Nitrogen oxide (NO and NOy) measurements were performed onboard an in-service aircraft within the framework of CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container). A total of 330 flights were completed from May 2005 through April 2013 between Frankfurt/Germany and destination airports in Canada, the USA, Brazil, Venezuela, Chile, Argentina, Colombia, South Africa, China, South Korea, Japan, India, Thailand, and the Philippines. Different regions show differing NO and NOy mixing ratios. In the mid-latitudes, observed NOy and NO generally shows clear seasonal cycles in the upper troposphere with a maximum in summer and a minimum in winter. Mean NOy mixing ratios vary between 1.36 nmol/mol in summer and 0.27 nmol/mol in winter. Mean NO mixing ratios range between 0.05 nmol/mol and 0.22 nmol/mol. Regions south of 40°N show no consistent seasonal dependence. Based on CO observations, low, median and high CO air masses were defined. According to this classification, more data was obtained in high CO air masses in the regions south of 40°N compared to the midlatitudes. This indicates that boundary layer emissions are more important in these regions. In general, NOy mixing ratios are highest when measured in high CO air masses. This dataset is one of the most comprehensive NO and NOy dataset available today for the upper troposphere and is therefore highly suitable for the validation of atmosphere-chemistry-models

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.

In this paper we present EMO-5 (“European Meteorological Observations”, spatial resolution of 5 km), a European high-resolution, (sub-)daily, multi-variable meteorological dataset built on historical and real-time observations obtained by integrating data from 18 964 ground weather stations, four high-resolution regional observational grids (i.e. CombiPrecip, ZAMG – INCA, EURO4M-APGD, and CarpatClim), and one global reanalysis (ERA-Interim/Land). EMO-5 includes the following at daily resolution: total precipitation, temperatures (minimum and maximum), wind speed, solar radiation, and water vapour pressure. In addition, EMO-5 also makes available 6-hourly precipitation and mean temperature data. The raw observations from the ground weather stations underwent a set of quality controls before SPHEREMAP and Yamamoto interpolation methods were applied in order to estimate for each 5×5 km grid cell the variable value and its affiliated uncertainty, respectively. The quality of the EMO-5 precipitation data was evaluated through (1) comparison with two regional high-resolution datasets (i.e. seNorge2 and seNorge2018), (2) analysis of 15 heavy precipitation events, and (3) examination of the interpolation uncertainty. Results show that EMO-5 successfully captured 80 % of the heavy precipitation events, and that it is of comparable quality to a regional high-resolution dataset. The availability of the uncertainty fields increases the transparency of the dataset and hence the possible usage. EMO-5 (version 1) covers the time period from 1990 to 2019, with a near real-time release of the latest gridded observations foreseen with version 2. As a product of Copernicus, the EU's Earth Observation Programme, the EMO-5 dataset is free and open, and can be accessed at https://doi.org/10.2905/0BD84BE4-CEC8-4180-97A6-8B3ADAAC4D26 (Thiemig et al., 2020).

Large volcanic eruptions impact significantly on climate and lead to ozone depletion due to injection of particles and gases into the stratosphere where their residence times are long. In this the composition of volcanic aerosol is an important but inadequately studied factor. Samples of volcanically influenced aerosol were collected following the Kasatochi (Alaska), Sarychev (Russia) and also during the Eyjafjallajökull (Iceland) eruptions in the period 2008–2010. Sampling was conducted by the CARIBIC platform during regular flights at an altitude of 10–12 km as well as during dedicated flights through the volcanic clouds from the eruption of Eyjafjallajökull in spring 2010. Elemental concentrations of the collected aerosol were obtained by accelerator-based analysis. Aerosol from the Eyjafjallajökull volcanic clouds was identified by high concentrations of sulphur and elements pointing to crustal origin, and confirmed by trajectory analysis. Signatures of volcanic influence were also used to detect volcanic aerosol in stratospheric samples collected following the Sarychev and Kasatochi eruptions. In total it was possible to identify 17 relevant samples collected between 1 and more than 100 days following the eruptions studied. The volcanically influenced aerosol mainly consisted of ash, sulphate and included a carbonaceous component. Samples collected in the volcanic cloud from Eyjafjallajökull were dominated by the ash and sulphate component (∼45% each) while samples collected in the tropopause region and LMS mainly consisted of sulphate (50–77%) and carbon (21–43%). These fractions were increasing/decreasing with the age of the aerosol. Because of the long observation period, it was possible to analyze the evolution of the relationship between the ash and sulphate components of the volcanic aerosol. From this analysis the residence time (1/e) of sulphur dioxide in the studied volcanic cloud was estimated to be 45 ± 22 days.

We compare in situ measurements of ozone (O₃) and carbon monoxide (CO) profiles from the CARIBIC program with the results from the regional chemistry transport model (WRF-Chem) to investigate the role of local and regional emissions and long-range transport over southern India during the summer monsoon of 2008. WRF-Chem successfully reproduces the general features of O₃ and CO distributions over the South Asian region. However, absolute CO concentrations in the lower troposphere are typically underestimated. Here we investigate the influence of local relative to remote emissions through sensitivity simulations. The influence of 50 % increased CO emissions over South Asia leads to a significant enhancement (upto 20 % in July) in upper tropospheric CO in the northern and central Indian regions. Over Chennai in southern India, this causes a 33 % increase in surface CO during June. However, the influence of enhanced local and regional emissions is found to be smaller (5 %) in the free troposphere over Chennai, except during September. Local to regional emissions are therefore suggested to play a minor role in the underestimation of CO by WRF-Chem during June–August. In the lower troposphere, a high pollution (O₃: 146.4 ± 12.8, CO: 136.4 ± 12.2 nmol mol⁻¹) event (15 July 2008), not reproduced by the model, is shown to be due to transport of photochemically processed air masses from the boundary layer in southern India. A sensitivity simulation combined with backward trajectories indicates that long-range transport of CO to southern India is significantly underestimated, particularly in air masses from the west, i.e., from Central Africa. This study highlights the need for more aircraft-based measurements over India and adjacent regions and the improvement of global emission inventories.