BOREAS – a new MAX-DOAS profile retrieval algorithm for aerosols and trace gases

We present a new MAX-DOAS profiling algorithm for aerosols and trace gases, BOREAS, which utilizes an iterative solution method including Tikhonov regularization and the optimal estimation technique. The aerosol profile retrieval is based on a novel approach in which the absorption depth of O4 is directly used in order to retrieve extinction coefficient profiles instead of the commonly used perturbation theory method. The retrieval of trace gases is done with the frequently used optimal estimation method but significant improvements are presented on how to deal with wrongly weighted a priori constraints and for scenarios in which the a priori profile is inaccurate. Performance tests are separated into two parts. First, we address the general sensitivity of the retrieval to the example of synthetic data calculated with the radiative transfer model SCIATRAN. In the second part of the study, we demonstrate BOREAS profiling accuracy by validating the results with the help of ancillary measurements carried out during the CINDI-2 campaign in Cabauw, the Netherlands, in 2016. The synthetic sensitivity tests indicate that the regularization between measurement and a priori constraints is insufficient when knowledge of the true state of the atmosphere is poor. We demonstrate a priori pre-scaling and extensive regularization tests as a tool for the optimization of retrieved profiles. The comparison of retrieval results with in situ, ceilometer, NO2 lidar, sonde and long-path DOAS measurements during the CINDI-2 campaign always shows high correlations with coefficients greater than 0.75. The largest differences can be found in the morning hours, when the planetary boundary layer is not yet fully developed and the concentration of trace gases and aerosol, as a result of a low night-time boundary layer having formed, is focused in a shallow, near-surface layer.</p

Intercomparison of NO2, O4, O3 and HCHO slant column measurements by MAX-DOAS and zenith-sky UV¿visible spectrometers during CINDI-2

40 pags., 22 figs., 13 tabs.In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17¿d during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, the Netherlands (51.97¿¿N, 4.93¿¿E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were (1) to characterise and better understand the differences between a large number of multi-axis differential optical absorption spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, (2) to define a robust methodology for performance assessment of all participating instruments, and (3) to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen collision complex (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region, and NO2 in an additional (smaller) wavelength range in the visible region. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in a unique set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the selected reference (which is obtained from the median of either all data sets or a subset), and the rms error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the consistency between all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques.CINDI-2 received funding from the Netherlands Space Office (NSO). Funding for this study was provided by ESA through the CINDI-2 (ESA contract no. 4000118533/16/ISbo) and FRM4DOAS (ESA contract no. 4000118181/16/I-EF) projects and partly within the EU 7th Framework Programme QA4ECV project (grant agreement no. 607405). The BOKU MAX-DOAS instrument was funded and the participation of Stefan F. Schreier was supported by the Austrian Science Fund (FWF): I 2296-N29. The participation of the University of Toronto team was supported by the Canadian Space Agency (through the AVATARS project) and the Natural Sciences and Engineering Research Council (through the PAHA project). The instrument was primarily funded by the Canada Foundation for Innovation and is usually operated at the Polar Environment Atmospheric Research Laboratory (PEARL) by the Canadian Network for the Detection of Atmospheric Change (CANDAC). Funding for CISC was provided by the UVAS (“Ultraviolet and Visible Atmospheric Sounder”) projects SEOSAT/INGENIO, ESP2015-71299- R, MINECO-FEDER and UE. The activities of the IUP-Heidelberg were supported by the DFG project RAPSODI (grant no. PL 193/17-1). SAOZ and Mini-SAOZ instruments are supported by the Centre National de la Recherche Scientifique (CNRS) and the Centre National d’Etudes Spatiales (CNES). INTA recognises support from the National funding projects HELADO (CTM2013-41311-P) and AVATAR (CGL2014-55230-R). AMOIAP recognises support from the Russian Science Foundation (grant no. 16-17-10275) and the Russian Foundation for Basic Research (grant nos. 16-05- 01062 and 18-35-00682). Ka L. Chan received transnational access funding from ACTRIS-2 (H2020 grant agreement no. 654109). Rainer Volkamer recognises funding from NASA’s Atmospheric Composition Program (NASA-16-NUP2016-0001) and the US National Science Foundation (award AGS-1620530). Henning Finkenzeller is the recipient of a NASA graduate fellowship. Mihalis Vrekoussis recognises support from the University of Bremen and the DFG Research Center/Cluster of Excellence “The Ocean in the Earth System-MARUM”. Financial support through the University of Bremen Institutional Strategy in the framework of the DFG Excellence Initiative is gratefully appreciated for Anja Schönhardt. Pandora instrument deployment was supported by Luftblick through the ESA Pandonia Project and NASA Pandora Project at the Goddard Space Flight Center under NASA Headquarters’ Tropospheric Composition Program. The article processing charges for this open-access publication were covered by BK Scientific

Copernicus Cal/Val Solution - D3.1 Recommendations for R&D activities on Instrumentation Technologies

The Document identifies the gaps in instrumentation technologies for pre-flight characterisation, onboard calibration and Fiducial Reference Measurements (FRM) used for calibration and validation (Cal/Val) activities for the current Copernicus missions. It also addresses the measurement needs for future Copernicus missions and gives a prioritised list of recommendations for R&D activities on instrumentation technologies. Four types of missions are covered based on the division used in the rest of the CCVS project: optical, altimetry, radar and microwave and atmospheric composition. It also gives an overview of some promising instrumentation technologies in each measurement field for FRM that could fill the gaps for requirements not yet met for the current and future Copernicus missions and identifies the research and development (R&D) activities needed to mature these example technologies. The Document does not provide an exhaustive list of all the new technologies being developed but will give a few examples for each field to show what efforts are being made to fill the gaps. None of the examples is promoted as the best possible solutions. The selection is based on the authors' knowledge during the preparation of the Document. The information included is mainly collected from the deliverables of work packages 1 and 2 in the CCVS project. The new technologies are primarily from the interviews with various measurement networks and campaigns carried out in tasks 2.4 and 2.5. Reference documents can be found in section 1.3

DOAS measurements of NO₂ from an ultralight aircraft during the Earth Challenge expedition

We report on airborne Differential Optical Absorption Spectroscopy (DOAS) measurements of NO₂ tropospheric columns above South Asia, the Arabic peninsula, North Africa, and Italy in November and December 2009. The DOAS instrument was installed on an ultralight aircraft involved in the Earth Challenge project, an expedition of seven pilots flying on four ultralight aircraft between Australia and Belgium. The instrument recorded spectra in limb geometry with a large field of view, a set-up which provides a high sensitivity to the boundary layer NO₂ while minimizing the uncertainties related to the attitude variations. We compare our measurements with OMI (Ozone Monitoring Instrument) and GOME-2 (Global Ozone Monitoring Experiment 2) tropospheric NO₂ products when the latter are available. Above Rajasthan and the Po Valley, two areas where the NO₂ field is homogeneous, data sets agree very well. Our measurements in these areas are 0.1 &plusmn; 0.1 to 3 &plusmn; 1 &times; 10¹⁵ molec cm^&minus;2 and 2.6 &plusmn; 0.8 &times; 10¹⁶ molec cm^&minus;2, respectively. Flying downwind of Riyadh, our NO² measurements show the structure of the megacity's exhaust plume with a higher spatial resolution than OMI. Moreover, our measurements are larger (up to 40%) than those seen by satellites. We also derived tropospheric columns when no satellite data were available if it was possible to get information on the visibility from satellite measurements of aerosol optical thickness. This experiment also provides a confirmation for the recent finding of a soil signature above desert

Tropospheric nitrogen dioxide column retrieval from ground-based zenith–sky DOAS observations

We present an algorithm for retrieving tropospheric nitrogen dioxide (NO₂) vertical column densities (VCDs) from ground-based zenith–sky (ZS) measurements of scattered sunlight. The method is based on a four-step approach consisting of (1) the differential optical absorption spectroscopy (DOAS) analysis of ZS radiance spectra using a fixed reference spectrum corresponding to low NO₂ absorption, (2) the determination of the residual amount in the reference spectrum using a Langley-plot-type method, (3) the removal of the stratospheric content from the daytime total measured slant column based on stratospheric VCDs measured at sunrise and sunset, and simulation of the rapid NO₂ diurnal variation, (4) the retrieval of tropospheric VCDs by dividing the resulting tropospheric slant columns by appropriate air mass factors (AMFs). These steps are fully characterized and recommendations are given for each of them. The retrieval algorithm is applied on a ZS data set acquired with a multi-axis (MAX-) DOAS instrument during the Cabauw (51.97° N, 4.93° E, sea level) Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI) held from 10 June to 21 July 2009 in the Netherlands. A median value of 7.9 × 10¹⁵ molec cm⁻² is found for the retrieved tropospheric NO₂ VCDs, with maxima up to 6.0 × 10¹⁶ molec cm⁻². The error budget assessment indicates that the overall error &sigma;_TVCD on the column values is less than 28%. In the case of low tropospheric contribution, &sigma;_TVCD is estimated to be around 39% and is dominated by uncertainties in the determination of the residual amount in the reference spectrum. For strong tropospheric pollution events, &sigma;_TVCD drops to approximately 22% with the largest uncertainties on the determination of the stratospheric NO₂ abundance and tropospheric AMFs. The tropospheric VCD amounts derived from ZS observations are compared to VCDs retrieved from off-axis and direct-sun measurements of the same MAX-DOAS instrument as well as to data from a co-located Système d'Analyse par Observations Zénithales (SAOZ) spectrometer. The retrieved tropospheric VCDs are in good agreement with the different data sets with correlation coefficients and slopes close to or larger than 0.9. The potential of the presented ZS retrieval algorithm is further demonstrated by its successful application on a 2-year data set, acquired at the NDACC (Network for the Detection of Atmospheric Composition Change) station Observatoire de Haute Provence (OHP; Southern France)

High-resolution mapping of the NO₂ spatial distribution over Belgian urban areas based on airborne APEX remote sensing

We present retrieval results of tropospheric nitrogen dioxide (NO2) vertical column densities (VCDs), mapped at high spatial resolution over three Belgian cities, based on the DOAS analysis of Airborne Prism EXperiment (APEX) observations. APEX, developed by a Swiss-Belgian consortium on behalf of ESA (European Space Agency), is a pushbroom hyperspectral imager characterised by a high spatial resolution and high spectral performance. APEX data have been acquired under clear-sky conditions over the two largest and most heavily polluted Belgian cities, i.e. Antwerp and Brussels on 15 April and 30 June 2015. Additionally, a number of background sites have been covered for the reference spectra. The APEX instrument was mounted in a Dornier DO-228 aeroplane, operated by Deutsches Zentrum für Luft- und Raumfahrt (DLR). NO2 VCDs were retrieved from spatially aggregated radiance spectra allowing urban plumes to be resolved at the resolution of 60  ×  80 m2. The main sources in the Antwerp area appear to be related to the (petro)chemical industry while traffic-related emissions dominate in Brussels. The NO2 levels observed in Antwerp range between 3 and 35  ×  1015 molec cm−2, with a mean VCD of 17.4 ± 3.7  ×  1015 molec cm−2. In the Brussels area, smaller levels are found, ranging between 1 and 20  ×  1015 molec cm−2 and a mean VCD of 7.7 ± 2.1  ×  1015 molec cm−2. The overall errors on the retrieved NO2 VCDs are on average 21 and 28 % for the Antwerp and Brussels data sets. Low VCD retrievals are mainly limited by noise (1σ slant error), while high retrievals are mainly limited by systematic errors. Compared to coincident car mobile-DOAS measurements taken in Antwerp and Brussels, both data sets are in good agreement with correlation coefficients around 0.85 and slopes close to unity. APEX retrievals tend to be, on average, 12 and 6 % higher for Antwerp and Brussels, respectively. Results demonstrate that the NO2 distribution in an urban environment, and its fine-scale variability, can be mapped accurately with high spatial resolution and in a relatively short time frame, and the contributing emission sources can be resolved. High-resolution quantitative information about the atmospheric NO2 horizontal variability is currently rare, but can be very valuable for (air quality) studies at the urban scale

Airborne DOAS measurements in Arctic: vertical distributions of aerosol extinction coefficient and NO₂ concentration

We report on airborne Differential Optical Absorption Spectroscopy (DOAS) measurements of aerosol extinction and NO₂ tropospheric profiles performed off the North coast of Norway in April 2008. The DOAS instrument was installed on the Safire ATR-42 aircraft during the POLARCAT-France spring campaign and recorded scattered light spectra in near-limb geometry using a scanning telescope. We use O₄ slant column measurements to derive the aerosol extinction at 360 nm. Regularization is based on the maximum a posteriori solution, for which we compare a linear and a logarithmic approach. The latter inherently constrains the solution to positive values and yields aerosol extinction profiles more consistent with independently measured size distributions. We present results from two soundings performed on 8 April 2008 above 71&deg; N, 22&deg; E and on 9 April 2008 above 70&deg; N, 17.8&deg; E. The first profile shows aerosol extinction and NO₂ in the marine boundary layer with respective values of 0.04 ± 0.005 km⁻¹ and 1.9 ± 0.3 × 10⁹ molec cm⁻³. A second extinction layer of 0.01 ± 0.003 km⁻¹ is found at 4 km altitude where the NO₂ concentration is 0.32 ± 0.2 × 10⁹ molec cm⁻³. During the second sounding, clouds prevent retrieval of profile parts under 3 km altitude but a layer with enhanced extinction (0.025 ± 0.005 km⁻¹) and NO₂ (1.95 ± 0.2 × 10⁹ molec cm⁻³) is clearly detected at 4 km altitude. <br><br> From CO and ozone in-situ measurements complemented by back-trajectories, we interpret the measurements in the free troposphere as, for the first sounding, a mix between stratospheric and polluted air from Northern Europe and for the second sounding, polluted air from Central Europe containing NO₂. Considering the boundary layer measurements of the first flight, modeled source regions indicate closer sources, especially the Kola Peninsula smelters, which can explain the NO₂ enhancement not correlated with a CO increase at the same altitude

High-resolution airborne imaging DOAS-measurements of NO₂ above Bucharest during AROMAT

In this study we report on airborne imaging DOAS measurements of NO2 from two flights performed in Bucharest during the AROMAT campaign (Airborne ROmanian Meeasurements of Aerosols an Trace gases) in September 2014. These measurements were performed with the Airborne imaging Differential Optical Absorption Spectroscopy (DOAS) instrument for Measurements of Atmospheric Pollution (AirMAP) and provide nearly gapless maps of column densities of NO2 below the aircraft with a high spatial resolution of better than 100 m. The airmass factors, which are needed to convert the measured differential Slant Column Densities (dSCDs) to Vertical Column Densities (VCDs) have a strong dependence on the surface reflectance, which has to be accounted for in the retrieval. This is especially important for measurements above urban areas, where the surface properties vary strongly. As the instrument is not radiometrically calibrated, we have developed a method to derive the surface reflectance from measured intensities at the aircraft. This method is based on radiative transfer calculation with SCIATRAN and a reference area for which the surface reflectance is known. While surface properties are clearly seen in the NO2 dSCD results, this effect is successfully corrected for in the VCD results. Furthermore we investigate the influence of aerosols on the retrieval for a variety of aerosol profiles that were measured in the context of the AROMAT campaigns. The results of two research flights are presented which reveal distinct horizontal distribution patterns and strong spatial gradients of NO2 across the city. Pollution levels range from background values in the outskirts located upwind of the city to about 4 × 1016 molec cm−2 in the polluted city center. Validation against two co-located mobile car-DOAS measurements yields good agreement between the datasets with correlation cofficients of R = 0.94 and R = 0.85, respectively. Estimations on the NOx emission rate of Bucharest for the two flights yield emission rates of 15.1 ± 9.4 mol s−1 and 13.6 ± 8.4 mol s−1, respectively