ALBERT

Description: Satellite observations from the SCIAMACHY, GOME-2 and OMI spectrometers have been used to retrieve atmospheric columns of glyoxal (CHOCHO) with the DOAS method. High CHOCHO levels were found over regions with large biogenic and pyrogenic emissions, and hot-spots have been identified over areas of anthropogenic activities. This study focuses on the development of an improved retrieval for CHOCHO from measurements by the OMI instrument. From sensitivity tests, a fitting window and a polynomial degree are determined. Two different approaches to reduce the interference of liquid water absorption over oceanic regions are evaluated, achieving significant reduction of the number of negative columns over clear water regions. The impact of using different absorption cross-sections for water vapour is evaluated and only small differences are found. Finally, a high-temperature (boundary layer ambient: 294 K) absorption cross-section of nitrogen dioxide (NO2) is introduced in the DOAS retrieval to account for potential interferences of NO2 over regions with large anthropogenic emissions, leading to improved fit quality over these areas. A comparison with vertical CHOCHO columns retrieved from GOME-2 and SCIAMACHY measurements over continental regions is performed, showing overall good consistency. However, SCIAMACHY CHOCHO columns are systematically higher than those obtained from the other instruments. Using the new OMI CHOCHO data set, the link between fires and glyoxal columns is investigated for two selected regions in Africa. In addition, mapped averages are computed for a fire event in Russia between mid-July and mid-August 2010. In both cases, enhanced CHOCHO levels are found in close spatial and temporal proximity to elevated levels of MODIS fire radiative power, demonstrating that pyrogenic emissions can be clearly identified in the new OMI CHOCHO product.

Description: Spectral effects of liquid water are present in absorption (differential optical absorption spectroscopy – DOAS) measurements above the ocean and, if insufficiently removed, may interfere with trace gas absorptions, leading to wrong results. Currently available literature cross sections of liquid water absorption are provided in coarser resolution than DOAS applications require, and vibrational Raman scattering (VRS) is mostly not considered, or is compensated for using simulated pseudo cross sections from radiative transfer modeling. During the ship-based TransBrom campaign across the western Pacific in October 2009, MAX-DOAS (Multi-AXis differential optical absorption spectroscopy) measurements of light penetrating very clear natural waters were performed, achieving average underwater light paths of up to 50 m. From these measurements, the retrieval of a correction spectrum (H2Ocorr) is presented, compensating simultaneously for insufficiencies in the liquid water absorption cross section and broad-banded VRS structures. Small-banded structures caused by VRS were found to be very efficiently compensated for by the intensity offset correction included in the DOAS fit. No interference between the H2Ocorr spectrum and phytoplankton absorption was found. In the MAX-DOAS tropospheric NO2 retrieval, this method was able to compensate entirely for all liquid water effects that decrease the fit quality, and performed better than using a liquid water cross section in combination with a simulated VRS spectrum. The decrease in the residual root mean square (rms) of the DOAS fit depends on the measurement's contamination with liquid water structures, and ranges from ≈ 30% for measurements slightly towards the water surface to several percent in small angles above the horizon. Furthermore, the H2Ocorr spectrum was found to prevent misfits of NO2 slant columns, especially for very low NO2 scenarios, and thus increases the reliability of the fit. In test fits on OMI satellite data, the H2Ocorr spectrum was found selectively above ocean surfaces, where it decreases the rms by up to ≈ 11%.

Description: Satellite observations from the SCIAMACHY, GOME-2, and OMI spectrometers have been used to retrieve atmospheric columns of glyoxal (CHOCHO) with the DOAS method. High CHOCHO levels are found over regions with large biogenic and pyrogenic emissions, and hot-spots have been identified over areas of anthropogenic activities. This study focuses on the development of an improved retrieval for CHOCHO from measurements by the OMI instrument. From sensitivity tests, an optimal fitting window and polynomial degree are determined. Two different approaches to reduce the interference of liquid water absorption over oceanic regions are evaluated, achieving significant reduction of negative columns over clear water regions. Moreover, a high temperature absorption cross-section of nitrogen dioxide (NO2) is introduced in the DOAS retrieval to account for potential interferences of NO2 over regions with large anthropogenic emissions, leading to improved fit quality over these areas. A comparison with vertical CHOCHO columns retrieved from measurements of the GOME-2 and SCIAMACHY instruments over continental regions is performed, showing overall good consistency. Using the new OMI CHOCHO data set, the link between fires and glyoxal columns is investigated for two selected regions in Africa. In addition, mapped averages are computed for a fire event in the east of Moscow between mid-July and mid-August 2010. In both cases, enhanced CHOCHO levels are found in close spatial and temporal proximity to MODIS fire radiative power, demonstrating that pyrogenic emissions can be clearly identified in the OMI CHOCHO product.

Description: It is well-known that spectral effects of liquid water are present in absorption (DOAS) measurements above the ocean and insufficiently removed liquid water structures may interfere with trace gas absorptions leading to wrong (sometimes even non-physical) results. Currently available literature cross-sections of liquid water absorption are provided in coarser resolution than hyperspectral DOAS applications require and Vibrational Raman Scattering (VRS) is mostly unconsidered or compensated for using simulated pseudo cross-sections from radiative transfer modelling. During the ship-based TransBrom campaign across the western Pacific in October 2009, MAX-DOAS measurements were performed into very clear natural waters achieving underwater light paths of up to 50 m. From these measurements, the retrieval of a residual (H2Ores) spectrum is presented compensating simultaneously for insufficiencies of the liquid water absorption cross-section and broad-banded VRS structures. Small-banded (Ring) structures caused by VRS were found to be very efficiently compensated for by the intensity offset (straylight) correction included in the DOAS fit. In the MAX-DOAS tropospheric NO2 retrieval, this method was able to compensate entirely for all liquid water effects that decrease the fit quality. This was not achieved using a liquid water cross-section in combination with a simulated VRS spectrum. Typical values of improvement depend on the measurement's contamination with liquid water structures and range from ≈ 30% for measurements slightly towards the water surface to several percent in small angles above the horizon. Furthermore, the H2Ores spectrum was found to prevent misfits of NO2 slant columns especially for very low NO2 scenarios and thus increase the reliability of the fit. In test fits on OMI satellite data, the H2Ores spectrum was found selectively above ocean surfaces where it leads to fit quality improvements of up to 6–18%.