ALBERT

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: We present an analysis of SO2 column densities derived from GOME-2 satellite measurements for the Kīlauea volcano (Hawai`i) for 2007–2012. During a period of enhanced degassing activity in March–November 2008, monthly mean SO2 emission rates and effective SO2 lifetimes are determined simultaneously from the observed downwind plume evolution and meteorological wind fields, without further model input. Kīlauea is particularly suited for quantitative investigations from satellite observations owing to the absence of interfering sources, the clearly defined downwind plumes caused by steady trade winds, and generally low cloud fractions. For March–November 2008, the effective SO2 lifetime is 1–2 days, and Kīlauea SO2 emission rates are 9–21 kt day−1, which is about 3 times higher than initially reported from ground-based monitoring systems.

Description: The satellite instruments Optical Transient Detector (OTD) and Lightning Imaging Sensor (LIS) provide unique empirical data about the frequency of lightning flashes around the globe (OTD), and the tropics (LIS), which have been used before to compile a well received global climatology of flash rate densities. Here we present a statistical analysis of various additional lightning properties derived from OTD/LIS, i.e. the number of so-called "events" and "groups" per flash, as well as the mean flash duration, footprint and radiance. These normalized quantities, which can be associated with the flash "strength", show consistent spatial patterns; most strikingly, oceanic flashes show higher values than continental flashes for all properties. Over land, regions with high (Eastern US) and low (India) flash strength can be clearly identified. We discuss possible causes and implications of the observed regional differences. Although a direct quantitative interpretation of the investigated flash properties is difficult, the observed spatial patterns provide valuable information for the interpretation and application of climatological flash rates. Due to the systematic regional variations of physical flash characteristics, viewing conditions, and/or measurement sensitivities, parametrisations of lightning NOx based on total flash rate densities alone are probably affected by regional biases.

Description: The satellite instruments Optical Transient Detector (OTD) and Lightning Imaging Sensor (LIS) provide unique empirical data about the frequency of lightning flashes around the globe (OTD), and the tropics (LIS), which have been used before to compile a well-received global climatology of flash rate densities. Here we present a statistical analysis of various additional lightning properties derived from OTD / LIS, i.e., the number of so-called "events" and "groups" per flash, as well as the mean flash duration, footprint and radiance. These normalized quantities, which can be associated with the flash "strength", show consistent spatial patterns; most strikingly, oceanic flashes show higher values than continental flashes for all properties. Over land, regions with high (eastern US) and low (India) flash strength can be clearly identified. We discuss possible causes for and implications of the observed regional differences. Although a direct quantitative interpretation of the investigated flash properties is difficult, the observed spatial patterns provide valuable information for the interpretation and application of climatological flash rates. Due to the systematic regional variations of physical flash characteristics, viewing conditions, and/or measurement sensitivities, parametrizations of lightning NOx based on total flash rate densities alone are probably affected by regional biases.

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 sulphate aerosols could be detected for several months following the eruption. It is generally assumed that the formation of sulphate aerosols in the stratosphere takes about a month, but in plumes from explosive eruptions significant amounts of aerosols have been seen to form within a few hours. We show that sulphate 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 sulphate 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: We report on MAX-DOAS observations of NO2 over an oasis-ecotone-desert ecosystem in NW-China. There, local ambient NO2 concentrations originate from enhanced biogenic NO emission of intensively managed soils. Our target oasis "Milan" is located at the southern edge of the Taklimakan desert, very remote and well isolated from other potential anthropogenic and biogenic NOx sources. Four observation sites for MAX-DOAS measurements were selected, at the oasis center, downwind and upwind of the oasis, and in the desert. Biogenic NO emissions in terms of (i) soil moisture and (ii) soil temperature of Milan oasis' (iii) different land-cover type sub-units (cotton, Jujube trees, cotton/Jujube mixture, desert) were quantified by laboratory incubation of corresponding soil samples. Net potential NO fluxes were up-scaled to oasis scale by areal distribution and classification of land-cover types derived from satellite images using GIS techniques. A Lagrangian dispersion model (LASAT, Lagrangian Simulation of Aerosol-Transport) was used to calculate the dispersion of soil emitted NO into the atmospheric boundary layer over Milan oasis. Three dimensional NO concentrations (30 m horizontal resolution) have been converted to 3-D NO2 concentrations, assuming photostationary state conditions. NO2 column densities were simulated by suitable vertical integration of modeled 3-D NO2 concentrations at those downwind and upwind locations, where the MAX-DOAS measurements were performed. Downwind-upwind differences (a direct measure of Milan oasis' contribution to the areal increase of ambient NO2 concentration) of measured and simulated slant (as well as vertical) NO2 column densities show excellent agreement. This agreement is considered as the first successful attempt to prove the validity of the chosen approach to up-scale laboratory derived biogenic NO fluxes to ecosystem field conditions, i.e. from the spatial scale of a soil sample (cm2) to the size of an entire agricultural ecosystem (km2).

Description: We apply a novel experimental procedure for the rapid measurement of the average volume mixing ratios (VMRs) and horizontal distributions of trace gases such as NO2, SO2, and HCHO in the boundary layer, which was recently suggested by Sinreich et al. (2013). The method is based on two-dimensional scanning multi-axis differential optical absorption spectroscopy (MAX-DOAS). It makes use of two facts (Sinreich et al., 2013): first, the light path for observations at 1° elevation angle traverses mainly air masses located close to the ground (typically 〈 200 m); second, the light path length can be calculated using the simultaneous measured absorption of the oxygen dimer O4. Thus, the average value of the trace gas VMR in the atmospheric layer between the surface and the particular altitude, for which this observation was sensitive, can be calculated. Compared to the originally proposed method, we introduce several important modifications and improvements: We apply the method only to measurements at 1° elevation angle (besides zenith view), for which the uncertainties of the retrieved values of the VMRs and surface extinctions are especially small. Using only 1° elevation angle for off-axis observation also allows an increased temporal resolution. We determine (and apply) correction factors (and their uncertainties) directly as function of the measured O4 absorption. Finally, the method is extended to trace gases analysed at other wavelengths and also to the retrieval of aerosol extinction. Depending on atmospheric visibility, the typical uncertainty of the results ranges from about 20% to 30%. We apply the rapid method to observations of a newly-developed ground-based multifunctional passive differential optical absorption spectroscopy (GM-DOAS) instrument in the north-west outskirts near Hefei in China. We report NO2, SO2, and HCHO VMRs and aerosol extinction for four azimuth angles and compare these results with those from simultaneous long-path DOAS observations. Good agreement is found (squares of the correlation coefficients for NO2, SO2, and HCHO were 0.92, 0.85, and 0.60, respectively), verifying the reliability of this novel method. Similar agreement is found for the comparison of the aerosol extinction with results from visibility meters. Future studies may conduct measurements using a larger number of azimuth angles to increase the spatial resolution.

Description: Multi-axis differential optical absorption spectroscopy (MAX-DOAS) observations of aerosols and trace gases can be strongly influenced by clouds. Thus, it is important to identify clouds and characterise their properties. In this study we investigate the effects of clouds on several quantities which can be derived from MAX-DOAS observations, like radiance, the colour index (radiance ratio at two selected wavelengths), the absorption of the oxygen dimer O4 and the fraction of inelastically scattered light (Ring effect). To identify clouds, these quantities can be either compared to their corresponding clear-sky reference values, or their dependencies on time or viewing direction can be analysed. From the investigation of the temporal variability the influence of clouds can be identified even for individual measurements. Based on our investigations we developed a cloud classification scheme, which can be applied in a flexible way to MAX-DOAS or zenith DOAS observations: in its simplest version, zenith observations of the colour index are used to identify the presence of clouds (or high aerosol load). In more sophisticated versions, other quantities and viewing directions are also considered, which allows subclassifications like, e.g., thin or thick clouds, or fog. We applied our cloud classification scheme to MAX-DOAS observations during the Cabauw intercomparison campaign of Nitrogen Dioxide measuring instruments (CINDI) campaign in the Netherlands in summer 2009 and found very good agreement with sky images taken from the ground and backscatter profiles from a lidar.

Description: Water vapour plays a dominant role in the climate change debate. However, observing water vapour over a climatological time period in a consistent and homogeneous manner is challenging. On one hand, networks of ground-based instruments able to retrieve homogeneous integrated water vapour (IWV) data sets are being set up. Typical examples are Global Navigation Satellite System (GNSS) observation networks such as the International GNSS Service (IGS), with continuous GPS (Global Positioning System) observations spanning over the last 15+ years, and the AErosol RObotic NETwork (AERONET), providing long-term observations performed with standardized and well-calibrated sun photometers. On the other hand, satellite-based measurements of IWV already have a time span of over 10 years (e.g. AIRS) or are being merged to create long-term time series (e.g. GOME, SCIAMACHY, and GOME-2). This study performs an intercomparison of IWV measurements from satellite devices (in the visible, GOME/SCIAMACHY/GOME-2, and in the thermal infrared, AIRS), in situ measurements (radiosondes) and ground-based instruments (GPS, sun photometer), to assess their use in water vapour trends analysis. To this end, we selected 28 sites world-wide for which GPS observations can directly be compared with coincident satellite IWV observations, together with sun photometer and/or radiosonde measurements. The mean biases of the different techniques compared to the GPS estimates vary only between −0.3 to 0.5 mm of IWV. Nevertheless these small biases are accompanied by large standard deviations (SD), especially for the satellite instruments. In particular, we analysed the impact of clouds on the IWV agreement. The influence of specific issues for each instrument on the intercomparison is also investigated (e.g. the distance between the satellite ground pixel centre and the co-located ground-based station, the satellite scan angle, daytime/nighttime differences). Furthermore, we checked if the properties of the IWV scatter plots between these different instruments are dependent on the geography and/or altitude of the station. For all considered instruments, the only dependency clearly detected is with latitude: the SD of the IWV observations with respect to the GPS IWV retrievals decreases with increasing latitude and decreasing mean IWV.

Description: The chemistry in large thunderstorm clouds is influenced by local lightning-NOx production and uplift of boundary layer air. Under these circumstances trace gases like nitrous acid (HONO) or formaldehyde (HCHO) are expected to be formed or to reach the tropopause region. However, up to now only few observations of HONO at this altitude have been reported. Here we report on a case study where enhancements in HONO, HCHO and nitrogen oxides (NOx) were observed by the CARIBIC flying laboratory (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container). The event took place in a convective system over the Caribbean Sea in August 2011. Inside the cloud the light path reaches up to 100 km. Therefore the DOAS instrument on CARIBIC was very sensitive to the tracers inside the cloud. Based on the enhanced slant column densities of HONO, HCHO and NO2, average mixing ratios of 37, 468 and 210 ppt, respectively, were calculated. These data represent averages for constant mixing ratios inside the cloud. However, a large dependency on the assumed profile is found; for HONO a mixing ratio of 160 ppt is retrieved if the total amount is assumed to be situated in the uppermost 2 km of the cloud. The NO in situ instrument measured peaks up to 5 ppb NO inside the cloud; the background in the cloud was about 1.3 ppb, and hence clearly above the average outside the cloud (≈ 150 ppt). The high variability and the fact that the enhancements were observed over a pristine marine area led to the conclusion that, in all likelihood, the high NO concentrations were caused by lighting. This assumption is supported by the number of flashes that the World Wide Lightning Location Network (WWLLN) counted in this area before and during the overpass. The chemical box model CAABA is used to estimate the NO and HCHO source strengths which are necessary to explain our measurements. For NO a source strength of 10 × 109 molec cm−2 s−1 km−1 is found, which corresponds to the lightning activity as observed by the World Wide Lightning Location network, and lightning emissions of 5 × 1025 NO molec flash−1 (2.3–6.4 × 1025). The uncertainties are determined by a change of the input parameters in the box model, the cloud top height and the flash density. The emission rate per flash is scaled up to a global scale and 1.9 (1.4–2.5) tg N a−1 is estimated. The HCHO updraught is of the order of 120 × 109 molec cm−2 s−1 km−1. Also isoprene and CH3OOH as possible HCHO sources are discussed.