Three-dimensional radiative transfer effects on airborne and ground-based trace gas remote sensing

Air mass factors (AMFs) are used in passive trace gas remote sensing for converting slant column densities (SCDs) to vertical column densities (VCDs). AMFs are traditionally computed with 1D radiative transfer models assuming horizontally homogeneous conditions. However, when observations are made with high spatial resolution in a heterogeneous atmosphere or above a heterogeneous surface, 3D effects may not be negligible. To study the importance of 3D effects on AMFs for different types of trace gas remote sensing, we implemented 1D-layer and 3D-box AMFs into the Monte carlo code for the phYSically correct Tracing of photons In Cloudy atmospheres (MYSTIC), a solver of the libRadtran radiative transfer model (RTM). The 3D-box AMF implementation is fully consistent with 1D-layer AMFs under horizontally homogeneous conditions and agrees very well ( < 5 % relative error) with 1D-layer AMFs computed by other RTMs for a wide range of scenarios. The 3D-box AMFs make it possible to visualize the 3D spatial distribution of the sensitivity of a trace gas observation, which we demonstrate with two examples. First, we computed 3D-box AMFs for ground-based multi-axis spectrometer (MAX-DOAS) observations for different viewing geometry and aerosol scenarios. The results illustrate how the sensitivity reduces with distance from the instrument and that a non-negligible part of the signal originates from outside the line of sight. Such information is invaluable for interpreting MAX-DOAS observations in heterogeneous environments such as urban areas. Second, 3D-box AMFs were used to generate synthetic nitrogen dioxide (NO2) SCDs for an air-borne imaging spectrometer observing the NO2 plume emitted from a tall stack. The plume was imaged under different solar zenith angles and solar azimuth angles. To demonstrate the limitations of classical 1D-layer AMFs, VCDs were then computed assuming horizontal homogeneity. As a result, the imaged NO2 plume was shifted in space, which led to a strong underestimation of the total VCDs in the plume maximum and an underestimation of the integrated line densities that can be used for estimating emissions from NO2 images. The two examples demonstrate the importance of 3D effects for several types of ground-based and airborne remote sensing when the atmosphere cannot be assumed to be horizontally homogeneous, which is typically the case in the vicinity of emission sources or in cities

Spatial and temporal representativeness of point measurements for nitrogen dioxide pollution levels in cities

In many cities around the world the overall air quality is improving, but at the same time nitrogen dioxide (NO2) trends show stagnating values and in many cases could not be reduced below air quality standards recommended by the World Health Organization (WHO). Many large cities have built monitoring stations to continuously measure different air pollutants. While most stations follow defined rules in terms of measurement height and distance to traffic emissions, the question remains of how representative are those point measurements for the city-wide air quality. The question of the spatial coverage of a point measurement is important because it defines the area of influence and coverage of monitoring networks, determines how to assimilate monitoring data into model simulations or compare to satellite data with a coarser resolution, and is essential to assess the impact of the acquired data on public health. In order to answer this question, we combined different measurement data sets consisting of path-averaging remote sensing data and in situ point measurements in stationary and mobile setups from a measurement campaign that took place in Munich, Germany, in June and July 2016. We developed an algorithm to strip temporal from spatial patterns in order to construct a consistent NO2 pollution map for Munich. Continuous long-path differential optical absorption spectroscopy (LP DOAS) measurements were complemented with mobile cavity-enhanced (CE) DOAS, chemiluminescence (CL) and cavity attenuated phase shift (CAPS) instruments and were compared to monitoring stations and satellite data. In order to generate a consistent composite map, the LP DOAS diurnal cycle has been used to normalize for the time of the day dependency of the source patterns, so that spatial and temporal patterns can be analyzed separately. The resulting concentration map visualizes pollution hot spots at traffic junctions and tunnel exits in Munich, providing insights into the strong spatial variations. On the other hand, this database is beneficial to the urban planning and the design of control measures of environment pollution. Directly comparing on-street mobile measurements in the vicinity of monitoring stations resulted in a difference of 48 %. For the extrapolation of the monitoring station data to street level, we determined the influence of the measuring height and distance to the street. We found that a measuring height of 4 m, at which the Munich monitoring stations measure, results in 16 % lower average concentrations than a measuring height of 1.5 m, which is the height of the inlet of our mobile measurements and a typical pedestrian breathing height. The horizontal distance of most stations to the center of the street of about 6 m also results in an average reduction of 13 % compared to street level concentration. A difference of 21 % in the NO2 concentrations remained, which could be an indication that city-wide measurements are needed for capturing the full range and variability of concentrations for assessing pollutant exposure and air quality in cities

Analyzing Local Carbon Dioxide and Nitrogen Oxide Emissions From Space Using the Divergence Method: An Application to the Synthetic SMARTCARB Dataset

Since the Paris Agreement was adopted in 2015, the role of space-based observations for monitoring anthropogenic greenhouse gas (GHG) emissions has increased. To meet the requirements for monitoring carbon dioxide (CO2) emissions, the European Copernicus programme is preparing a dedicated CO2 Monitoring (CO2M) satellite constellation that will provide CO2 and nitrogen dioxide (NO2) observations at 4 km2 resolution along a 250 km wide swath. In this paper, we adapt the recently developed divergence method to derive both CO2 and nitrogen oxide (NOx) emissions of cities and power plants from a CO2M satellite constellation by using synthetic observations from the COSMO-GHG model. Due to its long lifetime, the large CO2 atmospheric background needs to be removed to highlight the anthropogenic enhancements before calculating the divergence. Since the CO2 noise levels are large compared to the anthropogenic enhancements, we apply different denoising methods and compare the effect on the CO2 emission estimates. The annual NOx and CO2 emissions estimated from the divergence maps using the peak fitting approach are in agreement with the expected values, although with larger uncertainties for CO2. We also consider the possibility to use co-emitted NOx emission estimates for quantifying the CO2 emissions, by using source-specific NOx-to-CO2 emission ratios derived directly from satellite observations. In general, we find that the divergence method provides a promising tool for estimating CO2 emissions, alternative to typical methods based on inverse modeling or on the analysis of individual CO2 plumes

Mapping the spatial distribution of NO2 with in situ and remote sensing instruments during the Munich NO2 imaging campaign

We present results from the Munich Nitrogen dioxide (NO2) Imaging Campaign (MuNIC), where NO2 near-surface concentrations (NSCs) and vertical column densities (VCDs) were measured with stationary, mobile, and airborne in situ and remote sensing instruments in Munich, Germany. The most intensive day of the campaign was 7 July 2016, when the NO2 VCD field was mapped with the Airborne Prism Experiment (APEX) imaging spectrometer. The spatial distribution of APEX VCDs was rather smooth, with a horizontal gradient between lower values upwind and higher values downwind of the city center. The NO2 map had no pronounced source signatures except for the plumes of two combined heat and power (CHP) plants. The APEX VCDs have a fair correlation with mobile multi-axis differential optical absorption spectroscopy (MAX-DOAS) observations from two vehicles conducted on the same afternoon (r=0.55). In contrast to the VCDs, mobile NSC measurements revealed high spatial and temporal variability along the roads, with the highest values in congested areas and tunnels. The NOx emissions of the two CHP plants were estimated from the APEX observations using a mass-balance approach. The NOx emission estimates are consistent with CO2 emissions determined from two ground-based Fourier transform infrared (FTIR) instruments operated near one CHP plant. The estimates are higher than the reported emissions but are probably overestimated because the uncertainties are large, as conditions were unstable and convective with low and highly variable wind speeds. Under such conditions, the application of mass-balance approaches is problematic because they assume steady-state conditions. We conclude that airborne imaging spectrometers are well suited for mapping the spatial distribution of NO2 VCDs over large areas. The emission plumes of point sources can be detected in the APEX observations, but accurate flow fields are essential for estimating emissions with sufficient accuracy. The application of airborne imaging spectrometers for studying NSCs is less straightforward and requires us to account for the non-trivial relationship between VCDs and NSCs

Quantifying CO2 emissions of a city with the Copernicus Anthropogenic CO2 Monitoring satellite mission

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An Algorithm for In-Flight Spectral Calibration of Imaging Spectrometers

Accurate spectral calibration of satellite and airborne spectrometers is essential for remote sensing applications that rely on accurate knowledge of center wavelength (CW) positions and slit function parameters (SFP). We present a new in-flight spectral calibration algorithm that retrieves CWs and SFPs across a wide spectral range by fitting a high-resolution solar spectrum and atmospheric absorbers to in-flight radiance spectra. Using a maximum a posteriori optimal estimation approach, the quality of the fit can be improved with a priori information. The algorithm was tested with synthetic spectra and applied to data from the APEX imaging spectrometer over the spectral range of 385–870 nm. CWs were retrieved with high accuracy (uncertainty &lt;0.05 spectral pixels) from Fraunhofer lines below 550 nm and atmospheric absorbers above 650 nm. This enabled a detailed characterization of APEX’s across-track spectral smile and a previously unknown along-track drift. The FWHMs of the slit function were also retrieved with good accuracy (&lt;10% uncertainty) for synthetic spectra, while some obvious misfits appear for the APEX spectra that are likely related to radiometric calibration issues. In conclusion, our algorithm significantly improves the in-flight spectral calibration of APEX and similar spectrometers, making them better suited for the retrieval of atmospheric and surface variables relying on accurate calibration

Deep learning applied to CO₂ power plant emissions quantification using simulated satellite images

International audienceAbstract. The quantification of emissions of greenhouse gases and air pollutants through the inversion of plumes in satellite images remains a complex problem that current methods can only assess with significant uncertainties. The anticipated launch of the CO2M (Copernicus Anthropogenic Carbon Dioxide Monitoring) satellite constellation in 2026 is expected to provide high-resolution images of CO2 (carbon dioxide) column-averaged mole fractions (XCO2), opening up new possibilities. However, the inversion of future CO2 plumes from CO2M will encounter various obstacles. A challenge is the low CO2 plume signal-to-noise ratio due to the variability in the background and instrumental errors in satellite measurements. Moreover, uncertainties in the transport and dispersion processes further complicate the inversion task. To address these challenges, deep learning techniques, such as neural networks, offer promising solutions for retrieving emissions from plumes in XCO2 images. Deep learning models can be trained to identify emissions from plume dynamics simulated using a transport model. It then becomes possible to extract relevant information from new plumes and predict their emissions. In this paper, we develop a strategy employing convolutional neural networks (CNNs) to estimate the emission fluxes from a plume in a pseudo-XCO2 image. Our dataset used to train and test such methods includes pseudo-images based on simulations of hourly XCO2, NO2 (nitrogen dioxide), and wind fields near various power plants in eastern Germany, tracing plumes from anthropogenic and biogenic sources. CNN models are trained to predict emissions from three power plants that exhibit diverse characteristics. The power plants used to assess the deep learning model's performance are not used to train the model. We find that the CNN model outperforms state-of-the-art plume inversion approaches, achieving highly accurate results with an absolute error about half of that of the cross-sectional flux method and an absolute relative error of ∼ 20 % when only the XCO2 and wind fields are used as inputs. Furthermore, we show that our estimations are only slightly affected by the absence of NO2 fields or a detection mechanism as additional information. Finally, interpretability techniques applied to our models confirm that the CNN automatically learns to identify the XCO2 plume and to assess emissions from the plume concentrations. These promising results suggest a high potential of CNNs in estimating local CO2 emissions from satellite images

Detectability of CO2 emission plumes of cities and power plants with the Copernicus Anthropogenic CO2 Monitoring (CO2M) mission

International audienceHigh-resolution atmospheric transport simulations were used to investigate the potential for detecting carbon dioxide (CO 2) plumes of the city of Berlin and neighboring power stations with the Copernicus Anthropogenic Carbon Dioxide Monitoring (CO2M) mission, which is a proposed constellation of CO 2 satellites with imaging capabilities. The potential for detecting plumes was studied for satellite images of CO 2 alone or in combination with images of nitrogen dioxide (NO 2) and carbon monoxide (CO) to investigate the added value of measurements of other gases co-emitted with CO 2 that have better signal-to-noise ratios. The additional NO 2 and CO images were either generated for instruments on the same CO2M satellites (2 km× 2 km resolution) or for the Sentinel-5 instrument (7.5 km× 7.5 km) assumed to fly 2 h earlier than CO2M. Realistic CO 2 , CO and NO X (= NO+NO 2) fields were simulated at 1 km× 1 km horizontal resolution with the Consortium for Small-scale Modeling model extended with a module for the simulation of greenhouse gases (COSMO-GHG) for the year 2015, and they were used as input for an orbit simulator to generate synthetic observations of columns of CO 2 , CO and NO 2 for constellations of up to six satellites. A simple plume detection algorithm was applied to detect coherent structures in the images of CO 2 , NO 2 or CO against instrument noise and variability in background levels. Although six satellites with an assumed swath of 250 km were sufficient to overpass Berlin on a daily basis, only about 50 out of 365 plumes per year could be observed in conditions suitable for emission estimation due to frequent cloud cover. With the CO 2 instrument only 6 and 16 of these 50 plumes could be detected assuming a high-noise (σ VEG50 = 1.0 ppm) and low-noise (σ VEG50 = 0.5 ppm) scenario, respectively, because the CO 2 signals were often too weak. A CO instrument with specifications similar to the Sentinel-5 mission performed worse than the CO 2 instrument, while the number of detectable plumes could be significantly increased to about 35 plumes with an NO 2 instrument. CO 2 and NO 2 plumes were found to overlap to a large extent, although NO X had a limited lifetime (assumed to be 4 h) and although CO 2 and NO X were emitted with different NO X : CO 2 emission ratios by different source types with different temporal and vertical emission profiles. Using NO 2 observations from the Sentinel-5 platform instead resulted in a significant spatial mismatch between NO 2 and CO 2 plumes due to the 2 h time difference between Sentinel-5 and CO2M. The plumes of the coal-fired power plant Jänschwalde were easier to detect with the CO 2 instrument (about 40-45 plumes per year), but, again, an NO 2 instrument could detect significantly more plumes (about 70). Auxiliary measurements of NO 2 were thus found to greatly enhance the capability of detecting the location of CO 2 plumes, which will be invaluable for the quantification of CO 2 emissions from large point sources