitude of the XCO2 seasonal cycle as retrieved by SCIAMACHY, which is 4.3±0.2 ppm for the Northern Hemisphere and 1.4±0.2 ppm for the Southern Hemisphere, is on average about 1 ppm larger than for CarbonTracker. An investigation of the boreal forest carbon uptake during the growing season via the analysis of longitudinal gradients shows good agreement between SCIAMACHY and CarbonTracker concerning the overall magnitude of the gradients and their annual variations. The analysis includes a discussion of the relative uptake strengths of the Russian and North American boreal forest regions. The retrieved XCH4 results show that after years of stability, atmospheric methane has started to rise again in recent years which is consistent with surface measurements. The largest increase is observed for the tropics and northern mid- and high-latitudes amounting to about 7.5±1.5 ppb yr−1 since 2007. Due care has been exercised to minimise the influence of detector degradation on the quantitative estimate of this anomaly.

Total column concentrations of methane have been retrieved from ground-based solar absorption FTIR spectra in the near-infrared recorded in Paramaribo (Suriname). The methane FTIR observations are compared with TM5 model simulations and satellite observations from SCIAMACHY, and represent the first validation of SCIAMACHY retrievals in the inner tropics using ground-based remote sensing techniques. Apart from local biomass burning features, our methane FTIR observations agree well with TM5 model simulations. The comparison of the direct measured CH4/CO2 ratios by FTIR and satellite reveals that the satellite can hardly detect methane emissions of tropical biomass burning due to the used retrieval method.

Carbon dioxide (CO2) and methane (CH4) are the two most important anthropogenic greenhouse gases. SCIAMACHY on ENVISAT is the first satellite instrument whose measurements are sensitive to concentration changes of the two gases at all altitude levels down to the Earth's surface where the source/sink signals are largest. We have processed three years (2003–2005) of SCIAMACHY near-infrared nadir measurements to simultaneously retrieve vertical columns of CO2 (from the 1.58 μm absorption band), CH4 (1.66 μm) and oxygen (O2 A-band at 0.76 μm) using the scientific retrieval algorithm WFM-DOAS. We show that the latest version of WFM-DOAS, version 1.0, which is used for this study, has been significantly improved with respect to its accuracy compared to the previous versions while essentially maintaining its high processing speed (~1 min per orbit, corresponding to ~6000 single measurements, and per gas on a standard PC). The greenhouse gas columns are converted to dry air column-averaged mole fractions, denoted XCO2 (in ppm) and XCH4 (in ppb), by dividing the greenhouse gas columns by simultaneously retrieved dry air columns. For XCO2 dry air columns are obtained from the retrieved O2 columns. For XCH4 dry air columns are obtained from the retrieved CO2 columns because of better cancellation of light path related errors compared to using O2 columns retrieved from the spectrally distant O2 A-band. Here we focus on a discussion of the XCH4 data set. The XCO2 data set is discussed in a separate paper (Part 1). For 2003 we present detailed comparisons with the TM5 model which has been optimally matched to highly accurate but sparse methane surface observations. After accounting for a systematic low bias of ~2% agreement with TM5 is typically within 1–2%. We investigated to what extent the SCIAMACHY XCH4 is influenced by the variability of atmospheric CO2 using global CO2 fields from NOAA's CO2 assimilation system CarbonTracker. We show that the CO2 corrected and uncorrected XCH4 spatio-temporal pattern are very similar but that agreement with TM5 is better for the CarbonTracker CO2 corrected XCH4. In line with previous studies (e.g., Frankenberg et al., 2005b) we find higher methane over the tropics compared to the model. We show that tropical methane is also higher when normalizing the CH4 columns with retrieved O2 columns instead of CO2. In consistency with recent results of Frankenberg et al. (2008b) it is shown that the magnitude of the retrieved tropical methane is sensitive to the choice of the spectroscopic line parameters of water vapour. Concerning inter-annual variability we find similar methane spatio-temporal pattern for 2003 and 2004. For 2005 the retrieved methane shows significantly higher variability compared to the two previous years, most likely due to somewhat larger noise of the spectral measurements.

Carbon dioxide (CO2) and methane (CH4) are the two most important anthropogenic greenhouse gases. SCIAMACHY on ENVISAT is the first satellite instrument whose measurements are sensitive to concentration changes of the two gases at all altitude levels down to the Earth's surface where the source/sink signals are largest. We have processed three years (2003–2005) of SCIAMACHY near-infrared nadir measurements to simultaneously retrieve vertical columns of CO2 (from the 1.58 μm absorption band), CH4 (1.66 μm) and oxygen (O2 A-band at 0.76 μm) using the scientific retrieval algorithm WFM-DOAS. We show that the latest version of WFM-DOAS, version 1.0, which is used for this study, has been significantly improved with respect to its accuracy compared to the previous versions while essentially maintaining its high processing speed (~1 min per orbit, corresponding to ~6000 single measurements, and per gas on a standard PC). The greenhouse gas columns are converted to dry air column-averaged mole fractions, denoted XCO2 (in ppm) and XCH4 (in ppb), by dividing the greenhouse gas columns by simultaneously retrieved dry air columns. For XCO2 dry air columns are obtained from the retrieved O2 columns. For XCH4 dry air columns are obtained from the retrieved CO2 columns because of better cancellation of light path related errors compared to using O2 columns retrieved from the spectrally distant O2 A-band. Here we focus on a discussion of the XCO2 data set. The XCH4 data set is discussed in a separate paper (Part 2). In order to assess the quality of the retrieved XCO2 we present comparisons with Fourier Transform Spectroscopy (FTS) XCO2 measurements at two northern hemispheric mid-latitude ground stations. To assess the quality globally, we present detailed comparisons with global XCO2 fields obtained from NOAA's CO2 assimilation system CarbonTracker. For the Northern Hemisphere we find good agreement with the reference data for the CO2 seasonal cycle and the CO2 annual increase. For the Southern Hemisphere, where significantly less data are available for averaging compared to the Northern Hemisphere, the CO2 annual increase is also in good agreement with CarbonTracker but the amplitude and phase of the seasonal cycle show systematic differences (up to several ppm) arising partially from the O2 normalization most likely caused by unconsidered scattering effects due to subvisual cirrus clouds. The retrieved XCO2 regional pattern at monthly resolution over various regions show clear correlations with CarbonTracker but also significant differences. Typically the retrieved variability is about 4 ppm (1% of 380 ppm) higher but depending on time and location differences can reach or even exceed 8 ppm. Based on the error analysis and on the comparison with the reference data we conclude that the XCO2 data set can be characterized by a single measurement retrieval precision (random error) of 1–2%, a systematic low bias of about 1.5%, and by a relative accuracy of about 1–2% for monthly averages at a spatial resolution of about 7°×7°. When averaging the SCIAMACHY XCO2 over all three years we find elevated CO2 over the highly populated region of western central Germany and parts of the Netherlands ("Rhine-Main area") reasonably well correlated with EDGAR anthropogenic CO2 emissions. On average the regional enhancement is 2.7 ppm including an estimated contribution of 1–1.5 ppm due to aerosol related errors and sampling.

The reliable prediction of future atmospheric CO2 concentrations and associated global climate change requires an adequate understanding of the CO2 sources and sinks. The sparseness of the existing surface measurement network limits current knowledge about the global distribution of CO2 surface fluxes. The retrieval of CO2 total vertical columns from satellite observations is predicted to improve this situation. Such an application however requires very high accuracy and precision. We report on retrievals of the column-averaged CO2 dry air mole fraction, denoted XCO2, from the near-infrared nadir spectral radiance and solar irradiance measurements of the SCIAMACHY satellite instrument between 2003 and 2005. We focus on northern hemispheric large scale CO2 features such as the CO2 seasonal cycle and show - for the first time - that the atmospheric annual increase of CO2 can be directly observed using satellite measurements of the CO2 total column. The satellite retrievals are compared with global XCO2 obtained from NOAA's CO2 assimilation system CarbonTracker taking into account the spatio-temporal sampling and altitude sensitivity of the satellite data. We show that the measured CO2 year-to-year increase agrees within about 1 ppm/year with CarbonTracker. We also show that the latitude dependent amplitude of the northern hemispheric CO2 seasonal cycle agrees with CarbonTracker within about 2 ppm with the retrieved amplitude being systematically larger. The analysis demonstrates that it is possible using satellite measurements of the CO2 total column to retrieve information on the atmospheric CO2 on the level of a few parts per million.

The three carbon gases carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) are important atmospheric constituents affecting air quality and climate. The near-infrared nadir spectra measured by SCIAMACHY on ENVISAT contain information on the vertical columns of these gases which we retrieve using a modified DOAS algorithm (WFM-DOAS or WFMD). Our main data products are CO vertical columns and dry-air column averaged mixing ratios of methane (CH4) and CO2 (denoted XCH4 and XCO2). For CO and CH4 we present new results for the year 2003 obtained with an improved version of WFM-DOAS (WFMDv0.5) retrieved from Level 1 version 4 (Lv1v4) spectra. This data set has recently been compared with a network of ground based FTIR stations. Here we describe the WFMDv0.5 algorithm, present global and regional maps, and comparisons with global reference data. We show that major problems of the previous versions (v0.4 and v0.41) related to the varying ice-layer on the SCIAMACHY channel 8 detector have been solved. Compared to MOPITT the SCIAMACHY CO columns are on average higher by about 10–20%. Regionally, however, especially over central South America, differences can be much larger. For methane we present global and regional maps which are compared to TM5 model simulations performed using standard methane emission inventories. We show that methane source regions can be clearly detected with SCIAMACHY. We also show that the methane data product can be significantly further improved using Lv1v5 spectra with improved calibration. For CO2 we present three years of SCIAMACHY CO2 measurements over Park Falls, Wisconsin, USA, retrieved from Lv1v5. We show that the quality of CO2 retrieved from these spectra is significantly higher compared to WFMDv0.4 XCO2 retrieved from Lv1v4.

No abstract available.