Power plant exhausts can be identified and quantified from satellite observations.

<p>Satellite observations of NO<sub>2</sub> provide valuable information on the location and strength of NO<sub>x</sub> emissions, but spatial resolution is limited by horizontal transport and smearing of temporal averages due to changing wind fields. The divergence (spatial derivative) of the mean horizontal flux, however, is highly sensitive for point sources like power plant exhaust stacks.</p><p>In a previous study, point source emissions have been identified and quantified exemplarily for Riyadh, South Africa, and Germany with a detection limit of about 0.11 kg/s down to 0.03 kg/s for ideal conditions, based on TROPOMI NO<sub>2</sub> columns and ECMWF wind fields (Beirle et al., Science Advances, 2019).</p><p>Here we extend this study and derive a global catalog of NO<sub>x</sub> emissions from point sources. The specific challenges for e.g. high latitudes (longer NO<sub>x</sub> lifetime) or coastlines (potentially persistent diurnal wind patterns) are investigated.</p>

Abstract. This work presents the methane (CH4) and nitrous oxide (N2O) products as generated by the IASI (Infrared Atmospheric Sounding Interferometer) processor developed during the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water). The processor retrieves CH4 and N2O with different water vapour and water vapour isotopologues (as well as HNO3) and uses a single a priori data set for all the retrievals (no variation in space and time). Firstly, the characteristics and errors of the products are analytically described. Secondly, the products are comprehensively evaluated by comparisons to the following reference data measured by different techniques and from different platforms as follows: (1) aircraft CH4 and N2O profiles from the five HIAPER Pole-to-Pole Observation (HIPPO) missions; (2) continuous in situ CH4 and N2O observations performed between 2007 and 2017 at subtropical and mid-latitude high-mountain observatories (Izaña Atmospheric Observatory and Jungfraujoch, respectively) in the framework of the WMO–GAW (World Meteorological Organization–Global Atmosphere Watch) programme; (3) ground-based FTIR (Fourier-transform infrared spectrometer) measurements made between 2007 and 2017 in the framework of the NDACC (Network for the Detection of Atmospheric Composition Change) at the subtropical Izaña Atmospheric Observatory, the mid-latitude station of Karlsruhe and the Kiruna polar site.The theoretical estimations and the comparison studies suggest a precision for the N2O and CH4 retrieval products of about 1.5–3 % and systematic errors due to spectroscopic parameters of about 2 %. The MUSICA IASI CH4 data offer a better sensitivity than N2O data. While for the latter the sensitivity is mainly limited to the UTLS (upper troposphere–lower stratosphere) region, for CH4 we are able to prove that at low latitudes the MUSICA IASI processor can detect variations that take place in the free troposphere independently from the variations in the UTLS region. We demonstrate that the MUSICA IASI data qualitatively capture the CH4 gradients between low and high latitudes and between the Southern Hemisphere and Northern Hemisphere; however, we also find an inconsistency between low- and high-latitude CH4 data of up to 5 %. The N2O latitudinal gradients are very weak and cannot be detected. We make comparisons over a 10-year time period and analyse the agreement with the reference data on different timescales. The MUSICA IASI data can detect day-to-day signals (only in the UTLS), seasonal cycles and long-term evolution (in the UTLS and for CH4 also in the free troposphere) similar to the reference data; however, there are also inconsistencies in the long-term evolution connected to inconsistencies in the used atmospheric temperature a priori data.Moreover, we present a method for analytically describing the a posteriori-calculated logarithmic-scale difference of the CH4 and N2O retrieval estimates. By correcting errors that are common in the CH4 and N2O retrieval products, the a posteriori-calculated difference can be used for generating an a posteriori-corrected CH4 product with a theoretically better precision than the original CH4 retrieval products. We discuss and evaluate two different approaches for such a posteriori corrections. It is shown that the correction removes the inconsistencies between low and high latitudes and enables the detection of day-to-day signals also in the free troposphere. Furthermore, they reduce the impact of short-term atmospheric dynamics, which is an advantage, because respective signals are presumably hardly comparable to model data. The approach that affects the correction solely on the scales on which the errors dominate is identified as the most efficient, because it reduces the inconsistencies and errors without removing measurable real atmospheric signals. We give a brief outlook on a possible usage of this a posteriori-corrected MUSICA IASI CH4 product in combination with inverse modelling.

Abstract. Total column water vapour has been retrieved from TROPOMI measurements in the visible blue spectral range and compared to a variety of different reference data sets for clear-sky conditions during boreal summer and winter. The retrieval consists of the common two-step DOAS approach: first the spectral analysis is performed within a linearized scheme and then the retrieved slant column densities are converted to vertical columns using an iterative scheme for the water vapour a priori profile shape, which is based on an empirical parameterization of the water vapour scale height. Moreover, a modified albedo map was used combining the OMI LER albedo and scaled MODIS albedo map. The use of the alternative albedo is especially important over regions with very low albedo and high probability of clouds like the Amazon region. The errors of the total column water vapour (TCWV) retrieval have been theoretically estimated considering the contribution of a variety of different uncertainty sources. For observations during clear-sky conditions, over ocean surface, and at low solar zenith angles the error typically is around values of 10 %–20 %, and during cloudy-sky conditions, over land surface, and at high solar zenith angles it reaches values around 20 %–50 %. In the framework of a validation study the retrieval demonstrates that it can well capture the global water vapour distribution: the retrieved H2O vertical column densities (VCDs) show very good agreement with the reference data sets over ocean for boreal summer and winter whereby the modified albedo map substantially improves the retrieval's consistency to the reference data sets, in particular over tropical land masses. However, over land the retrieval underestimates the VCD by about 10 %, particularly during summertime. Our investigations show that this underestimation is likely caused by uncertainties within the surface albedo and the cloud input data: low-level clouds cause an underestimation, but for mid- to high-level clouds good agreement is found. In addition, our investigations indicate that these biases can probably be further reduced by the use of improved cloud input data. For the general purpose we recommend only using VCDs with cloud fraction <20 % and AMF >0.1, which represents a good compromise between spatial coverage and retrieval accuracy. The TCWV retrieval can be easily applied to further satellite sensors (e.g. GOME-2 or OMI) for creating uniform, long-term measurement data sets, which is particularly interesting for climate and trend studies of water vapour.

Abstract. Volume mixing ratio water vapour profiles have been retrieved from IASI (Infrared Atmospheric Sounding Interferometer) spectra using the MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water) processor. The retrievals are done for IASI observations that coincide with Vaisala RS92 radiosonde measurements performed in the framework of the GCOS (Global Climate Observing System) Reference Upper-Air Network (GRUAN) in three different climate zones: the tropics (Manus Island, 2° S), mid-latitudes (Lindenberg, 52° N), and polar regions (Sodankylä, 67° N). The retrievals show good sensitivity with respect to the vertical H2O distribution between 1 km above ground and the upper troposphere. Typical DOFS (degrees of freedom for signal) values are about 5.6 for the tropics, 5.1 for summertime mid-latitudes, 3.8 for wintertime mid-latitudes, and 4.4 for summertime polar regions. The errors of the MUSICA IASI water vapour profiles have been theoretically estimated considering the contribution of many different uncertainty sources. For all three climate regions, unrecognized cirrus clouds and uncertainties in atmospheric temperature have been identified as the most important error sources and they can reach about 25 %. The MUSICA IASI water vapour profiles have been compared to 100 individual coincident GRUAN water vapour profiles. The systematic difference between the data is within 11 % below 12 km altitude; however, at higher altitudes the MUSICA IASI data show a dry bias with respect to the GRUAN data of up to 21 %. The scatter is largest close to the surface (30 %), but never exceeds 21 % above 1 km altitude. The comparison study documents that the MUSICA IASI retrieval processor provides H2O profiles that capture the large variations in H2O volume mixing ratio profiles well from 1 km above ground up to altitudes close to the tropopause. Above 5 km the observed scatter with respect to GRUAN data is in reasonable agreement with the combined MUSICA IASI and GRUAN random errors. The increased scatter at lower altitudes might be explained by surface emissivity uncertainties at the summertime continental sites of Lindenberg and Sodankylä, and the upper tropospheric dry bias might suggest deficits in correctly modelling the spectroscopic line shapes of water vapour.

Abstract. We present version 1.0 of a global catalog of NOx emissions from point sources, derived from TROPOspheric Monitoring Instrument (TROPOMI) measurements of tropospheric NO2 for 2018–2019. The identification of sources and quantification of emissions are based on the divergence (spatial derivative) of the mean horizontal flux, which is highly sensitive for point sources like power plant exhaust stacks. The catalog lists 451 locations which could be clearly identified as NOx point sources by a fully automated algorithm, while ambiguous cases as well as area sources such as megacities are skipped. A total of 242 of these point sources could be automatically matched to power plants. Other NOx point sources listed in the catalog are metal smelters, cement plants, or industrial areas. The four largest localized NOx emitters are all coal combustion plants in South Africa. About 1/4 of all detected point sources are located in the Indian subcontinent and are mostly associated with power plants. The catalog is incomplete, mainly due to persisting gaps in the TROPOMI NO2 product at some coastlines, inaccurate or complex wind fields in coastal and mountainous regions, and high noise in the divergence maps for high background pollution. The derived emissions are generally too low, lacking a factor of about 2 up to 8 for extreme cases. This strong low bias results from combination of different effects, most of all a strong underestimation of near-surface NO2 in TROPOMI NO2 columns. Still, the catalog has high potential for checking and improving emission inventories, as it provides accurate and independent up-to-date information on the location of sources of NOx and thus also CO2. The catalog of NOx emissions from point sources is freely available at https://doi.org/10.26050/WDCC/Quant_NOx_TROPOMI (Beirle et al., 2020).

Abstract. The project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water) has shown that the sensor IASI aboard the satellite MetOp can measure the free tropospheric {H2O,δD} pair distribution twice per day on a quasi-global scale. Such data are very promising for investigating tropospheric moisture pathways, however, the complex data characteristics compromise their usage in the context of model evaluation studies. Here we present a tool that allows for simulating MUSICA MetOp/IASI {H2O,δD} pair remote sensing data for a given model atmosphere, thereby creating model data that have the remote sensing data characteristics assimilated. This model data can then be compared to the MUSICA data. The retrieval simulation method is based on the physical principles of radiative transfer and we show that the uncertainty of the simulations is within the uncertainty of the MUSICA MetOp/IASI products, i.e. the retrieval simulations are reliable enough. We demonstrate the working principle of the simulator by applying it to ECHAM5-wiso model data. The few case studies clearly reveal the large potential of the MUSICA MetOp/IASI {H2O,δD} data pairs for evaluating modelled moisture pathways. The tool is made freely available in form of MATLAB and Python routines and can be easily connected to any atmospheric water vapour isotopologue model.

Abstract. In this study, we investigate trends in total column water vapour (TCWV) retrieved from measurements of the Ozone Monitoring Instrument (OMI) for the time range between January 2005 to December 2020. The trend analysis reveals, on global average, an annual increase in the TCWV amount of approximately +0.054 kg m−2 yr−1 or +0.21 % yr−1. After the application of a Z test (to the significance level of 5 %) and a false discovery rate (FDR) test to the results of the trend analysis, mainly positive trends remain, in particular over the northern subtropics in the eastern Pacific. Combining the relative TCWV trends with trends in air temperature, we also analyse trends in relative humidity (RH) on the local scale. This analysis reveals that the assumption of temporally invariant RH is not always fulfilled, as we obtain increasing and decreasing RH trends over large areas of the ocean and land surface and also observe that these trends are not limited to arid and humid regions, respectively. For instance, we find decreasing RH trends over the (humid) tropical Pacific Ocean in the region of the Intertropical Convergence Zone. Interestingly, these decreasing RH trends in the tropical Pacific Ocean coincide well with decreasing trends in precipitation. Moreover, by combining the trends of TCWV, surface temperature, and precipitation, we derive trends for the global water vapour turnover time (TUT) of approximately +0.02 d yr−1. Also, we obtain a TUT rate of change of around 8.4 % K−1, which is 2 to 3 times higher than the values obtained in previous studies.