Abstract. High-resolution atmospheric transport simulations were used to investigate the potential for detecting carbon dioxide (CO2) 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 CO2 satellites with imaging capabilities. The potential for detecting plumes was studied for satellite images of CO2 alone or in combination with images of nitrogen dioxide (NO2) and carbon monoxide (CO) to investigate the added value of measurements of other gases coemitted with CO2 that have better signal-to-noise ratios. The additional NO2 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 CO2, CO and NOX(=NO+NO2) 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 CO2, CO and NO2 for constellations of up to six satellites. A simple plume detection algorithm was applied to detect coherent structures in the images of CO2, NO2 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 CO2 instrument only 6 and 16 of these 50 plumes could be detected assuming a high-noise (σVEG50=1.0 ppm) and low-noise (σVEG50=0.5 ppm) scenario, respectively, because the CO2 signals were often too weak. A CO instrument with specifications similar to the Sentinel-5 mission performed worse than the CO2 instrument, while the number of detectable plumes could be significantly increased to about 35 plumes with an NO2 instrument. CO2 and NO2 plumes were found to overlap to a large extent, although NOX had a limited lifetime (assumed to be 4 h) and although CO2 and NOX were emitted with different NOX:CO2 emission ratios by different source types with different temporal and vertical emission profiles. Using NO2 observations from the Sentinel-5 platform instead resulted in a significant spatial mismatch between NO2 and CO2 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 CO2 instrument (about 40–45 plumes per year), but, again, an NO2 instrument could detect significantly more plumes (about 70). Auxiliary measurements of NO2 were thus found to greatly enhance the capability of detecting the location of CO2 plumes, which will be invaluable for the quantification of CO2 emissions from large point sources.

Abstract. In this paper, we present the custom Hong Kong NO2 retrieval (HKOMI) for the Ozone Monitoring Instrument (OMI) on board the Aura satellite which was used to evaluate a high-resolution chemistry transport model (CTM) (3 km × 3 km spatial resolution). The atmospheric chemistry transport was modelled in the Pearl River Delta (PRD) region in southern China by the Models-3 Community Multiscale Air Quality (CMAQ) modelling system from October 2006 to January 2007. In the HKOMI NO2 retrieval, tropospheric air mass factors (AMFs) were recalculated using high-resolution ancillary parameters of surface reflectance, a priori NO2 and aerosol profiles, of which the latter two were taken from the CMAQ simulation. We tested the influence of the ancillary parameters on the data product using four different aerosol parametrizations. Ground-level measurements by the PRD Regional Air Quality Monitoring (RAQM) network were used as additional independent measurements. The HKOMI retrieval increases estimated tropospheric NO2 vertical column densities (VCD) by (+31 ± 38)%, when compared to NASA's standard product (OMNO2-SP), and improves the normalized mean bias (NMB) between satellite and ground observations by 26 percentage points from −41 to −15%. The individual influences of the parameters are (+11.4 ± 13.4)% for NO2 profiles, (+11.0 ± 20.9)% for surface reflectance and (+6.0 ± 8.4)% for the best aerosol parametrization. The correlation coefficient r is low between ground and satellite observations (r = 0.35). The low r and the remaining NMB can be explained by the low model performance and the expected differences when comparing point measurements with area-averaged satellite observations. The correlation between CMAQ and the RAQM network is low (r ≈ 0.3) and the model underestimates the NO2 concentrations in the northwestern model domain (Foshan and Guangzhou). We compared the CMAQ NO2 time series of the two main plumes with our best OMI NO2 data set (HKOMI-4). The model overestimates the NO2 VCDs by about 15% in Hong Kong and Shenzhen, while the correlation coefficient is satisfactory (r = 0.56). In Foshan and Guangzhou, the correlation is low (r = 0.37) and the model underestimates the VCDs strongly (NMB = −40%). In addition, we estimated that the OMI VCDs are also underestimated by about 10 to 20% in Foshan and Guangzhou because of the influence of the model parameters on the AMFs. In this study, we demonstrate that the HKOMI NO2 retrieval reduces the bias of the satellite observations and how the data set can be used to study the magnitude of NO2 concentrations in a regional model at high spatial resolution of 3 × 3 km2. The low bias was achieved with recalculated AMFs using updated surface reflectance, aerosol profiles and NO2 profiles. Since unbiased concentrations are important, for example, in air pollution studies, the results of this paper can be very helpful in future model evaluation studies.

Abstract. Inverse modeling of anthropogenic and biospheric CO2 fluxes from ground-based and satellite observations critically depends on the accuracy of atmospheric transport simulations. Previous studies emphasized the impact of errors in simulated winds and vertical mixing in the planetary boundary layer, whereas the potential importance of releasing emissions not only at the surface but distributing them in the vertical was largely neglected. Accounting for elevated emissions may be critical, since more than 50 % of CO2 in Europe is emitted by large point sources such as power plants and industrial facilities. In this study, we conduct high-resolution atmospheric simulations of CO2 with the mesoscale Consortium for Small-scale Modeling model extended with a module for the simulation of greenhouse gases (COSMO-GHG) over a domain covering the city of Berlin and several coal-fired power plants in eastern Germany, Poland and Czech Republic. By including separate tracers for anthropogenic CO2 emitted only at the surface or according to realistic, source-dependent profiles, we find that releasing CO2 only at the surface overestimates near-surface CO2 concentrations in the afternoon on average by 14 % in summer and 43 % in winter over the selected model domain. Differences in column-averaged dry air mole XCO2 fractions are smaller, between 5 % in winter and 8 % in summer, suggesting smaller yet non-negligible sensitivities for inversion modeling studies assimilating satellite rather than surface observations. The results suggest that the traditional approach of emitting CO2 only at the surface is problematic and that a proper allocation of emissions in the vertical deserves as much attention as an accurate simulation of atmospheric transport.

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 <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 (<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.

Abstract. The recent increase in spatial resolution for satellite instruments has made it feasible to study distributions of trace gas column densities on a regional scale. For this application a new gridding algorithm was developed to map measurements from the instrument's frame of reference (level 2) onto a longitude-latitude grid (level 3). The algorithm is designed for the Ozone Monitoring Instrument (OMI) and can easily be employed for similar instruments -for example, the upcoming TROPOspheric Monitoring Instrument (TROPOMI). Trace gas distributions are reconstructed by a continuous parabolic spline surface. The algorithm explicitly considers the spatially varying sensitivity of the sensor resulting from the instrument function. At the swath edge, the inverse problem of computing the spline coefficients is very sensitive to measurement errors and is regularised by a second-order difference matrix. Since this regularisation corresponds to the penalty term for smoothing splines, it similarly attenuates the effect of measurement noise over the entire swath width. Monte Carlo simulations are conducted to study the performance of the algorithm for different distributions of trace gas column densities. The optimal weight of the penalty term is found to be proportional to the measurement uncertainty and the width of the instrument function. A comparison with an established gridding algorithm shows improved performance for small to moderate measurement errors due to better parametrisation of the distribution. The resulting maps are smoother and extreme values are more accurately reconstructed. The performance improvement is further illustrated with high-resolution distributions obtained from a regional chemistry model. The new algorithm is applied to tropospheric NO 2 column densities measured by OMI. Examples of regional NO 2 maps are shown for densely populated areas in China, Europe and the United States of America. This work demonstrates that the newly developed gridding algorithm improves regional trace gas maps; its application could be very helpful for the study of satellite-derived trace gas distributions.

Abstract. In this study we present the first long term measurements of atmospheric nitrogen dioxide (NO 2 ) using a LED based Long Path Differential Optical Absorption Spectroscopy (LP-DOAS) instrument. This instrument is measuring continuously in Hong Kong since December 2009, first in a setup with a 550 m absorption path and then with a 3820 m path at about 30 m to 50 m above street level. The instrument is using a high power blue light LED with peak intensity at 450 nm coupled into the telescope using a Y-fibre bundle. The LP-DOAS instrument measures NO 2 levels in the Kowloon Tong and Mongkok district of Hong Kong and we compare the measurement results to mixing ratios reported by monitoring stations operated by the Hong Kong Environmental Protection Department in that area. Hourly averages of coinciding measurements are in reasonable agreement (R = 0.74). Furthermore, we used the long-term data set to validate the Ozone Monitoring Instrument (OMI) NO 2 data product. Monthly averaged LP-DOAS and OMI measurements correlate well (R = 0.84) when comparing the data for the OMI overpass time. We analyzed weekly patterns in both data sets and found that the LP-DOAS detects a clear weekly cycle with a reduction on weekends during rush hour peaks, whereas OMI is not able to observe this weekly cycle due to its fix overpass time (13:30-14:30 LT -local time).

One important goal of the Copernicus CO2 monitoring (CO2M) mission is to quantify CO2 emissions of large point sources. We analyzed the feasibility of such quantifications using synthetic CO2 and NO2 observations for a constellation of CO2M satellites. Observations were generated from kilometer-scale COSMO-GHG simulations over parts of the Czech Republic, Germany and Poland. CO2 and NOX emissions of the 15 largest power plants (3.7–40.3 Mt CO2 yr−1) were quantified using a data-driven method that combines a plume detection algorithm with a mass-balance approach. CO2 and NOX emissions could be estimated from single overpasses with 39–150% and 33–116% uncertainty (10–90th percentile), respectively. NO2 observations were essential for estimating CO2 emissions as they helped detecting and constraining the shape of the plumes. The uncertainties are dominated by uncertainties in the CO2M observations (2–72%) and limitations of the mass-balance approach to quantify emissions of complex plumes (25–95%). Annual CO2 emissions could be estimated with 23–119% and 18–65% uncertainties with two and three satellites, respectively. The uncertainty in the temporal variability of emissions contributes about half to the total uncertainty. The estimated uncertainty was extrapolated to determine uncertainties for point sources globally, suggesting that two satellites would be able to quantify the emissions of up to 300 point sources with &lt;30% uncertainty, while adding a third satellite would double the number to about 600 point sources. Annual NOX emissions can be determined with better accuracy of 16–73% and 13–52% with two and three satellites, respectively. Estimating CO2 emissions from NOX emissions using a CO2:NOX emission ratio may thus seem appealing, but this approach is significantly limited by the high uncertainty in the emission ratios as determined from the same CO2M observations. The mass-balance approach studied here will be particularly useful for estimating emissions in countries where power plant emissions are not routinely monitored and reported. Further reducing the uncertainties will require the development of advanced atmospheric inversion systems for emission plumes and an improved constraint on the temporal variability of emissions using additional sources of information such as other satellite observations or energy demand statistics.

Abstract. High-resolution atmospheric transport simulations were used to investigate the potential for detecting carbon dioxide (CO2) 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 CO2 satellites with imaging capabilities. The potential for detecting plumes was studied for satellite images of CO2 alone or in combination with images of nitrogen dioxide (NO2) and carbon monoxide (CO) to investigate the added value of measurements of other gases co-emitted with CO2 that have better signal-to-noise ratios. The additional NO2 and CO images were either generated for instruments on the same CO2M satellites (2×2 km2 resolution) or for the Sentinel-5 instrument (7×7 km2) assumed to fly two hours earlier than CO2M. Realistic CO2, CO and NO2 fields were simulated at 1×1 km2 horizontal resolution with COSMO-GHG model for the year 2015, and used as input for an orbit simulator to generate synthetic observations of columns of CO2, CO and NO2 for constellations of up to six satellites. A new plume detection algorithm was applied to detect coherent structures in the images of CO2, NO2 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 CO2 instrument only 6 and 16 of these 50 plumes could be detected assuming a high (σVEG50 = 1.0 ppm) and low noise (σVEG50 = 0.5 ppm) scenario, respectively, because the CO2 signals were often too weak. A CO instrument with specifications similar to the Sentinel-5 mission performed worse than the CO2 instrument, while the number of detectable plumes could be significantly increased to about 35 plumes with an NO2 instrument. Using NO2 observations from the Sentinel-5 platform instead resulted in a significant spatial mismatch between NO2 and CO2 plumes due to the two hour time difference between Sentinel-5 and CO2M. The plumes of the coal-fired power plant Jänschwalde were easier to detect with the CO2 instrument (about 40–45 plumes per year), but again, an NO2 instrument performed significantly better (about 70 plumes). Auxiliary measurements of NO2 were thus found to greatly enhance the capability of detecting the location of CO2 plumes, which will be invaluable for the quantification of CO2 emissions from large point sources.