Biogenic volatile organic compounds (BVOCs) emitted from the terrestrial vegetation into the Earth's atmosphere play an important role in atmospheric chemical processes. Gridded information of their temporal and spatial distribution is therefore needed for proper representation of the atmospheric composition by the air quality models. Here we present three newly developed high-resolution global emission inventories of the main BVOC species including isoprene, monoterpenes, sesquiterpenes, methanol, acetone and ethene. Monthly mean and monthly averaged daily profile emissions were calculated by the Model of Emission of Gases and Aerosols from Nature (MEGANv2.1) driven by meteorological reanalyses of the European Centre for Medium-Range Weather Forecasts for the period of 2000–2019. The dataset CAMS-GLOB-BIOv1.2 is based on ERA-Interim meteorology (0.5^∘ × 0.5^∘ horizontal spatial resolution); the datasets CAMS-GLOB-BIOv3.0 and v3.1 were calculated with ERA5 (both 0.25^∘ × 0.25^∘ horizontal spatial resolution). Furthermore, European isoprene emission potential data were updated using high-resolution land cover maps and detailed information of tree species composition and emission factors from the EMEP MSC-W model system. Updated isoprene emissions are included in the CAMS-GLOB-BIOv3.1 dataset. The effect of annually changing land cover on BVOC emissions is captured by the CAMS-GLOB-BIOv3.0 as it was calculated with land cover data provided by the Climate Change Initiative of the European Space Agency (ESA-CCI). The global total annual BVOC emissions averaged over the simulated period vary between the datasets from 424 to 591 Tg (C) yr⁻¹, with isoprene emissions from 299.1 to 440.5 Tg (isoprene) yr⁻¹. Differences between the datasets and variation in their emission estimates provide the emission uncertainty range and the main sources of uncertainty, i.e. meteorological inputs, emission potential data and land cover description. The CAMS-GLOB-BIO time series of isoprene and monoterpenes were compared to other available data. There is a general agreement in an interannual variability in the emission estimates, and the values fall within the uncertainty range. The CAMS-GLOB-BIO datasets (CAMS-GLOB-BIOv1.2, https://doi.org/10.24380/t53a-qw03, Sindelarova et al., 2021a; CAMS-GLOB-BIOv3.0, https://doi.org/10.24380/xs64-gj42, Sindelarova et al., 2021b; CAMS-GLOB-BIOv3.1, https://doi.org/10.24380/cv4p-5f79, Sindelarova et al., 2021c) are distributed from the Emissions of atmospheric Compounds and Compilation of Ancillary Data (ECCAD) system (https://eccad.aeris-data.fr/, last access: June 2021).

In recent years, the PALM 6.0 modelling system has been rapidly developing its capability to simulate physical processes within urban environments. Some examples in this regard are energy-balance solvers for building and land surfaces, a radiative transfer model to account for multiple reflections and shading, a plant-canopy model to consider the effects of plants on flow (thermo)dynamics, and a chemistry transport model to enable simulation of air quality. This study provides a thorough evaluation of modelled meteorological, air chemistry, and ground and wall-surface quantities against dedicated in situ measurements taken in an urban environment in Dejvice, Prague, the Czech Republic. Measurements included monitoring of air quality and meteorology in street canyons, surface temperature scanning with infrared cameras, and monitoring of wall heat fluxes. Large-eddy simulations (LES) using the PALM model driven by boundary conditions obtained from a mesoscale model were performed for multiple days within two summer and three winter episodes characterized by different atmospheric conditions. For the simulated episodes, the resulting temperature, wind speed, and chemical compound concentrations within street canyons show a realistic representation of the observed state, except that the LES did not adequately capture night-time cooling near the surface for certain meteorological conditions. In some situations, insufficient turbulent mixing was modelled, resulting in higher near-surface concentrations. At most of the evaluation points, the simulated surface temperature reproduces the observed surface temperature reasonably well for both absolute and daily amplitude values. However, especially for the winter episodes and for modern buildings with multilayer walls, the heat transfer through walls is not well captured in some cases, leading to discrepancies between the modelled and observed wall-surface temperature. Furthermore, the study corroborates model dependency on the accuracy of the input data. In particular, the temperatures of surfaces affected by nearby trees strongly depend on the spatial distribution of the leaf area density, land surface temperatures at grass surfaces strongly depend on the initial soil moisture, wall-surface temperatures depend on the correct setting of wall material parameters, and concentrations depend on detailed information on spatial distribution of emissions, all of which are often unavailable at sufficient accuracy. The study also points out some current model limitations, particularly the implications of representing topography and complex heterogeneous facades on a discrete Cartesian grid, and glass facades that are not fully represented in terms of radiative processes. Our findings are able to validate the representation of physical processes in PALM while also pointing out specific shortcomings. This will help to build a baseline for future developments of the model and improvements of simulations of physical processes in an urban environment.

Rising emissions of anthropogenic greenhouse gases (GHG) have led to tropospheric warming and stratospheric cooling over recent decades. As a thermodynamic consequence, the troposphere has expanded and the rise of the tropopause, the boundary between the troposphere and stratosphere, has been suggested as one of the most robust fingerprints of anthropogenic climate change. Conversely, at altitudes above ∼55 km (in the mesosphere and thermosphere) observational and modeling evidence indicates a downward shift of the height of pressure levels or decreasing density at fixed altitudes. The layer in between, the stratosphere, has not been studied extensively with respect to changes of its global structure. Here we show that this atmospheric layer has contracted substantially over the last decades, and that the main driver for this are increasing concentrations of GHG. Using data from coupled chemistry-climate models we show that this trend will continue and the mean climatological thickness of the stratosphere will decrease by 1.3 km following representative concentration pathway 6.0 by 2080. We also demonstrate that the stratospheric contraction is not only a response to cooling, as changes in both tropopause and stratopause pressure contribute. Moreover, its short emergence time (less than 15 years) makes it a novel and independent indicator of GHG induced climate change.

In general, regional and global chemistry transport models apply instantaneous mixing of emissions into the model's finest resolved scale. In case of a concentrated source, this could result in erroneous calculation of the evolution of both primary and secondary chemical species. Several studies discussed this issue in connection with emissions from ships and aircraft. In this study, we present an approach to deal with the non-linear effects during dispersion of NO_x emissions from ships. It represents an adaptation of the original approach developed for aircraft NO_x emissions, which uses an exhaust tracer to trace the amount of the emitted species in the plume and applies an effective reaction rate for the ozone production/destruction during the plume's dilution into the background air. In accordance with previous studies examining the impact of international shipping on the composition of the troposphere, we found that the contribution of ship induced surface NO_x to the total reaches 90% over remote ocean and makes 10–30% near coastal regions. Due to ship emissions, surface ozone increases by up to 4–6 ppbv making 10% contribution to the surface ozone budget. When applying the ship plume parameterization, we show that the large scale NO_x decreases and the ship NO_x contribution is reduced by up to 20–25%. A similar decrease was found in the case of O₃. The plume parameterization suppressed the ship induced ozone production by 15–30% over large areas of the studied region. To evaluate the presented parameterization, nitrogen monoxide measurements over the English Channel were compared with modeled values and it was found that after activating the parameterization the model accuracy increases.

Cities are characterized by different physical properties of surface compared to their rural counterparts, resulting in a specific regime of the meteorological phenomenon. Our study aims to evaluate the impact of typical urban surfaces on the central European urban climate in several model simulations, performed with the Weather Research and Forecasting (WRF) model and Regional Climate Model (RegCM). The specific processes occurring in the typical urban environment are described in the models by various types of urban parameterizations, greatly differing in complexity. Our results show that all models and urban parameterizations are able to reproduce the most typical urban effect, the summer evening and nocturnal urban heat island, with the average magnitude of 2–3 °C. The impact of cities on the wind is clearly dependent on the urban parameterization employed, with more simple ones unable to fully capture the wind speed reduction induced by the city. In the summer, a significant difference in the boundary-layer height (about 25 %) between models is detected. The urban-induced changes of temperature and wind speed are propagated into higher altitudes up to 2 km, with a decreasing tendency of their magnitudes. With the exception of the daytime in the summer, the urban environment improves the weather conditions a little with regard to the pollutant dispersion, which could lead to the partly decreased concentration of the primary pollutants.

It is well known that the urban canopy (UC) layer, i.e., the layer of air corresponding to the assemblage of the buildings, roads, park, trees and other objects typical to cities, is characterized by specific meteorological conditions at city scales generally differing from those over rural surroundings. We refer to the forcing that acts on the meteorological variables over urbanized areas as the urban canopy meteorological forcing (UCMF). UCMF has multiple aspects, while one of the most studied is the generation of the urban heat island (UHI) as an excess of heat due to increased absorption and trapping of radiation in street canyons. However, enhanced drag plays important role too, reducing mean wind speeds and increasing vertical eddy mixing of pollutants. As air quality is strongly tied to meteorological conditions, the UCMF leads to modifications of air chemistry and transport of pollutants. Although it has been recognized in the last decade that the enhanced vertical mixing has a dominant role in the impact of the UCMF on air quality, very little is known about the uncertainty of vertical eddy diffusion arising from different representation in numerical models and how this uncertainty propagates to the final species concentrations as well as to the changes due to the UCMF. To bridge this knowledge gap, we set up the Regional Climate Model version 4 (RegCM4) coupled to the Comprehensive Air Quality Model with Extensions (CAMx) chemistry transport model over central Europe and designed a series of simulations to study how UC affects the vertical turbulent transport of selected pollutants through modifications of the vertical eddy diffusion coefficient (K_v) using six different methods for K_v calculation. The mean concentrations of ozone and PM_2.5 in selected city canopies are analyzed. These are secondary pollutants or having secondary components, upon which turbulence acts in a much more complicated way than in the case of primary pollutants by influencing their concentrations not only directly but indirectly via precursors too. Calculations are performed over cascading domains (of 27, 9, and 3 km horizontal resolutions), which further enables to analyze the sensitivity of the numerical model to grid resolution. A number of model simulations are carried out where either urban canopies are considered or replaced by rural ones in order to isolate the UC meteorological forcing. Apart from the well-pronounced and expected impact on temperature (increases up to 2 ^∘C) and wind (decreases by up to 2 ms⁻¹), there is a strong impact on vertical eddy diffusion in all of the six K_v methods. The K_v enhancement ranges from less than 1 up to 30 m² s⁻¹ at the surface and from 1 to 100 m² s⁻¹ at higher levels depending on the methods. The largest impact is obtained for the turbulent kinetic energy (TKE)-based methods. The range of impact on the vertical eddy diffusion coefficient propagates to a range of ozone (O₃) increase of 0.4 to 4 ppbv in both summer and winter (5 %–10 % relative change). In the case of PM_2.5, we obtained decreases of up to 1 µg m⁻³ in summer and up to 2 µg m⁻³ in winter (up to 30 %–40 % relative change). Comparing these results to the “total-impact”, i.e., to the impact of all meteorological modifications due to UCMF, we can conclude that much of UCMF is explained by the enhanced vertical eddy diffusion, which counterbalances the opposing effects of other components of this forcing (temperature, humidity and wind). The results further show that this conclusion holds regardless of the resolution chosen and in both the warm and cold parts of the year.