ALBERT

Description: The ash cloud of the Eyjafjallajökull1 volcano on Iceland caused closure of large parts of European airspace in April and May 2010. For the validation and improvement of the European volcanic ash forecast models several research flights were performed. Also the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) flying laboratory, which routinely measures at cruise altitude (≈11 km) performed three dedicated measurements flights through sections of the ash plume. Although the focus of these flights was on the detection and quantification of the volcanic ash, we report here on sulphur dioxide (SO2) and bromine monoxide (BrO) measurements with the CARIBIC DOAS (Differential Optical Absorption Spectroscopy) instrument during the second of these special flights on 16 May 2010. As the BrO and the SO2 observations coincide, we assume the BrO to have been formed inside the volcanic plume. Both SO2 and BrO observations agree well with simultaneous satellite (GOME-2) observations. SO2 column densities retrieved from satellite observations are often used as an indicator for volcanic ash. For SO2 some additional information on the local distribution can be derived from a~comparison of forward and back scan GOME-2 data. More details on the local plume size and position are retrieved by combining CARIBIC and GOME-2 data. 1Also referred to as: Eyjafjalla (e.g. Schumann et al., 2010), Eyjafjöll or Eyjafjoll (e.g. Ansmann et al., 2010).

Description: The UV Aerosol Indices (UVAI) form one of very few available tools in satellite remote sensing that provide information on aerosol absorption. The UVAI are also quite insensitive to surface type and are determined in the presence of clouds – situations where most aerosol retrieval algorithms do not work. The UVAI are most sensitive to elevated layers of absorbing aerosols, such as mineral dust and smoke from biomass burning, but they can also be used to study non-absorbing aerosols, such as sulphate and secondary organic aerosols. Although UVAI are determined for cloud-contaminated pixels, clouds do affect the value of UVAI in several ways. One way to correct for these effects is to remove clouded pixels using a cloud filter. However, this causes a large loss of data, biases the results towards clear skies, and removes all potentially very interesting pixels where aerosols and clouds co-exist. We here propose to correct the effects of clouds on UVAI in a more sophisticated way, namely by simulating the contribution of clouds to UVAI, and then subtracting it from the measured data. To this aim, we modelled UVAI from clouds by using measured cloud optical parameters – either with low spatial resolution from SCIAMACHY, or high resolution from MERIS – as input. The modelled UVAI were compared with UVAI measured by SCIAMACHY on different spatial (local, regional and global) and temporal scales (single measurement, daily means and seasonal means). The general dependencies of UVAI on cloud parameters were quite well reproduced, but several issues remain unclear: compared to the modelled UVAI, measured UVAI show a bias, in particular for large cloud fractions, and much larger scatter. Also, the viewing angle dependence differs for measured and modelled UVAI. The modelled UVAI from clouds will be used to correct measured UVAI for the effect of clouds, thus allowing a more quantitative analysis of UVAI and enabling investigations of aerosol-cloud interactions.

Description: The ash cloud of the Eyjafjallajökull (also referred to as: Eyjafjalla (e.g. Schumann et al., 2011), Eyjafjöll or Eyjafjoll (e.g. Ansmann et al., 2010)) volcano on Iceland caused closure of large parts of European airspace in April and May 2010. For the validation and improvement of the European volcanic ash forecast models several research flights were performed. Also the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) flying laboratory, which routinely measures at cruise altitude (≈11 km) performed three dedicated measurements flights through sections of the ash plume. Although the focus of these flights was on the detection and quantification of the volcanic ash, we report here on sulphur dioxide (SO2) and bromine monoxide (BrO) measurements with the CARIBIC DOAS (Differential Optical Absorption Spectroscopy) instrument during the second of these special flights on 16 May 2010. As the BrO and the SO2 observations coincide, we assume the BrO to have been formed inside the volcanic plume. Average SO2 and BrO mixing ratios of ≈40 ppb and ≈5 ppt respectively are retrieved inside the plume. The BrO to SO2 ratio retrieved from the CARIBIC observation is ≈1.3×10−4. Both SO2 and BrO observations agree well with simultaneous satellite (GOME-2) observations. SO2 column densities retrieved from satellite observations are often used as an indicator for volcanic ash. As the CARIBIC O4 column densities changed rapidly during the plume observation, we conclude that the aerosol and the SO2 plume are collocated. For SO2 some additional information on the local distribution can be derived from a comparison of forward and back scan GOME-2 data. More details on the local plume size and position are retrieved by combining CARIBIC and GOME-2 data.

Description: Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed in a rural location of southwestern Ontario during the Border Air Quality and Meteorology Study. Slant column densities (SCDs) of NO2 and O4 were determined using the standard DOAS technique. Using a radiative transfer model and the O4 SCDs, aerosol optical depths were determined for clear sky conditions and compared to OMI, MODIS, AERONET, and local PM2.5 measurements. This aerosol information was input to a radiative transfer model to calculate NO2 air mass factors, which were fit to the measured NO2 SCDs to determine tropospheric vertical column densities (VCDs) of NO2. The method of determining NO2 VCDs in this way was validated for the first time by comparison to composite VCDs derived from aircraft and ground-based measurements of NO2. The new VCDs were compared to VCDs of NO2 determined via retrievals from the satellite instruments SCIAMACHY and OMI, for overlapping time periods. The satellite-derived VCDs were higher, with a mean bias of +0.5–0.9×1015 molec cm−2. This last finding is different from previous studies whereby MAX-DOAS geometric VCDs were higher than satellite determinations, albeit for urban areas with higher VCDs. An effective boundary layer height, BLHeff, is defined as the ratio of the tropospheric VCD and the ground level concentration of NO2. Variations of BLHeff can be linked to time of day, source region, stability of the atmosphere, and the presence or absence of elevated NOx sources. In particular, a case study is shown where a high VCD and BLHeff were observed when an elevated industrial plume of NOx and SO2 was fumigated to the surface as a lake breeze impacted the measurement site. High BLHeff values (~1.9 km) were observed during a regional smog event when high winds from the SW and high convection promoted mixing throughout the boundary layer. During this event, the regional line flux of NO2 through the region was estimated to be greater than 112 kg NO2 km−1 h−1.

Description: The eruption of the Nabro volcano (Eritrea), which started on 12 June 2011, caused the introduction of large quantities of SO2 into the lower stratosphere. The subsequently formed sulfate aerosols could be detected for several months following the eruption. It is generally assumed that the formation of sulfate aerosols in the stratosphere is a relatively slow process, but in plumes from explosive eruptions significant amounts of aerosols have been seen to form within a few hours. We show that sulfate aerosols were present in the lower stratosphere within hours of the onset of the eruption of Nabro. Evidence comes from nadir UV Aerosol Index (UVAI) and SO2 measurements by SCIAMACHY, GOME-2 and OMI, and limb aerosol measurements by SCIAMACHY. The sulfate plume displays negative UVAI in the western part of OMI's swath and positive UVAI in the eastern part – an effect that is due to the strong viewing angle dependence of UVAI and can only be caused by a high-altitude (〉11 km), non-absorbing (single-scattering albedo 〉0.97) aerosol plume. For the retrieval of the aerosol profile from limb measurements, the horizontal dimensions and the position of the aerosol plume need to be taken into account, otherwise both extinction and layer height may be underestimated appreciably. By combining nadir SO2 column density and UVAI with limb aerosol profiles, a stratospheric plume from Nabro could be tracked from 13 to 17 June, before the plumes from later, lower-altitude explosions started interfering with the signal. Our findings are in agreement with ground-based lidar and sun-photometer data from an MPLNET/AERONET station in Israel and with data from the satellite-borne CALIOP lidar.

Description: Limb measurements provided by the Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) on the ENVISAT satellite allow retrieving stratospheric profiles of various trace gases on a global scale. Combining measurements of the same air volume from different viewing positions along the orbit, a tomographic approach can be applied and 2-D distribution fields of stratospheric trace gases can be acquired in one inversion. With this approach, it is possible to improve the accounting for the effect of horizontal gradients in the trace gas distribution on the profile retrieval. This was shown in a previous study for the retrieval of NO2 and OClO profiles in the Arctic region near the polar vortex boundary. In this study, the tomographic retrieval is applied on measurements during special limb-only orbits performed on 14 December 2008. For these orbits the distance between consecutive limb scanning sequences was reduced to ~3.3° of the orbital circle (i.e. more than two times with respect to the nominal operational mode). Thus, the same air volumes are scanned successively by more than one scanning sequence also for midlatitudes and the tropics. It is found that the profiles obtained by the tomographic 2-D approach show significant differences to those obtained by the 1-D approach. In particular, for regions close to stratospheric transport barriers (i.e. near to the edge of the polar vortex and subtropical transport barrier) up to 50% larger or smaller NO2 number densities (depending on the sign of the gradient along the line of sight) for altitudes below the peak of the profile (around 20 km) are obtained. The limb-only measurements allow examining the systematic error if the horizontal gradient is not accounted for, and studying the impact of the gradient strength on the profile retrieval on a global scale. The findings for the actual SCIAMACHY observations are verified by sensitivity studies for simulated data for which the NO2 distributions to be retrieved are known in advance. In addition, the impact of the horizontal distance between consecutive limb scanning sequences on the quality of the tomographic 2-D retrieval is investigated and a possibility to take into account the horizontal gradients by an interpolation approach is studied.

Description: Lightning is an important source of NOx in the free troposphere, especially in the tropics, with strong impact on ozone production. However, estimates of lightning NOx (LNOx) production efficiency (LNOx per flash) are still quite uncertain. In this study we present a systematic analysis of NO2 column densities from SCIAMACHY measurements over active thunderstorms, as detected by the World-Wide Lightning Location Network (WWLLN), where the WWLLN detection efficiency was estimated using the flash climatology of the satellite lightning sensors LIS/OTD. Only events with high lightning activity are considered, where corrected WWLLN flash rate densities inside the satellite pixel within the last hour are above 1 /km2/h. For typical SCIAMACHY ground pixels of 30 × 60 km2, this threshold corresponds to 1800 flashes over the last hour, which, for literature estimates of lightning NOx production, should result in clearly enhanced NO2 column densities. From 2004–2008, we find 287 coincidences of SCIAMACHY measurements and high WWLLN flash rate densities. For some of these events, a clear enhancement of column densities of NO2 could be observed, indeed. But overall, the measured column densities are below the expected values by more than one order of magnitude, and in most of the cases, no enhanced NO2 could be found at all. Our results are in contradiction to the currently accepted range of LNOx production per flash of 15 (2–40)×1025 molec/flash. This probably partly results from the specific conditions for the events under investigation, i.e. events of high lightning activity in the morning (local time) and mostly (for 162 out of 287 events) over ocean. Within the detected coincidences, the highest NO2 column densities were observed around the US Eastcoast. This might be partly due to interference with ground sources of NOx being uplifted by the convective systems. However, it could also indicate that flashes in this region are particularly productive. We conclude that current estimates of LNOx production might be biased high for two reasons. First, we observe a high variability of NO2 for coincident lightning events. This high variability can easily cause a publication bias, since studies reporting on high NOx production have likely been published, while studies finding no or low amounts of NOx might have been rejected as errorneous or not significant. Second, many estimates of LNOx production in literature have been performed over the US, which is probably not representative for global lightning.

Description: The UV Aerosol Indices (UVAI) form one of very few available tools in satellite remote sensing that provide information on aerosol absorption. The UVAI are also quite insensitive to surface type and are determined in the presence of clouds – situations where most aerosol retrieval algorithms do not work. The UVAI are most sensitive to elevated layers of absorbing aerosols, such as mineral dust and smoke, but they can also be used to study non-absorbing aerosols, such as sulphate and secondary organic aerosols. Although UVAI are determined for cloud-contaminated pixels, clouds do affect the value of UVAI in several ways: (1) they shield the underlying scene (potentially containing aerosols) from view, (2) they enhance the apparent surface albedo of an elevated aerosol layer, and (3) clouds unpolluted by aerosols also yield non-zero UVAI, here referred to as "cloudUVAI". The main purpose of this paper is to demonstrate that clouds can cause significant UVAI and that this cloudUVAI can be well modelled using simple assumptions on cloud properties. To this aim, we modelled cloudUVAI by using measured cloud optical parameters – either with low spatial resolution from SCIAMACHY, or high resolution from MERIS – as input. The modelled cloudUVAI were compared with UVAI determined from SCIAMACHY reflectances on different spatial (local, regional and global) and temporal scales (single measurement, daily means and seasonal means). The general dependencies of UVAI on cloud parameters were quite well reproduced, but several issues remain unclear: compared to the modelled cloudUVAI, measured UVAI show a bias, in particular for large cloud fractions. Also, the spread in measured UVAI is larger than in modelled cloudUVAI. In addition to the original, Lambert Equivalent Reflector (LER)-based UVAI algorithm, we have also investigated the effects of clouds on UVAI determined using the so-called Modified LER (MLER) algorithm (currently applied to TOMS and OMI data). For medium-sized clouds the MLER algorithm performs better (UVAI are closer to 0), but like for LER UVAI, MLER UVAI can become as large as −1.2 for small clouds and deviate significantly from zero for cloud fractions near 1. The effects of clouds should therefore also be taken into account when MLER UVAI data are used. Because the effects of clouds and aerosols on UVAI are not independent, a simple subtraction of modelled cloudUVAI from measured UVAI does not yield a UVAI representative of a cloud-free scene when aerosols are present. We here propose a first, simple approach for the correction of cloud effects on UVAI. The method is shown to work reasonably well for small to medium-sized clouds located above aerosols.

Description: Meteorological conditions may drive relationships between aerosol and cloud-related properties. It is important to account for the meteorological contribution to observed cloud–aerosol relationships in order to improve understanding of aerosol–cloud–climate interactions. A new method of investigating the contribution of meteorological covariation to observed cloud–aerosol relationships is introduced. Other studies have investigated the contribution of local meteorology to cloud–aerosol relationships. In this paper, a complimentary large-scale view is presented. Extratropical cyclones have been previously shown to affect satellite-retrieved aerosol optical depth (τ), due to enhanced emission of sea salt and sea surface brightness artefacts in regions of higher wind speed. Extratropical cyclones have also been shown to affect cloud-related properties such as cloud fraction (fc) and cloud top temperature (Ttop). Therefore, it seems plausible to hypothesise that extratropical cyclones may drive relationships between cloud-related properties and τ. In this paper, this hypothesis is investigated for extratropical cyclones, henceforth referred to as storms, over the Atlantic Ocean. MODerate resolution Imaging Spectroradiometer (MODIS) retrieved τ, fc and Ttop data are analysed using a storm-centric coordinate system centred on extratropical cyclones which have been tracked using European Centre for Medium Range Weather Forecasts (ECMWF) reanalysis 850 hPa relative vorticity data. The tracked relative vorticity (ω) is used as a measure of storm strength, while position in the storm-centric domain is used to account for storm structure. Relationships between the cloud-related properties and τ are measured by calculating regression slopes and correlations. The fc–τ relationships are positive, while the Ttop–τ relationships are negative. By shuffling the pairing of the cloud and τ data at each location in the storm-centric domain and within narrow ω bins, the contribution of storm strength and storm structure to the observed relationships can be investigated. It is found that storm strength and storm structure can explain only a small component of the relationships observed in the MODIS data. The primary causes for observed cloud–aerosol relationships are likely to be other factors such as retrieval errors, local meteorology or aerosol–cloud interactions.