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: Forest fire emissions have a strong impact on the concentrations of trace gases and aerosols in the atmosphere. In order to quantify the influence of boreal forest fire emissions on the atmospheric composition, the fire seasons of 1997 and 1998 are compared in this paper. Fire activity in 1998 was very strong, especially over Canada and Eastern Siberia, whereas it was much weaker in 1997. According to burned area estimates the burning in 1998 was more than six times as intense as in 1997. Based on hot spot locations derived from ATSR (Along Track Scanning Radiometer) data and official burned area data, fire emissions were estimated and their transport was simulated with a Lagrangian tracer transport model. Siberian and Canadian forest fire tracers were distinguished to investigate the transport of both separately. The fire emissions were transported even over intercontinental distances. Due to the El Niño induced meteorological situation, transport from Siberia to Canada was enhanced in 1998. Siberian fire emissions were transported towards Canada and contributed concentrations more than twice as high as those due to Canada's own CO emissions by fires. In 1998 both tracers arrive at higher latitudes over Europe, which is due to a higher North Atlantic Oscillation (NAO) index in 1998. The simulated emission plumes are compared to CMDL (Climate Monitoring and Diagnostics Laboratory) CO2 and CO data, Total Ozone Mapping Spectrometer (TOMS) aerosol index (AI) data and Global Ozone Monitoring Experiment (GOME) tropospheric NO2 and HCHO columns. All the data show clearly enhanced signals during the burning season of 1998 compared to 1997. The results of the model simulation are in good agreement with ground-based as well as satellite-based measurements.

Description: This paper studies the interannual variability of pollution pathways from northern hemisphere (NH) continents into the Arctic. Using a 15-year model simulation of the dispersion of passive tracers representative of anthropogenic emissions from NH continents, we show that the North Atlantic Oscillation (NAO) exerts a strong control on the pollution transport into the Arctic, particularly in winter and spring. For tracer lifetimes of 5 (30) days, surface concentrations in the Arctic winter are enhanced by about 70% (30%) during high phases of the NAO (in the following referred to as NAO+) compared to its low phases (NAO-). This is mainly due to great differences in the pathways of European pollution during NAO+ and NAO- phases, respectively, but reinforced by North American pollution, which is also enhanced in the Arctic during NAO+ phases. In contrast, Asian pollution in the Arctic does not significantly depend on the NAO phase. The model results are confirmed using remotely-sensed NO2 vertical atmospheric columns obtained from seven years of satellite measurements, which show enhanced northward NO2 transport and reduced NO2 outflow into the North Atlantic from Central Europe during NAO+ phases. Surface measurements of carbon monoxide (CO) and black carbon at high-latitude stations further corroborate the overall picture of enhanced Arctic pollution levels during NAO+ phases

Description: Intercontinental transport (ICT) of trace substances normally occurs on timescales ranging from a few days to several weeks. In this paper an extraordinary episode in November 2001 is presented, where pollution transport across the North Atlantic took only about one day. The transport mechanism, termed here an intercontinental pollution express highway because of the high wind speeds, was exceptional, as it involved an explosively generated cyclone, a so-called meteorological "bomb''. To the authors' knowledge, this is the first study describing pollution transport in a bomb. The discovery of this event was based on tracer transport model calculations and satellite measurements of NO2, a species with a relatively short lifetime in the atmosphere, which could be transported that far only because of the high wind speeds produced by the bomb. A 15-year transport climatology shows that intercontinental express highways are about four times more frequent in winter than in summer, in agreement with bomb climatologies. The climatology furthermore suggests that intercontinental express highways may be important for the budget of short-lived substances in the remote troposphere. For instance, for a substance with a lifetime of 1 day, express highways may be responsible for about two thirds of the total ICT. We roughly estimate that express highways connecting North America with Europe enhance the average NOx mixing ratios over Europe, due to North American emissions, by about 2-3 pptv in winter.

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: Absolute radiometric calibrations are important for measurements of the atmospheric spectral radiance. Such measurements can be used to determine actinic fluxes, the properties of aerosols and clouds and the short wave energy budget. Conventional calibration methods in the laboratory are based on calibrated light sources and reflectors and are expensive, time consuming and subject to relatively large uncertainties. Also, the calibrated instruments might change during transport from the laboratory to the measurement sites. Here we present a new calibration method for UV/vis instruments that measure the spectrally resolved sky radiance, like for example zenith sky Differential Optical Absorption Spectroscopy (DOAS-) instruments or Multi-AXis (MAX-) DOAS instruments. Our method is based on the comparison of the solar zenith angle dependence of the measured zenith sky radiance with radiative transfer simulations. For the application of our method clear sky measurements during periods with almost constant aerosol optical depth are needed. The radiative transfer simulations have to take polarisation into account. We show that the calibration results are almost independent from the knowledge of the aerosol optical properties and surface albedo, which causes a rather small uncertainty of about

Description: Multi-Axis-Differential Optical Absorption Spectroscopy (MAX-DOAS) observations of trace gases can be strongly influenced by clouds and aerosols. Thus it is important to identify clouds and characterise their properties. In a recent study Wagner et al. (2014) developed a cloud classification scheme based on the MAX-DOAS measurements themselves with which different "sky conditions" (e.g. clear sky, continuous clouds, broken clouds) can be distinguished. Here we apply this scheme to long term MAX-DOAS measurements from 2011 to 2013 in Wuxi, China (31.57° N, 120.31° E). The original algorithm has been modified, in particular in order to account for smaller solar zenith angles (SZA). Instrumental degradation is accounted for to avoid artificial trends of the cloud classification. We compared the results of the MAX-DOAS cloud classification scheme to several independent measurements: aerosol optical depth from a nearby AERONET station and from MODIS, visibility derived from a visibility meter; and various cloud parameters from different satellite instruments (MODIS, OMI, and GOME-2). The most important findings from these comparisons are: (1) most cases characterized as clear sky with low or high aerosol load were associated with the respective AOD ranges obtained by AERONET and MODIS, (2) the observed dependences of MAX-DOAS results on cloud optical thickness and effective cloud fraction from satellite indicate that the cloud classification scheme is sensitive to cloud (optical) properties, (3) separation of cloudy scenes by cloud pressure shows that the MAX-DOAS cloud classification scheme is also capable of detecting high clouds, (4) some clear sky conditions, especially with high aerosol load, classified from MAX-DOAS observations corresponding to the optically thin and low clouds derived by satellite observations probably indicate that the satellite cloud products contain valuable information on aerosols.