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The purpose of this study is to demonstrate the role of aerosol layer height (ALH) in quantifying the single scattering albedo (SSA) from ultraviolet satellite observations for biomass burning aerosols. In the first experiment, we retrieve SSA by minimizing the near-ultraviolet (near-UV) absorbing aerosol index (UVAI) difference between observed values and those simulated by a radiative transfer model. With the recently released S-5P TROPOMI ALH product constraining forward simulations, a significant gap in the retrieved SSA (0.25) is found between radiative transfer simulations with spectral flat aerosols and those with strong spectrally dependent aerosols, implying that inappropriate assumptions regarding aerosol absorption spectral dependence may cause severe misinterpretations of the aerosol absorption. In the second part of this paper, we propose an alternative method to retrieve SSA based on a long-term record of co-located satellite and ground-based measurements using the support vector regression (SVR) approach. This empirical method is free from the uncertainties due to the imperfection of a priori assumptions on aerosol microphysics seen in the first experiment. We present the potential capabilities of SVR using several fire events that have occurred in recent years. For all cases, the difference between SVR-retrieved SSA and AERONET are generally within ±0.05, and over half of the samples are within ±0.03. The results are encouraging, although in the current phase the model tends to overestimate the SSA for relatively absorbing cases and fails to predict SSA for some extreme situations. The spatial contrast in SSA retrieved by radiative transfer simulations is significantly higher than that retrieved by SVR, and the latter better agrees with SSA from MERRA-2 reanalysis. In the future, more sophisticated feature selection procedures and kernel functions should be taken into consideration to improve the SVR model accuracy. Moreover, the high-resolution TROPOMI UVAI and co-located ALH products will guide us to more reliable training data sets and more powerful algorithms to quantify aerosol absorption from UVAI records.

The absorbing aerosol index (AAI) is a qualitative parameter directly calculated from satellite-measured reflectance. Its sensitivity to absorbing aerosols in combination with a long-term data record since 1978 makes it an important parameter for climate research. In this study, we attempt to quantify aerosol absorption by retrieving the single-scattering albedo (ω0) at 550 nm from the satellite-measured AAI. In the first part of this study, AAI sensitivity studies are presented exclusively for biomass-burning aerosols. Later on, we employ a radiative transfer model (DISAMAR) to simulate the AAI measured by the Ozone Monitoring Instrument (OMI) in order to derive ω0 at 550 nm. Inputs for the radiative transfer calculations include satellite measurement geometry and surface conditions from OMI, aerosol optical thickness (τ) from the Moderate Resolution Imaging Spectroradiometer (MODIS) and aerosol microphysical parameters from the AErosol RObotic NETwork (AERONET), respectively. This approach is applied to the Chile wildfires for the period from 26 to 30 January 2017, when the OMI-observed AAI of this event reached its peak. The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) overpasses missed the evolution of the smoke plume over the research region; therefore the aerosol profile is parameterized. The simulated plume is at an altitude of 4.5–4.9 km, which is in good agreement with available CALIOP backscatter coefficient measurements. The data may contain pixels outside the plume, so an outlier detection criterion is applied. The results show that the AAI simulated by DISAMAR is consistent with satellite observations. The correlation coefficients fall into the range between 0.85 and 0.95. The retrieved mean ω0 at 550 nm for the entire plume over the research period from 26 to 30 January 2017 varies from 0.81 to 0.87, whereas the nearest AERONET station reported ω0 between 0.89 and 0.92. The difference in geolocation between the AERONET site and the plume, the assumption of homogeneous plume properties, the lack of the aerosol profile information and the uncertainties in the inputs for radiative transfer calculation are primarily responsible for this discrepancy in ω0.

Mercury was measured onboard the IAGOS-CARIBIC passenger aircraft from May 2005 until February 2016 during near monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data.Increased upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Speciation experiments suggest comparable TM and gaseous elementary mercury (GEM) concentrations at and below the tropopause leaving little space for Hg2+ (TM − GEM) being the dominating component of TM here. In the stratosphere significant GEM concentrations were found to exist up to 4 km altitude above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72±37 and 74±27 years for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation and cloud scavenging processes.

The development and application of chemistry transport models has a long tradition. Within the Netherlands the LOTOS–EUROS model has been developed by a consortium of institutes, after combining its independently developed predecessors in 2005. Recently, version 2.0 of the model was released as an open-source version. This paper presents the curriculum vitae of the model system, describing the model's history, model philosophy, basic features and a validation with EMEP stations for the new benchmark year 2012, and presents cases with the model's most recent and key developments. By setting the model developments in context and providing an outlook for directions for further development, the paper goes beyond the common model description.With an origin in ozone and sulfur modelling for the models LOTOS and EUROS, the application areas were gradually extended with persistent organic pollutants, reactive nitrogen, and primary and secondary particulate matter. After the combination of the models to LOTOS–EUROS in 2005, the model was further developed to include new source parametrizations (e.g. road resuspension, desert dust, wildfires), applied for operational smog forecasts in the Netherlands and Europe, and has been used for emission scenarios, source apportionment, and long-term hindcast and climate change scenarios. LOTOS–EUROS has been a front-runner in data assimilation of ground-based and satellite observations and has participated in many model intercomparison studies. The model is no longer confined to applications over Europe but is also applied to other regions of the world, e.g. China. The increasing interaction with emission experts has also contributed to the improvement of the model's performance. The philosophy for model development has always been to use knowledge that is state of the art and proven, to keep a good balance in the level of detail of process description and accuracy of input and output, and to keep a good record on the effect of model changes using benchmarking and validation. The performance of v2.0 with respect to EMEP observations is good, with spatial correlations around 0.8 or higher for concentrations and wet deposition. Temporal correlations are around 0.5 or higher. Recent innovative applications include source apportionment and data assimilation, particle number modelling, and energy transition scenarios including corresponding land use changes as well as Saharan dust forecasting. Future developments would enable more flexibility with respect to model horizontal and vertical resolution and further detailing of model input data. This includes the use of different sources of land use characterization (roughness length and vegetation), detailing of emissions in space and time, and efficient coupling to meteorology from different meteorological models.

This paper describes the pre-operational analysis and forecasting system developed during MACC (Monitoring Atmospheric Composition and Climate) and continued in the MACC-II (Monitoring Atmospheric Composition and Climate: Interim Implementation) European projects to provide air quality services for the European continent. This system is based on seven state-of-the art models developed and run in Europe (CHIMERE, EMEP, EURAD-IM, LOTOS-EUROS, MATCH, MOCAGE and SILAM). These models are used to calculate multi-model ensemble products. The paper gives an overall picture of its status at the end of MACC-II (summer 2014) and analyses the performance of the multi-model ensemble. The MACC-II system provides daily 96 h forecasts with hourly outputs of 10 chemical species/aerosols (O3, NO2, SO2, CO, PM10, PM2.5, NO, NH3, total NMVOCs (non-methane volatile organic compounds) and PAN+PAN precursors) over eight vertical levels from the surface to 5 km height. The hourly analysis at the surface is done a posteriori for the past day using a selection of representative air quality data from European monitoring stations. The performance of the system is assessed daily, weekly and every 3 months (seasonally) through statistical indicators calculated using the available representative air quality data from European monitoring stations. Results for a case study show the ability of the ensemble median to forecast regional ozone pollution events. The seasonal performances of the individual models and of the multi-model ensemble have been monitored since September 2009 for ozone, NO2 and PM10. The statistical indicators for ozone in summer 2014 show that the ensemble median gives on average the best performances compared to the seven models. There is very little degradation of the scores with the forecast day but there is a marked diurnal cycle, similarly to the individual models, that can be related partly to the prescribed diurnal variations of anthropogenic emissions in the models. During summer 2014, the diurnal ozone maximum is underestimated by the ensemble median by about 4 μg m−3 on average. Locally, during the studied ozone episodes, the maxima from the ensemble median are often lower than observations by 30–50 μg m−3. Overall, ozone scores are generally good with average values for the normalised indicators of 0.14 for the modified normalised mean bias and of 0.30 for the fractional gross error. Tests have also shown that the ensemble median is robust to reduction of ensemble size by one, that is, if predictions are unavailable from one model. Scores are also discussed for PM10 for winter 2013–1014. There is an underestimation of most models leading the ensemble median to a mean bias of −4.5 μg m−3. The ensemble median fractional gross error is larger for PM10 (~ 0.52) than for ozone and the correlation is lower (~ 0.35 for PM10 and ~ 0.54 for ozone). This is related to a larger spread of the seven model scores for PM10 than for ozone linked to different levels of complexity of aerosol representation in the individual models. In parallel, a scientific analysis of the results of the seven models and of the ensemble is also done over the Mediterranean area because of the specificity of its meteorology and emissions. The system is robust in terms of the production availability. Major efforts have been done in MACC-II towards the operationalisation of all its components. Foreseen developments and research for improving its performances are discussed in the conclusion.

Short-lived organic brominated compounds make up a significant part of the organic bromine budget in the atmosphere. Emissions of these compounds are highly variable and there are limited measurements, particularly in the extra-tropical upper troposphere/lower stratosphere and tropical troposphere. Measurements of five very short-lived bromomethanes (VSLB) were made in air samples collected on the CARIBIC project aircraft over three flight routes; Germany to Venezuela/Columbia during 2009–2011, Germany to South Africa during 2010 and 2011 and Germany to Thailand/Kuala Lumpur, Malaysia during 2012 and 2013. In the tropical troposphere, as the most important entrance region to the stratosphere, we observe a total mean organic bromine derived from these compounds across all flights at 10–12 km altitude of 3.4 ± 1.5 ppt. Individual mean tropical tropospheric mixing ratios across all flights were 0.43, 0.74, 0.14, 0.23 and 0.11 ppt for CHBr3, CH2Br2, CHBr2Cl, CHBrCl2 and CH2BrCl respectively. The highest levels of VSLB-derived bromine (4.20 ± 0.56 ppt) were observed in flights between Bangkok and Kuala Lumpur indicating that the South China Sea is an important source region for these compounds. Across all routes, CHBr3 and CH2Br2 accounted for 34% (4.7–71) and 48% (14–73) respectively of total bromine derived from the analysed VSLB in the tropical mid-upper troposphere totalling 82% (54–89). In samples collected between Germany and Venezuela/Columbia, we find decreasing mean mixing ratios with increasing potential temperature in the extra-tropics. Tropical mean mixing ratios are higher than extra-tropical values between 340–350 K indicating that rapid uplift is important in determining mixing ratios in the lower tropical tropopause layer in the West Atlantic tropics. O3 was used as a tracer for stratospherically influenced air and we detect rapidly decreasing mixing ratios for all VSLB above ∼100 ppb O3 corresponding to the extra-tropical tropopause layer.

The future impact of traffic emissions on atmospheric ozone and OH has been investigated separately for the three sectors AIRcraft, maritime SHIPping and ROAD traffic. To reduce uncertainties we present results from an ensemble of six different atmospheric chemistry models, each simulating the atmospheric chemical composition in a possible high emission scenario (A1B), and with emissions from each transport sector reduced by 5% to estimate sensitivities. Our results are compared with optimistic future emission scenarios (B1 and B1 ACARE), presented in a companion paper, and with the recent past (year 2000). Present-day activity indicates that anthropogenic emissions so far evolve closer to A1B than the B1 scenario. As a response to expected changes in emissions, AIR and SHIP will have increased impacts on atmospheric O3 and OH in the future while the impact of ROAD traffic will decrease substantially as a result of technological improvements. In 2050, maximum aircraft-induced O3 occurs near 80° N in the UTLS region and could reach 9 ppbv in the zonal mean during summer. Emissions from ship traffic have their largest O3 impact in the maritime boundary layer with a maximum of 6 ppbv over the North Atlantic Ocean during summer in 2050. The O3 impact of road traffic emissions in the lower troposphere peaks at 3 ppbv over the Arabian Peninsula, much lower than the impact in 2000. Radiative forcing (RF) calculations show that the net effect of AIR, SHIP and ROAD combined will change from a marginal cooling of −0.44 ± 13 mW m−2 in 2000 to a relatively strong cooling of −32 ± 9.3 (B1) or −32 ± 18 mW m−2 (A1B) in 2050, when taking into account RF due to changes in O3, CH4 and CH4-induced O3. This is caused both by the enhanced negative net RF from SHIP, which will change from −19 ± 5.3 mW m−2 in 2000 to −31 ± 4.8 (B1) or −40 ± 9 mW m−2 (A1B) in 2050, and from reduced O3 warming from ROAD, which is likely to turn from a positive net RF of 12 ± 8.5 mW m−2 in 2000 to a slightly negative net RF of −3.1 ± 2.2 (B1) or −3.1 ± 3.4 (A1B) mW m−2 in the middle of this century. The negative net RF from ROAD is temporary and induced by the strong decline in ROAD emissions prior to 2050, which only affects the methane cooling term due to the longer lifetime of CH4 compared to O3. The O3 RF from AIR in 2050 is strongly dependent on scenario and ranges from 19 ± 6.8 (B1 ACARE) to 61 ± 14 mW m−2 (A1B). There is also a considerable span in the net RF from AIR in 2050, ranging from −0.54 ± 4.6 (B1 ACARE) to 12 ± 11 (A1B) mW m−2 compared to 6.6 ± 2.2 mW m−2 in 2000.

The impact of future emissions from aviation and shipping on the atmospheric chemical composition has been estimated using an ensemble of six different atmospheric chemistry models. This study considers an optimistic emission scenario (B1) taking into account e.g. rapid introduction of clean and resource-efficient technologies, and a mitigation option for the aircraft sector (B1 ACARE), assuming further technological improvements. Results from sensitivity simulations, where emissions from each of the transport sectors were reduced by 5%, show that emissions from both aircraft and shipping will have a larger impact on atmospheric ozone and OH in near future (2025; B1) and for longer time horizons (2050; B1) compared to recent time (2000). However, the ozone and OH impact from aircraft can be reduced substantially in 2050 if the technological improvements considered in the B1 ACARE will be achieved. Shipping emissions have the largest impact in the marine boundary layer and their ozone contribution may exceed 4 ppbv (when scaling the response of the 5% emission perturbation to 100% by applying a factor 20) over the North Atlantic Ocean in the future (2050; B1) during northern summer (July). In the zonal mean, ship-induced ozone relative to the background levels may exceed 12% near the surface. Corresponding numbers for OH are 6.0 × 105 molecules cm−3 and 30%, respectively. This large impact on OH from shipping leads to a relative methane lifetime reduction of 3.92 (±0.48) on the global average in 2050 B1 (ensemble mean CH4 lifetime is 8.0 (±1.0) yr), compared to 3.68 (±0.47)% in 2000. Aircraft emissions have about 4 times higher ozone enhancement efficiency (ozone molecules enhanced relative to NOx molecules emitted) than shipping emissions, and the maximum impact is found in the UTLS region. Zonal mean aircraft-induced ozone could reach up to 5 ppbv at northern mid- and high latitudes during future summer (July 2050; B1), while the relative impact peaks during northern winter (January) with a contribution of 4.2%. Although the aviation-induced impact on OH is lower than for shipping, it still causes a reduction in the relative methane lifetime of 1.68 (±0.38)% in 2050 B1. However, for B1 ACARE the perturbation is reduced to 1.17 (±0.28)%, which is lower than the year 2000 estimate of 1.30 (±0.30)%. Based on the fully scaled perturbations we calculate net radiative forcings from the six models taking into account ozone, methane (including stratospheric water vapour), and methane-induced ozone changes. For the B1 scenario, shipping leads to a net cooling with radiative forcings of −28.0 (±5.1) and −30.8 (±4.8) mW m−2 in 2025 and 2050, respectively, due to the large impact on OH and, thereby, methane lifetime reductions. Corresponding values for the aviation sector shows a net warming effect with 3.8 (±6.1) and 1.9 (±6.3) mW m−2, respectively, but with a small net cooling of -0.6 (±4.6) mW m−2 for B1 ACARE in 2050.

Natural methane (CH4) emissions from wet ecosystems are an important part of today's global CH4 budget. Climate affects the exchange of CH4 between ecosystems and the atmosphere by influencing CH4 production, oxidation, and transport in the soil. The net CH4 exchange depends on ecosystem hydrology, soil and vegetation characteristics. Here, the LPJ-WHyMe global dynamical vegetation model is used to simulate global net CH4 emissions for different ecosystems: northern peatlands (45°–90° N), naturally inundated wetlands (60° S–45° N), rice agriculture and wet mineral soils. Mineral soils are a potential CH4 sink, but can also be a source with the direction of the net exchange depending on soil moisture content. The geographical and seasonal distributions are evaluated against multi-dimensional atmospheric inversions for 2003–2005, using two independent four-dimensional variational assimilation systems. The atmospheric inversions are constrained by the atmospheric CH4 observations of the SCIAMACHY satellite instrument and global surface networks. Compared to LPJ-WHyMe the inversions result in a~significant reduction in the emissions from northern peatlands and suggest that LPJ-WHyMe maximum annual emissions peak about one month late. The inversions do not put strong constraints on the division of sources between inundated wetlands and wet mineral soils in the tropics. Based on the inversion results we diagnose model parameters in LPJ-WHyMe and simulate the surface exchange of CH4 over the period 1990–2008. Over the whole period we infer an increase of global ecosystem CH4 emissions of +1.11 Tg CH4 yr−1, not considering potential additional changes in wetland extent. The increase in simulated CH4 emissions is attributed to enhanced soil respiration resulting from the observed rise in land temperature and in atmospheric carbon dioxide that were used as input. The long-term decline of the atmospheric CH4 growth rate from 1990 to 2006 cannot be fully explained with the simulated ecosystem emissions. However, these emissions show an increasing trend of +3.62 Tg CH4 yr−1 over 2005–2008 which can partly explain the renewed increase in atmospheric CH4 concentration during recent years.

Between April and December 2008 the CARIBIC commercial aircraft conducted monthly measurement flights between Frankfurt, Germany and Chennai, India. These flights covered the period of the Asian summer monsoon (June–September), during which enhancements in a number of atmospheric species were observed in the upper troposphere over southwestern Asia. In addition to in situ measurements of trace gases and aerosols, whole air samples were collected during the flights, and these were subsequently analyzed for a suite of trace gases that included a number of C2–C8 non-methane hydrocarbons. Non-methane hydrocarbons are relatively short-lived compounds and the large enhancements in their mixing ratios in the upper troposphere over southwestern Asia during the monsoon, sometimes more than double their spring and fall means, provides qualitative evidence for the influence of convectively uplifted boundary layer air. The particularly large enhancements of the combustion tracers benzene and ethyne, along with the similarity of their ratios with carbon monoxide and emission ratios from the burning of household biofuels, indicate a strong influence of biofuel burning to NMHC emissions in this region. Conversely, the ratios of ethane and propane to carbon monoxide, along with the ratio between i-butane and n-butane, indicate a significant source of these compounds from the use of fossil fuels, and comparison to previous campaigns suggests that this source could be increasing. Photochemical aging patterns of NMHCs showed that the CARIBIC samples were collected in two distinctly different regions of the monsoon circulation: a southern region where air masses had been recently influenced by low level contact and a northern region, where air parcels had spent substantial time in transit in the upper troposphere before being probed. Estimates of age using ratios of individual NMHCs have ranges of 3–6 days in the south and 9–12 days in the north.

In this study, the LMDz-INCA climate-chemistry model and up-to-date global emission inventories are used to investigate the "present" (2000) and future (2050) impacts of transport emissions (road traffic, shipping and aircraft) on global tropospheric ozone. For the first time, both impacts of emissions and climate changes on transport-induced ozone are investigated. The 2000 transport emissions are shown to mainly affect ozone in the Northern Hemisphere, with a maximum increase of the tropospheric column of up to 5 DU, from the South-eastern US to Central Europe. The impact is dominated by road traffic in the middle and upper troposphere, North of 40° S, and by shipping in the northern lower troposphere, over oceanic regions. A strong reduction of road emissions and a moderate (B1 scenario) to high (A1B scenario) increase of the ship and aircraft emissions are projected by the year 2050. As a consequence, LMDz-INCA simulations predict a drastic decrease in the impact of road emissions, whereas aviation would become the major transport perturbation on tropospheric ozone, even in the case of a very optimistic aircraft mitigation scenario. The A1B emission scenario leads to an increase of the impact of transport on zonal mean ozone concentrations in 2050 by up to +30% and +50%, in the Northern and Southern Hemispheres, respectively. Despite a similar total amount of global NOx emissions by the various transport sectors compared to 2000, the overall impact on the tropospheric ozone column is increased everywhere in 2050, due to a sectoral shift in the emissions of the respective transport modes. On the opposite, the B1 mitigation scenario leads to a significant reduction (by roughly 50%) of the ozone perturbation throughout the troposphere compared to 2000. Considering climate change, and according to scenario A1B, a decrease of the O3 tropospheric burden is simulated by 2050 due to climate change (−1.2%), whereas an increase of ozone of up to 2% is calculated in the upper troposphere in the inter-tropical zone, due to enhanced lightning activity. A global impact of similar magnitude is simulated for the transport-induced ozone burden perturbation (−1.6%). As a result, the future increase in global ozone due to changes in anthropogenic emissions is lowered by 12% and by 4%, for the background and the transport-induced ozone, respectively. However, positive and negative climate effects are obtained on ozone, depending on the season, region and altitude, with an increase of the transport-induced ozone perturbation (+0.4 DU) in the already most affected area of Northern Hemisphere.

African biomass burning emission inventories for gaseous and particulate species have been constructed at a resolution of 1 km by 1km with daily coverage for the 2000–2007 period. These inventories are higher than the GFED2 inventories, which are currently widely in use. Evaluation specifically focusing on combustion aerosol has been carried out with the ORISAM-TM4 global chemistry transport model which includes a detailed aerosol module. This paper compares modeled results with measurements of surface BC concentrations and scattering coefficients from the AMMA Enhanced Observations period, aerosol optical depths and single scattering albedo from AERONET sunphotometers, LIDAR vertical distributions of extinction coefficients as well as satellite data. Aerosol seasonal and interannual evolutions over the 2004–2007 period observed at regional scale and more specifically at the Djougou (Benin) and Banizoumbou (Niger) AMMA/IDAF sites are well reproduced by our global model, indicating that our biomass burning emission inventory appears reasonable.

We present a comprehensive description and benchmark evaluation of the tropospheric chemistry version of the global chemistry transport model TM5 (Tracer Model 5, version TM5-chem-v3.0). A full description is given concerning the photochemical mechanism, the interaction with aerosol, the treatment of the stratosphere, the wet and dry deposition parameterizations, and the applied emissions. We evaluate the model against a suite of ground-based, satellite, and aircraft measurements of components critical for understanding global photochemistry for the year 2006. The model exhibits a realistic oxidative capacity at a global scale. The methane lifetime is ~8.9 years with an associated lifetime of methyl chloroform of 5.86 years, which is similar to that derived using an optimized hydroxyl radical field. The seasonal cycle in observed carbon monoxide (CO) is well simulated at different regions across the globe. In the Northern Hemisphere CO concentrations are underestimated by about 20 ppbv in spring and 10 ppbv in summer, which is related to missing chemistry and underestimated emissions from higher hydrocarbons, as well as to uncertainties in the seasonal variation of CO emissions. The model also captures the spatial and seasonal variation in formaldehyde tropospheric columns as observed by SCIAMACHY. Positive model biases over the Amazon and eastern United States point to uncertainties in the isoprene emissions as well as its chemical breakdown. Simulated tropospheric nitrogen dioxide columns correspond well to observations from the Ozone Monitoring Instrument in terms of its seasonal and spatial variability (with a global spatial correlation coefficient of 0.89), but TM5 fields are lower by 25–40%. This is consistent with earlier studies pointing to a high bias of 0–30% in the OMI retrievals, but uncertainties in the emission inventories have probably also contributed to the discrepancy. TM5 tropospheric nitrogen dioxide profiles are in good agreement (within ~0.1 ppbv) with in situ aircraft observations from the INTEX-B campaign over (the Gulf of) Mexico. The model reproduces the spatial and seasonal variation in background surface ozone concentrations and tropospheric ozone profiles from the World Ozone and Ultraviolet Radiation Data Centre to within 10 ppbv, but at several tropical stations the model tends to underestimate ozone in the free troposphere. The presented model results benchmark the TM5 tropospheric chemistry version, which is currently in use in several international cooperation activities, and upon which future model improvements will take place.

Within the African Monsoon Multidisciplinary Analysis (AMMA), we investigate the impact of nitrogen oxides produced by lightning (LiNOx) and convective transport during the West African Monsoon (WAM) upon the composition of the upper troposphere (UT) in the tropics. For this purpose, we have performed simulations with 4 state-of-the-art chemistry transport models involved within AMMA, namely MOCAGE, TM4, LMDz-INCA and p-TOMCAT. The model intercomparison is complemented with an evaluation of the simulations based on both spaceborne and airborne observations. The baseline simulations show important differences between the UT CO and O3 distributions simulated by each of the 4 models when compared to measurements from the MOZAIC program and fom the Aura/MLS spaceborne sensor. We show that such model discrepancies can be explained by differences in the convective transport parameterizations and, more particularly, the altitude reached by convective updrafts (ranging between ~200–125 hPa). Concerning UT O3, the models exhibit a good agreement with the main observed features. Nevertheless the majority of models simulate low O3 concentrations compared to both MOZAIC and Aura/MLS observations south of the equator, and rather high concentrations in the Northern Hemisphere. Sensitivity studies are performed to quantify the effect of deep convective transport and the influence of LiNOx production on the UT composition. These clearly indicate that the CO maxima and the elevated O3 concentrations south of the equator are due to convective uplift of air masses impacted by Southern African biomass burning, in agreement with previous studies. Moreover, during the WAM, LiNOx from Africa are responsible for the highest UT O3 enhancements (10–20 ppbv) over the tropical Atlantic between 10° S–20° N. Differences between models are primarily due to the performance of the parameterizations used to simulate lightning activity which are evaluated using spaceborne observations of flash frequency. Combined with comparisons of in-situ NO measurements we show that the models producing the highest amounts of LiNOx over Africa during the WAM (INCA and p-TOMCAT) capture observed NO profiles with the best accuracy, although they both overestimate lightning activity over the Sahel.

A strong pollution episode in the upper troposphere between South China and the Philippines was observed during CARIBIC flights in April 2007. Five pollution events were observed, where enhancements in aerosol and trace gas concentrations including CO, CO2, CH4, non-methane hydrocarbons (NMHCs) and halocarbons were observed along the flight tracks during four sequential flights. The importance of the contribution of biomass/biofuel burning was investigated using chemical tracers, emission factor analysis, back-trajectory analysis and satellite images. The Indochinese peninsula was identified as the probable source region of biomass/biofuel burning. However, enhancements in the urban/industrial tracer C2Cl4 during the events also indicate a substantial contribution from urban anthropogenic emissions. An estimation of the contribution of fossil fuel versus biomass/biofuel to the CO enhancement was made, indicating a biomass/biofuel burning contribution of ~54 to ~92% of the observed CO enhancements. Biomass/biofuel burning was found to be the most important source category during the sampling period.

To estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH in the present-day atmosphere six different atmospheric chemistry models have been used. Based on newly developed global emission inventories for road, ship and aircraft emission data sets each model performed sensitivity simulations reducing the emissions of each transport sector by 5%. The model results indicate that on global annual average lower tropospheric ozone responds most sensitive to ship emissions (50.6%±10.9% of the total traffic induced perturbation), followed by road (36.7%±9.3%) and aircraft exhausts (12.7%±2.9%), respectively. In the northern upper troposphere between 200–300 hPa at 30–60° N the maximum impact from road and ship are 93% and 73% of the maximum effect of aircraft, respectively. The latter is 0.185 ppbv for ozone (for the 5% case) or 3.69 ppbv when scaling to 100%. On the global average the impact of road even dominates in the UTLS-region. The sensitivity of ozone formation per NOx molecule emitted is highest for aircraft exhausts. The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 0.2 DU and occurs over the northern subtropical Atlantic extending to central Europe. Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine lower troposphere over the Atlantic. Based on the 5% perturbation the effect on ozone can exceed 0.6% close to the marine surface (global zonal mean) which is 80% of the total traffic induced ozone perturbation. In the southern hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%–80% throughout the year. Methane lifetime changes against OH are affected strongest by ship emissions up to 0.21 (± 0.05)%, followed by road (0.08 (±0.01)%) and air traffic (0.05 (± 0.02)%). Based on the full scale ozone and methane perturbations positive radiative forcings were calculated for road emissions (7.3±6.2 mWm−2) and for aviation (2.9±2.3 mWm−2). Ship induced methane lifetime changes dominate over the ozone forcing and therefore lead to a net negative forcing (−25.5±13.2 mWm−2).

Total gaseous mercury (TGM) was measured onboard a passenger aircraft during monthly CARIBIC flights (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrumented Container) made between May 2005 and March 2007 on the routes Frankfurt–São Paulo–Santiago de Chile and back and Frankfurt–Guangzhou–Manila and back. The data provide for the first time an insight into the seasonal distributions of TGM in the upper troposphere and lower stratosphere (UT/LS) of both hemispheres and demonstrate the importance of mercury emissions from biomass burning in the Southern Hemisphere. Numerous plumes were observed in the upper troposphere, the larger of which could be characterized in terms of Hg/CO emission ratios and their probable origins. During the flights to China TGM correlated with CO in the upper troposphere with a seasonally dependent slope reflecting the longer lifetime of elemental mercury when compared to that of CO. A pronounced depletion of TGM was always observed in the extratropical lowermost stratosphere. TGM concentrations there were found to decrease with the increasing concentrations of particles. Combined with the large concentrations of particle bond mercury in the stratosphere observed by others, this finding suggests either a direct conversion of TGM to particle bound mercury or an indirect conversion via a semivolatile bivalent mercury compound. Based on concurrent measurements of SF6 during two flights, the rate of this conversion is estimated to 0.4 ng m−3 yr−1. A zero TGM concentration was not observed during some 200 flight hours in the lowermost stratosphere suggesting an equilibrium between the gaseous and particulate mercury.

An airfreight container with automated instruments for measurement of atmospheric gases and trace compounds was operated on a monthly basis onboard a Boeing 767-300 ER of LTU International Airways during long-distance flights from 1997 to 2002 (CARIBIC, Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container, http://www.caribic-atmospheric.com). Subsequently a more advanced system has been developed, using a larger capacity container with additional equipment and an improved inlet system. CARIBIC phase #2 was implemented on a new long-range aircraft type Airbus A340-600 of the Lufthansa German Airlines (Star Alliance) in December 2004, creating a powerful flying observatory. The instrument package comprises detectors for the measurement of O3, total and gaseous H2O, NO and NOy, CO, CO2, O2, Hg, and number concentrations of sub-micrometer particles (>4 nm, >12 nm, and >18 nm diameter). Furthermore, an optical particle counter (OPC) and a proton transfer mass spectrometer (PTR-MS) are incorporated. Aerosol samples are collected for analysis of elemental composition and particle morphology after flight. Air samples are taken in glass containers for laboratory analyses of hydrocarbons, halocarbons and greenhouse gases (including isotopic composition of CO2) in several laboratories. Absorption tubes collect oxygenated volatile organic compounds. Three differential optical absorption spectrometers (DOAS) with their telescopes mounted in the inlet system measure atmospheric trace gases such as BrO, HONO, and NO2. A video camera mounted in the inlet provides information about clouds along the flight track. The flying observatory, its equipment and examples of measurement results are reported.

This is the second part of a rigorous model evaluation study involving five global Chemistry-Transport and two Chemistry-Climate Models operated by different groups in Europe. Simulated trace gas fields were interpolated to the exact times and positions of the observations to account for the actual weather conditions and hence for the specific histories of the sampled air masses. In this part of the study we focus on a detailed comparison with two selected campaigns, PEM-Tropics A and SONEX, contrasting the clean environment of the tropical Pacific with the more polluted North Atlantic region. The study highlights the different strengths and weaknesses of the models in accurately simulating key processes in the UT/LS region including stratosphere-troposphere-exchange, rapid convective transport, lightning emissions, radical chemistry and ozone production. Model simulated Radon, which was used as an idealized tracer for continental influence, was occasionally much better correlated with measured CO than simulated CO pointing towards deficiencies in the used biomass burning emission fields. The abundance and variability of HOx radicals is in general well represented in the models as inferred directly from the comparison with measured OH and HO2 and indirectly from the comparison with hydrogen peroxide concentrations. Components of the NOy family such as PAN, HNO3 and NO were found to compare less favorably. Interestingly, models showing good agreement with observations in the case of PEM-Tropics A often failed in the case of SONEX and vice versa. A better description of NOx and NOy emissions, chemistry and sinks is thought to be key to future model improvements with respect to the representation of chemistry in the UT/LS region.

This paper describes the global chemistry Transport Model, version 5 (TM5) which allows two-way nested zooming. The model is used for global studies which require high resolution regionally but can work on a coarser resolution globally. The zoom algorithm introduces refinement in both space and time in some predefined regions. Boundary conditions of the zoom region are provided by a coarser parent grid and the results of the zoom area are communicated back to the parent. A case study using 222Rn measurements that were taken during the MINOS campaign reveals the advantages of local zooming. As a next step, it is investigated to what extent simulated concentrations over Europe are influenced by using an additional zoom domain over North America. An artificial ozone-like tracer is introduced with a lifetime of twenty days and simplified non-linear chemistry. The concentration differences at Mace Head (Ireland) are generally smaller than 10%, much smaller than the effects of the resolution enhancement over Europe. Thus, coarsening of resolution at some distance of a sampling station seems allowed. However, it is also noted that the budgets of the tracers change considerably due to resolution dependencies of, for instance, vertical transport. Due to the two-way nested algorithm, TM5 offers a consistent tool to study the effects of grid refinement on global atmospheric chemistry issues like intercontinental transport of air pollution.

Characterizing cellular diversity at different levels of biological organization and across data modalities is a prerequisite to understanding the function of cell types in the brain. Classification of neurons is also essential to manipulate cell types in controlled ways and to understand their variation and vulnerability in brain disorders. The BRAIN Initiative Cell Census Network (BICCN) is an integrated network of data-generating centers, data archives, and data standards developers, with the goal of systematic multimodal brain cell type profiling and characterization. Emphasis of the BICCN is on the whole mouse brain with demonstration of prototype feasibility for human and nonhuman primate (NHP) brains. Here, we provide a guide to the cellular and spatial approaches employed by the BICCN, and to accessing and using these data and extensive resources, including the BRAIN Cell Data Center (BCDC), which serves to manage and integrate data across the ecosystem. We illustrate the power of the BICCN data ecosystem through vignettes highlighting several BICCN analysis and visualization tools. Finally, we present emerging standards that have been developed or adopted toward Findable, Accessible, Interoperable, and Reusable (FAIR) neuroscience. The combined BICCN ecosystem provides a comprehensive resource for the exploration and analysis of cell types in the brain.

The trend and interannual variability of methane sources are derived from multi-annual simulations of tropospheric photochemistry using a 3-D global chemistry-transport model. Our semi-inverse analysis uses the fifteen years (1979--1993) re-analysis of ECMWF meteorological data and annually varying emissions including photo-chemistry, in conjunction with observed CH4 concentration distributions and trends derived from the NOAA-CMDL surface stations. Dividing the world in four zonal regions (45--90 N, 0--45 N, 0--45 S, 45--90 S) we find good agreement in each region between (top-down) calculated emission trends from model simulations and (bottom-up) estimated anthropogenic emission trends based on the EDGAR global anthropogenic emission database, which amounts for the period 1979--1993 2.7 Tg CH4 yr-1. Also the top-down determined total global methane emission compares well with the total of the bottom-up estimates. We use the difference between the bottom-up and top-down determined emission trends to calculate residual emissions. These residual emissions represent the inter-annual variability of the methane emissions. Simulations have been performed in which the year-to-year meteorology, the emissions of ozone precursor gases, and the stratospheric ozone column distribution are either varied, or kept constant. In studies of methane trends it is most important to include the trends and variability of the oxidant fields. The analyses reveals that the variability of the emissions is of the order of 8Tg CH4 yr-1, and likely related to wetland emissions and/or biomass burning.

A rigorous evaluation of five global Chemistry-Transport and two Chemistry-Climate Models operated by several different groups in Europe, was performed. Comparisons were made of the models with trace gas observations from a number of research aircraft measurement campaigns during the four-year period 1995-1998. Whenever possible the models were run over the same four-year period and at each simulation time step the instantaneous tracer fields were interpolated to all coinciding observation points. This approach allows for a very close comparison with observations and fully accounts for the specific meteorological conditions during the measurement flights. This is important considering the often limited availability and representativity of such trace gas measurements. A new extensive database including all major research and commercial aircraft measurements between 1995 and 1998, as well as ozone soundings, was established specifically to support this type of direct comparison. Quantitative methods were applied to judge model performance including the calculation of average concentration biases and the visualization of correlations and RMS errors in the form of so-called Taylor diagrams. We present the general concepts applied, the structure and content of the database, and an overall analysis of model skills over four distinct regions. These regions were selected to represent various atmospheric conditions and to cover large geographical domains such that sufficient observations are available for comparison. The comparison of model results with the observations revealed specific problems for each individual model. This study suggests the further improvements needed and serves as a benchmark for re-evaluations of such improvements. In general all models show deficiencies with respect to both mean concentrations and vertical gradients of important trace gases. These include ozone, CO and NOx at the tropopause. Too strong two-way mixing across the tropopause is suggested to be the main reason for differences between simulated and observed CO and ozone values. The generally poor correlations between simulated and measured NOx values suggest that in particular the NOx input by lightning and the convective transport from the polluted boundary layer are still not well described by current parameterizations, which may lead to significant differences in the spatial and seasonal distribution of NOx in the models. Simulated OH concentrations, on the other hand, were found to be in surprisingly good agreement with measured values.

A new method has been developed that provides mass-conserving wind fields for global chemistry-transport models. In previous global Eulerian modeling studies a mass-imbalance was found between the model mass transport and the surface pressure tendencies. Several methods have been suggested to correct for this imbalance, but so far no satisfactory solution has been found. Our new method solves these problems by using the wind fields in a spherical harmonical form (divergence and vorticity) by mimicing the physics of the weather forecast model as closely as possible. A 3-D chemistry-transport model was used to show that the calculated ozone fields with the new processing method agree remarkably better with ozone observations in the upper troposphere and lower stratosphere. In addition, the calculated age of air in the lower stratosphere show better agreement with observations, although the air remains still too young in the extra-tropical stratosphere.

An observation by UHF ST radar of a subsidence pattern on the right side of the exit region of a jet streak is reported. The onset of the subsidence pattern occurred at 23:30 UTC on the 29 November 1991, when a downward motion was initiated above 14 km. The injections of stratospheric air in this region seem to have an intermittent nature; they occur during at least three intervals during the lifetime of the subsidence pattern. Comparison of these results with an ECMWF analysis suggests that it is an unfolding case. However, observation of turbulent intensities w' greater than 60 cm s–1 at the tropopause level also suggests the existence of a turbulent flux between the stratosphere and the troposphere. From the turbulence characteristics measured by the radar and the potential temperature profile obtained by radiosonde data, the eddy diffusivity at the tropopause level has been calculated. An eddy diffusion coefficient ranging between 5 and 7 m2 s–1 is found. From these values, and with the assumption of a climatological gradient of the volume mixing ratio of ozone in the lower stratosphere, it is possible to deduce a rough estimate of the amount of ozone injected from the stratosphere into the troposphere during this event. A rate of transfer of 1.5×1020 molecules of ozone per day and per square meter is found.

Childhood obesity is a growing global health concern. Although mobile health apps have the potential to deliver behavioural interventions, their impact is commonly limited by a lack of sufficient engagement. The purpose of this study was to explore barriers and facilitators to engagement with a family-focused app and its perceived impact on motivation, self-efficacy, and behaviour. Parents with at least one child under 18 and healthcare professionals working with children were recruited; all participants were allocated to use the NoObesity app over a 6-month period. The mixed-methods design was based on the Non-adoption, Abandonment, Scale-Up, Spread, and Sustainability and Reach, Effectiveness, Adoption, Implementation, and Maintenance frameworks. Qualitative and quantitative data were gathered through semi-structured interviews, questionnaires, and app use data (logins and in-app self-reported data). 35 parents were included in the final analysis; quantitative results were analysed descriptively and thematic analysis was conducted on the qualitative data. Key barriers to engagement were boredom, forgetting, and usability issues and key barriers to potential impact on behaviours were accessibility, lack of motivation, and family characteristics. Novelty, gamification features, reminders, goal setting, progress monitoring and feedback, and suggestions for healthy foods and activities were key facilitators to engagement with the app and behaviours. A key observation was that intervention strategies could help address many motivation and capability barriers, but there was a gap in strategies addressing opportunity barriers. Without incorporating strategies that successfully mitigate barriers in all three determinants of behaviour, an intervention is unlikely to be successful. We highlight key recommendations for developers to consider when designing the features and implementation of digital health interventions. Trial Registration: ClinicalTrials.gov (NCT05261555).