ALBERT

Description: In this study, we analyse the sensitivity of nadir viewing satellite observations in the visible range to freshly produced lightning NOx, i.e. for meteorological and (photo-) chemical conditions found in and around cumulonimbus clouds. For the first time, such a study is performed accounting for photo-chemistry, dynamics, and radiative transfer in a consistent way: A one week episode in the TOGA COARE/CEPEX region (Pacific) in December 1992 is simulated with a 3-D cloud resolving chemistry model. The simulated hydrometeor mixing ratios are fed into a Monte Carlo radiative transfer model to calculate box-Air Mass Factors (box-AMFs) for NO2. From these box-AMFs, together with model NOx profiles, slant columns of NO2 (SNO2), i.e. synthetic satellite measurements, are calculated and set in relation to the actual model NOx vertical column (VNOx), yielding the "sensitivity" SNO2/VNOx. From this study, we find a mean sensitivity of 0.46. NOx below the cloud bottom is mostly present as NO2, but shielded from the satellites' view, whereas NOx at the cloud top or above is shifted to NO due to high photolysis and low temperature, and hence not detectable from space. But a significant fraction of the lightning produced NOx in the middle part of the cloud is present as NO2 and has a good visibility from space. Due to the resulting total sensitivity being quite high, nadir viewing satellites provide a valuable additional platform to quantify NOx production by lightning; strong lightning events over "clean" regions should be clearly detectable in satellite observations. Since the observed enhancement of NO2 column densities over mesoscale convective systems are lower than expected for current estimates of NOx production per flash, satellite measurements can in particular constrain the upper bound of lightning NOx production estimates.

Description: Zenith-sky scattered sunlight observations using differential optical absorption spectroscopy (DOAS) technique were carried out in Shanghai, China (31.3° N, 121.5° E) since December 2006. At this polluted urban site, the measurement provided NO2 total columns in the daytime. Here, we present a new method to extract time series of tropospheric vertical column densities (VCD) of NO2 from these observations. The derived tropospheric NO2 VCD is an important quantity for the estimation of emissions and for the validation of satellite observations. Our method makes use of assumptions on the relative NO2 height profiles and on the diurnal variation of the stratospheric NO2 VCD. The influence of these parameters on the retrieved tropospheric NO2 VCD is discussed; for a polluted site like Shanghai, the accuracy of our method is estimated to be

Description: In many investigations of tropospheric chemistry information about the two dimensional distribution of trace gases on a small scale (e.g. tens to hundreds of meters) is highly desirable. An airborne instrument based on imaging Differential Optical Absorption Spectroscopy has been built to map the 2-D distribution of a series of relevant trace gases including NO2, HCHO, C2H2O2, H2O, O4, SO2, and BrO on a scale of 100 m. Here we report on the first tests of the novel aircraft instrument over the industrialised South African Highveld, where large variations in NO2 column densities in the immediate vicinity of several sources e.g. power plants or steel works, were measured. The observed patterns in the trace gas distribution are interpreted with respect to flux estimates, and it is seen that the fine resolution of the measurements allows separate sources in close proximity to one another to be distinguished.

Description: With the increasing availability of observations from different space-borne sensors, the joint analysis of observational data from multiple sources becomes more and more attractive. For such an analysis – oftentimes with little prior knowledge about local and global interactions between the different observational variables available – an explorative data-driven analysis of the remote sensing data may be of particular relevance. In the present work we used generalized additive models (GAM) in this task, in an exemplary study of spatio-temporal patterns in the tropospheric NO2-distribution derived from GOME satellite observations (1996 to 2001) at global scale. We modelled different temporal trends in the time series of the observed NO2, but focused on identifying correlations between NO2 and local wind fields. Here, our nonparametric modelling approach had several advantages over standard parametric models: While the model-based analysis allowed to test predefined hypotheses (assuming, for example, sinusoidal seasonal trends) only, the GAM allowed to learn functional relations between different observational variables directly from the data. This was of particular interest in the present task, as little was known about relations between the observed NO2 distribution and transport processes by local wind fields, and the formulation of general functional relationships to be tested remained difficult. We found the observed temporal trends – weekly, seasonal and linear changes – to be in overall good agreement with previous studies and alternative ways of data analysis. However, NO2 observations showed to be affected by wind-dominated processes over several areas, world wide. Here we were able to estimate the extent of areas affected by specific NO2 emission sources, and to highlight likely atmospheric transport pathways. Overall, using a nonparametric model provided favourable means for a rapid inspection of this large spatio-temporal data set,with less bias than parametric approaches, and allowing to visualize dynamical processes of the NO2 distribution at a global scale.

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: International shipping is recognized as a pollution source of growing importance, in particular in the remote marine boundary layer. Nitrogen dioxide originating from ship emissions has previously been detected in satellite measurements. This study presents the first satellite measurements of formaldehyde (HCHO) linked to shipping emissions as derived from observations made by the Global Ozone Monitoring Experiment (GOME) instrument. We analyzed enhanced HCHO tropospheric columns from shipping emissions over the Indian Ocean between Sri Lanka and Sumatra. This region offers good conditions in term of plume detection with the GOME instrument as all ship tracks follow a single narrow track in the same east-west direction as used for the GOME pixel scanning. The HCHO signal alone is weak but could be clearly seen in the high-pass filtered data. The line of enhanced HCHO in the Indian Ocean as seen in the 7-year composite of cloud free GOME observations clearly coincides with the distinct ship track corridor from Sri Lanka to Indonesia. The observed mean HCHO column enhancement over this shipping route is about 2.0×1015 molec/cm2. Compared to the simultaneously observed NO2 values over the shipping route, those of HCHO are substantially higher; also the HCHO peaks are found at larger distance from the ship routes. These findings indicate that direct emissions of HCHO or degradation of emitted NMHC cannot explain the observed enhanced HCHO values. One possible reason might be increased CH4 degradation due to enhanced OH concentrations related to the ship emissions, but this source is probably too weak to fully explain the observed values. The observed HCHO pattern also agrees qualitatively well with results from the coupled earth system model ECHAM5/MESSy applied to atmospheric chemistry (EMAC). However, the modelled HCHO values over the ship corridor are two times lower than in the GOME high-pass filtered data. This might indicate uncertainties in the satellite data and used emission inventories and/or that the in-plume chemistry taking place in the narrow path of the shipping lanes are not well represented at the rather coarse model resolution.

Description: With the increasing availability of observational data from different sources at a global level, joint analysis of these data is becoming especially attractive. For such an analysis – oftentimes with little prior knowledge about local and global interactions between the different observational variables at hand – an exploratory, data-driven analysis of the data may be of particular relevance. In the present work we used generalized additive models (GAM) in an exemplary study of spatio-temporal patterns in the tropospheric NO2-distribution derived from GOME satellite observations (1996 to 2001) at global scale. We focused on identifying correlations between NO2 and local wind fields, a quantity which is of particular interest in the analysis of spatio-temporal interactions. Formulating general functional, parametric relationships between the observed NO2 distribution and local wind fields, however, is difficult – if not impossible. So, rather than following a model-based analysis testing the data for predefined hypotheses (assuming, for example, sinusoidal seasonal trends), we used a GAM with non-parametric model terms to learn this functional relationship between NO2 and wind directly from the data. The NO2 observations showed to be affected by wind-dominated processes over large areas. We estimated the extent of areas affected by specific NO2 emission sources, and were able to highlight likely atmospheric transport "pathways". General temporal trends which were also part of our model – weekly, seasonal and linear changes – showed to be in good agreement with previous studies and alternative ways of analysing the time series. Overall, using a non-parametric model provided favorable means for a rapid inspection of this large spatio-temporal NO2 data set, with less bias than parametric approaches, and allowing to visualize dynamical processes of the NO2 distribution at a global scale.

Description: In this study, we analyse the sensitivity of nadir viewing satellite observations in the visible range to freshly produced lightning NOx. This is a particular challenge due to the complex and highly variable conditions of meteorology, (photo-) chemistry, and radiative transfer in and around cumulonimbus clouds. For the first time, such a study is performed accounting for photo-chemistry, dynamics, and radiative transfer in a consistent way: A one week episode in the TOGA COARE/CEPEX region (Pacific) in December 1992 is simulated with a 3-D cloud resolving chemistry model. The simulated hydrometeor mixing ratios are fed into a Monte Carlo radiative transfer model to calculate box-Air Mass Factors (box-AMFs) for NO2. From these box-AMFs, together with model NOx profiles, slant columns of NO2 (SNO2), i.e. synthetic satellite measurements, are calculated and set in relation to the actual model NOx vertical column (VNOx), yielding the "sensitivity" SNO2/VNOx. From this study, we find a mean sensitivity of 0.46. NOx below the cloud bottom is mostly present as NO2, but shielded from the satellites' view, whereas NOx at the cloud top or above is shifted to NO due to high photolysis and low temperature, and hence not detectable from space. However, a significant fraction of the lightning produced NOx in the middle part of the cloud is present as NO2 and has a good visibility from space. Due to the resulting total sensitivity being quite high, nadir viewing satellites provide a valuable additional platform to quantify NOx production by lightning; strong lightning events over "clean" regions should be clearly detectable in satellite observations. Since the observed enhancement of NO2 column densities over mesoscale convective systems are lower than expected for current estimates of NOx production per flash, satellite measurements can in particular constrain the upper bound of lightning NOx production estimates.