ALBERT

Description: We perform a source attribution for tropospheric and ground-level ozone using a novel technique that accounts separately for the contributions of the two chemically distinct emitted precursors (reactive carbon and oxides of nitrogen) to the chemical production of ozone in the troposphere. By tagging anthropogenic emissions of these precursors according to the geographical region from which they are emitted, we determine source–receptor relationships for ground-level ozone. Our methodology reproduces earlier results obtained via other techniques for ozone source attribution, and it also delivers additional information about the modelled processes responsible for the intercontinental transport of ozone, which is especially strong during the spring months. The current generation of chemical transport models used to support international negotiations aimed at reducing the intercontinental transport of ozone shows especially strong inter-model differences in simulated springtime ozone. Current models also simulate a large range of different responses of surface ozone to methane, which is one of the major precursors of ground-level ozone. Using our novel source attribution technique, we show that emissions of NOx (oxides of nitrogen) from international shipping over the high seas play a disproportionately strong role in our model system regarding the hemispheric-scale response of surface ozone to changes in methane, as well as to the springtime maximum in intercontinental transport of ozone and its precursors. We recommend a renewed focus on the improvement of the representation of the chemistry of ship NOx emissions in current-generation models. We demonstrate the utility of ozone source attribution as a powerful model diagnostic tool and recommend that similar source attribution techniques become a standard part of future model intercomparison studies.

Description: We infer surface fluxes of bromoform (CHBr3) and dibromoform (CH2Br2) from aircraft observations over the western Pacific using a tagged version of the GEOS-Chem global 3-D atmospheric chemistry model and a maximum a posteriori inverse model. Using GEOS-Chem (GC) as an intermediary, we find that the distribution of a priori ocean emissions of these gases are reasonably consistent with observed atmospheric mole fractions of CHBr3 (r=0.62) and CH2Br2 (r=0.38). These a priori emissions result in a positive model bias in CHBr3 peaking in the marine boundary layer, but reproduce observed values of CH2Br2 with no significant bias by virtue of its longer atmospheric lifetime. Using GEOS-Chem, we find that observed variations in atmospheric CHBr3 are determined equally by sources over the western Pacific and those outside the study region, but observed variations in CH2Br2 are determined mainly by sources outside the western Pacific. Numerical closed-loop experiments show that the spatial and temporal distribution of boundary layer aircraft data have the potential to substantially improve current knowledge of these fluxes, with improvements related to data density. Using the aircraft data, we estimate aggregated regional fluxes of 3.6±0.3×108 and 0.7±0.1×108 g month−1 for CHBr3 and CH2Br2 over 130–155∘E and 0–12∘ N, respectively, which represent reductions of 20 %–40 % of the prior inventories by Ordóñez et al. (2012) and substantial spatial deviations from different a priori inventories. We find no evidence to support a robust linear relationship between CHBr3 and CH2Br2 oceanic emissions, as used by previous studies. We find that over regions with dense observation coverage, our choice of a priori inventory does not significantly impact our reported a posteriori flux estimates.

Description: The implementation of European emission abatement strategies has led to a significant reduction in the emissions of ozone precursors during the last decade. Ground-level ozone is also influenced by meteorological factors such as temperature, which exhibit interannual variability and are expected to change in the future. The impacts of climate change on air quality are usually investigated through air-quality models that simulate interactions between emissions, meteorology and chemistry. Within a multi-model assessment, this study aims to better understand how air-quality models represent the relationship between meteorological variables and surface ozone concentrations over Europe. A multiple linear regression (MLR) approach is applied to observed and modelled time series across 10 European regions in springtime and summertime for the period of 2000–2010 for both models and observations. Overall, the air-quality models are in better agreement with observations in summertime than in springtime and particularly in certain regions, such as France, central Europe or eastern Europe, where local meteorological variables show a strong influence on surface ozone concentrations. Larger discrepancies are found for the southern regions, such as the Balkans, the Iberian Peninsula and the Mediterranean basin, especially in springtime. We show that the air-quality models do not properly reproduce the sensitivity of surface ozone to some of the main meteorological drivers, such as maximum temperature, relative humidity and surface solar radiation. Specifically, all air-quality models show more limitations in capturing the strength of the ozone–relative-humidity relationship detected in the observed time series in most of the regions, for both seasons. Here, we speculate that dry-deposition schemes in the air-quality models might play an essential role in capturing this relationship. We further quantify the relationship between ozone and maximum temperature (mo3−T, climate penalty) in observations and air-quality models. In summertime, most of the air-quality models are able to reproduce the observed climate penalty reasonably well in certain regions such as France, central Europe and northern Italy. However, larger discrepancies are found in springtime, where air-quality models tend to overestimate the magnitude of the observed climate penalty.

Description: Methods to radiometrically calibrate a non-imaging airborne visible-to-shortwave infrared (VSWIR) spectrometer to measure the Greenland ice sheet surface are presented. Airborne VSWIR measurement performance for bright Greenland ice and dark bare rock/soil targets is compared against the MODerate resolution atmospheric TRANsmission (MODTRAN®) radiative transfer code (version 6.0), and a coincident Landsat 8 Operational Land Imager (OLI) acquisition on 29 July 2015 during an in-flight radiometric calibration experiment. Airborne remote sensing flights were carried out in northwestern Greenland in preparation for the Ice, Cloud, and land Elevation Satellite 2 (ICESat-2) laser altimeter mission. A total of nine science flights were conducted over the Greenland ice sheet, sea ice, and open-ocean water. The campaign's primary purpose was to correlate green laser pulse penetration into snow and ice with spectroscopic-derived surface properties. An experimental airborne instrument configuration that included a nadir-viewing (looking downward at the surface) non-imaging Analytical Spectral Devices (ASD) Inc. spectrometer that measured upwelling VSWIR (0.35 to 2.5 µm) spectral radiance (Wm-2sr-1µm-1) in the two-color Slope Imaging Multi-polarization Photon-Counting Lidar's (SIMPL) ground instantaneous field of view, and a zenith-viewing (looking upward at the sky) ASD spectrometer that measured VSWIR spectral irradiance (W m−2 nm−1) was flown. National Institute of Standards and Technology (NIST) traceable radiometric calibration procedures for laboratory, in-flight, and field environments are described in detail to achieve a targeted VSWIR measurement requirement of within 5 % to support calibration/validation efforts and remote sensing algorithm development. Our MODTRAN predictions for the 29 July flight line over dark and bright targets indicate that the airborne nadir-viewing spectrometer spectral radiance measurement uncertainty was between 0.6 % and 4.7 % for VSWIR wavelengths (0.4 to 2.0 µm) with atmospheric transmittance greater than 80 %. MODTRAN predictions for Landsat 8 OLI relative spectral response functions suggest that OLI is measuring 6 % to 16 % more top-of-atmosphere (TOA) spectral radiance from the Greenland ice sheet surface than was predicted using apparent reflectance spectra from the nadir-viewing spectrometer. While more investigation is required to convert airborne VSWIR spectral radiance into atmospherically corrected airborne surface reflectance, it is expected that airborne science flight data products will contribute to spectroscopic determination of Greenland ice sheet surface optical properties to improve understanding of their potential influence on ICESat-2 measurements.

Description: In this study 1 year of ceilometer measurements taken in the Kathmandu Valley, Nepal, in the framework of the SusKat project (A Sustainable Atmosphere for the Kathmandu Valley) were analysed to investigate the diurnal variation of the mixing layer height (MLH) and its dependency on the meteorological conditions. In addition, the impact of the MLH on the temporal variation and the magnitude of the measured black carbon concentrations are analysed for each season. Based on the assumption that black carbon aerosols are vertically well mixed within the mixing layer and the finding that the mixing layer varies only little during night time and morning hours, black carbon emission fluxes are estimated for these hours and per month. Even though this method is relatively simple, it can give an observationally based first estimate of the black carbon emissions in this region, especially illuminating the seasonal cycle of the emission fluxes. The monthly minimum median MLH values typically range between 150 and 200 m during night and early morning hours, the monthly maximum median values between 625 m in July and 1460 m in March. Seasonal differences are not only found in the absolute MLHs, but also in the duration of the typical daytime maximum ranging between 2 and 3 h in January and 6–7 h in May. During the monsoon season a diurnal cycle has been observed with the smallest amplitude (typically between 400 and 500 m), with the lowest daytime mixing height of all seasons (maximum monthly median values typically between 600 and 800 m), and also the highest night-time and early morning mixing height of all seasons (minimum monthly median values typically between 200 and 220 m). These characteristics can mainly be explained with the frequently present clouds and the associated reduction in incoming solar radiation and outgoing longwave radiation. In general, the black carbon concentrations show a clear anticorrelation with MLH measurements, although this relation is less pronounced in the monsoon season. The daily evolution of the black carbon diurnal cycle differs between the seasons, partly due to the different meteorological conditions including the MLH. Other important reasons are the different main emission sources and their diurnal variations in the individual seasons. The estimation of the black carbon emission flux for the morning hours show a clear seasonal cycle with maximum values in December to April. Compared to the emission flux values provided by different emission databases for this region, the estimated values here are considerably higher. Several possible sources of uncertainty are considered, and even the absolute lower bound of the emissions based on our methodology is higher than in most emissions datasets, providing strong evidence that the black carbon emissions for this region have likely been underestimated in modelling studies thus far.

Description: We use the GEOS-Chem global 3-D atmospheric chemistry transport model to interpret atmospheric observations of bromoform (CHBr3) and dibromomethane (CH2Br2) collected during the CAST and CONTRAST aircraft measurement campaigns over the western Pacific, January–February 2014. We use a new linearized, tagged version of CHBr3 and CH2Br2, allowing us to study the influence of emissions from specific geographical regions on observed atmospheric variations. The model describes 32 %–37 % of CHBr3 and 15 %–45 % of CH2Br2 observed variability during CAST and CONTRAST, reflecting model errors in vertical transport. The model has a mean positive bias of 30 % that is larger near the surface, reflecting errors in the poorly constrained prior emission estimates. We find using the model that observed variability of CHBr3 and CH2Br2 is driven by open ocean emissions where there is deep convection. Atmospheric variability above 6 km includes a significant contribution from coastal oceans, but it is still dominated by emissions from the open ocean and by older air masses that originate upwind. In the absence of reliable ocean emission estimates, we use a new physical age-of-air simulation to determine the relative abundance of halogens delivered by CHBr3 and CH2Br2 to the tropical transition layer (TTL). We find that 76 % (92 %) of air masses that originate from the ocean reach the TTL within two (three) atmospheric e-folding lifetimes of CHBr3 and almost all of them reach the TTL within one e-folding lifetime of CH2Br2. Over the duration of CAST and CONTRAST, and over our study region, oceans delivered a mean (range) CHBr3 and CH2Br2 mole fraction of 0.46 (0.13–0.72) and 0.88 (0.71–1.01) pptv, respectively, to the TTL, and a mean (range) Bry mole fraction of 3.14 (1.81–4.18) pptv from source gases to the upper troposphere.

Description: With NO2 limit values being frequently exceeded in European cities, complying with the European air quality regulations still poses a problem for many cities. Traffic is typically a major source of NOx emissions in urban areas. High-resolution chemistry transport modelling can help to assess the impact of high urban NOx emissions on air quality inside and outside of urban areas. However, many modelling studies report an underestimation of modelled NOx and NO2 compared with observations. Part of this model bias has been attributed to an underestimation of NOx emissions, particularly in urban areas. This is consistent with recent measurement studies quantifying underestimations of urban NOx emissions by current emission inventories, identifying the largest discrepancies when the contribution of traffic NOx emissions is high. This study applies a high-resolution chemistry transport model in combination with ambient measurements in order to assess the potential underestimation of traffic NOx emissions in a frequently used emission inventory. The emission inventory is based on officially reported values and the Berlin–Brandenburg area in Germany is used as a case study. The WRF-Chem model is used at a 3 km × 3 km horizontal resolution, simulating the whole year of 2014. The emission data are downscaled from an original resolution of ca. 7 km × 7 km to a resolution of 1 km × 1 km. An in-depth model evaluation including spectral decomposition of observed and modelled time series and error apportionment suggests that an underestimation in traffic emissions is likely one of the main causes of the bias in modelled NO2 concentrations in the urban background, where NO2 concentrations are underestimated by ca. 8 µg m−3 (−30 %) on average over the whole year. Furthermore, a diurnal cycle of the bias in modelled NO2 suggests that a more realistic treatment of the diurnal cycle of traffic emissions might be needed. Model problems in simulating the correct mixing in the urban planetary boundary layer probably play an important role in contributing to the model bias, particularly in summer. Also taking into account this and other possible sources of model bias, a correction factor for traffic NOx emissions of ca. 3 is estimated for weekday daytime traffic emissions in the core urban area, which corresponds to an overall underestimation of traffic NOx emissions in the core urban area of ca. 50 %. Sensitivity simulations for the months of January and July using the calculated correction factor show that the weekday model bias can be improved from −8.8 µg m−3 (−26 %) to −5.4 µg m−3 (−16 %) in January on average in the urban background, and −10.3 µg m−3 (−46 %) to −7.6 µg m−3 (−34 %) in July. In addition, the negative bias of weekday NO2 concentrations downwind of the city in the rural and suburban background can be reduced from −3.4 µg m−3 (−12 %) to −1.2 µg m−3 (−4 %) in January and from −3.0 µg m−3 (−22 %) to −1.9 µg m−3 (−14 %) in July. The results and their consistency with findings from other studies suggest that more research is needed in order to more accurately understand the spatial and temporal variability in real-world NOx emissions from traffic, and apply this understanding to the inventories used in high-resolution chemical transport models.

Description: The “Berlin Air quality and Ecosystem Research: Local and long-range Impact of anthropogenic and Natural hydrocarbons” (BAERLIN2014) campaign was conducted during the 3 summer months (June–August) of 2014. During this measurement campaign, both stationary and mobile measurements were undertaken to address complementary aims. This paper provides an overview of the stationary measurements and results that were focused on characterization of gaseous and particulate pollution, including source attribution, in the Berlin–Potsdam area, and quantification of the role of natural sources in determining levels of ozone and related gaseous pollutants. Results show that biogenic contributions to ozone and particulate matter are substantial. One indicator for ozone formation, the OH reactivity, showed a 31 % (0.82 ± 0.44 s−1) and 75 % (3.7 ± 0.90 s−1) contribution from biogenic non-methane volatile organic compounds (NMVOCs) for urban background (2.6 ± 0.68 s−1) and urban park (4.9 ± 1.0 s−1) location, respectively, emphasizing the importance of such locations as sources of biogenic NMVOCs in urban areas. A comparison to NMVOC measurements made in Berlin approximately 20 years earlier generally show lower levels today for anthropogenic NMVOCs. A substantial contribution of secondary organic and inorganic aerosol to PM10 concentrations was quantified. In addition to secondary aerosols, source apportionment analysis of the organic carbon fraction identified the contribution of biogenic (plant-based) particulate matter, as well as primary contributions from vehicles, with a larger contribution from diesel compared to gasoline vehicles, as well as a relatively small contribution from wood burning, linked to measured levoglucosan.

Description: Ozone (O3) is an important atmospheric oxidant, a greenhouse gas, and a hazard to human health and agriculture. Here we describe airborne in situ measurements and model simulations of O3 and its precursors during tropical and extratropical field campaigns over South America and Europe, respectively. Using the measurements, net ozone formation/destruction tendencies are calculated and compared to 3-D chemistry–transport model simulations. In general, observation-based net ozone tendencies are positive in the continental boundary layer and the upper troposphere at altitudes above  ∼  6 km in both environments. On the other hand, in the marine boundary layer and the middle troposphere, from the top of the boundary layer to about 6–8 km altitude, net O3 destruction prevails. The ozone tendencies are controlled by ambient concentrations of nitrogen oxides (NOx). In regions with net ozone destruction the available NOx is below the threshold value at which production and destruction of O3 balance. While threshold NO values increase with altitude, in the upper troposphere NOx concentrations are generally higher due to the integral effect of convective precursor transport from the boundary layer, downward transport from the stratosphere and NOx produced by lightning. Two case studies indicate that in fresh convective outflow of electrified thunderstorms net ozone production is enhanced by a factor 5–6 compared to the undisturbed upper tropospheric background. The chemistry–transport model MATCH-MPIC generally reproduces the pattern of observation-based net ozone tendencies but mostly underestimates the magnitude of the net tendency (for both net ozone production and destruction).

Description: The agreement between reanalysis datasets, in terms of the zonal-mean momentum budget, is evaluated during sudden stratospheric warming (SSW) events. It is revealed that there is a good agreement among datasets in the lower stratosphere and troposphere concerning zonal-mean zonal wind, but less so in the upper stratosphere. Forcing terms of the momentum equation are also relatively similar in the lower atmosphere, but their uncertainties are typically larger than uncertainties of the zonal-wind tendency. Similar to zonal-wind tendency, the agreement among forcing terms is degraded in the upper stratosphere. Discrepancies among reanalyses increase during the onset of SSW events, a period characterized by unusually large fluxes of planetary-scale waves from the troposphere to the stratosphere, and decrease substantially after the onset. While the largest uncertainties in the resolved terms of the momentum budget are found in the Coriolis torque, momentum flux convergence also presents a non-negligible spread among the reanalyses. Such a spread is reduced in the latest reanalysis products, decreasing the uncertainty of the momentum budget. It is also found that the uncertainties in the Coriolis torque depend on the strength of SSW events: the SSW events that exhibit the most intense deceleration of zonal-mean zonal wind are subject to larger discrepancies among reanalyses. These uncertainties in stratospheric circulation, however, are not communicated to the troposphere.