Representation of tropical deep convection in atmospheric models - Part 1 : Meteorology and comparison with satellite observations

Published under Creative Commons Licence 3.0. Original article can be found at : http://www.atmospheric-chemistry-and-physics.net/ "The author's copyright for this publication is transferred to University of Hertfordshire".Fast convective transport in the tropics can efficiently redistribute water vapour and pollutants up to the upper troposphere. In this study we compare tropical convection characteristics for the year 2005 in a range of atmospheric models, including numerical weather prediction (NWP) models, chemistry transport models (CTMs), and chemistry-climate models (CCMs). The model runs have been performed within the framework of the SCOUT-O3 (Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere) project. The characteristics of tropical convection, such as seasonal cycle, land/sea contrast and vertical extent, are analysed using satellite observations as a benchmark for model simulations. The observational datasets used in this work comprise precipitation rates, outgoing longwave radiation, cloud-top pressure, and water vapour from a number of independent sources, including ERA-Interim analyses. Most models are generally able to reproduce the seasonal cycle and strength of precipitation for continental regions but show larger discrepancies with observations for the Maritime Continent region. The frequency distribution of high clouds from models and observations is calculated using highly temporally-resolved (up to 3-hourly) cloud top data. The percentage of clouds above 15 km varies significantly between the models. Vertical profiles of water vapour in the upper troposphere-lower stratosphere (UTLS) show large differences between the models which can only be partly attributed to temperature differences. If a convective plume reaches above the level of zero net radiative heating, which is estimated to be ~15 km in the tropics, the air detrained from it can be transported upwards by radiative heating into the lower stratosphere. In this context, we discuss the role of tropical convection as a precursor for the transport of short-lived species into the lower stratosphere.Peer reviewe

Halogen chemistry in volcanic plumes: a 1D framework based on MOCAGE 1D (version R1.18.1) preparing 3D global chemistry modelling

HBr emissions from volcanoes lead rapidly to the formation of BrO within volcanic plumes and have an impact on tropospheric chemistry, at least at the local and regional scales. The motivation of this paper is to prepare a framework for further 3D modelling of volcanic halogen emissions in order to determine their fate within the volcanic plume and then in the atmosphere at the regional and global scales. The main aim is to evaluate the ability of the model to produce a realistic partitioning of bromine species within a grid box size typical of MOCAGE (Model Of atmospheric Chemistry At larGE scale) 3D (0.5×0.5). This work is based on a 1D single-column configuration of the global chemistry-transport model MOCAGE that has low enough computational cost to allow us to perform a large set of sensitivity simulations. This paper uses the emissions from the Mount Etna eruption on 10 May 2008. Several reactions are added to MOCAGE to represent the volcanic plume halogen chemistry. A simple plume parameterisation is also implemented and tested. The use of this parameterisation tends to only slightly limit the efficiency of BrO net production. Both simulations with and without the parameterisation give results for the partitioning of the bromine species, of ozone depletion and of the BrO/SO2 ratio that are consistent with previous studies. A series of test experiments were performed to evaluate the sensitivity of the results to the composition of the emissions (primary sulfate aerosols, Br radical and NO) and to the effective radius assumed for the volcanic sulfate aerosols. Simulations show that the plume chemistry is sensitive to all these parameters. We also find that the maximum altitude of the eruption changes the BrO production, which is linked to the vertical variability of the concentrations of oxidants in the background air. These sensitivity tests display changes in the bromine chemistry cycles that are generally at least as important as the plume parameterisation. Overall, the version of the MOCAGE chemistry developed for this study is suitable to produce the expected halogen chemistry in volcanic plumes during daytime and night-time

PREP-CHEM-SRC – 1.0: a preprocessor of trace gas and aerosol emission fields for regional and global atmospheric chemistry models

The preprocessor PREP-CHEM-SRC presented in the paper is a comprehensive tool aiming at preparing emission fields of trace gases and aerosols for use in atmospheric-chemistry transport models. The considered emissions are from the most recent databases of urban/industrial, biogenic, biomass burning, volcanic, biofuel use and burning from agricultural waste sources. For biomass burning, emissions can be also estimated directly from satellite fire detections using a fire emission model included in the tool. The preprocessor provides emission fields interpolated onto the transport model grid. Several map projections can be chosen. The inclusion of these emissions in transport models is also presented. The preprocessor is coded using Fortran90 and C and is driven by a <i>namelist</i> allowing the user to choose the type of emissions and the databases

Description and Evaluation of the specified-dynamics experiment in the Chemistry-Climate Model Initiative

We provide an overview of the REF-C1SD specified-dynamics experiment that was conducted as part of phase 1 of the Chemistry-Climate Model Initiative (CCMI). The REF-C1SD experiment, which consisted of mainly nudged general circulation models (GCMs) constrained with (re)analysis fields, was designed to examine the influence of the large-scale circulation on past trends in atmospheric composition. The REF-C1SD simulations were produced across various model frameworks and are evaluated in terms of how well they represent different measures of the dynamical and transport circulations. In the troposphere there are large (∼40 %) differences in the climatological mean distributions, seasonal cycle amplitude, and trends of the meridional and vertical winds. In the stratosphere there are similarly large (∼50 %) differences in the magnitude, trends and seasonal cycle amplitude of the transformed Eulerian mean circulation and among various chemical and idealized tracers. At the same time, interannual variations in nearly all quantities are very well represented, compared to the underlying reanalyses. We show that the differences in magnitude, trends and seasonal cycle are not related to the use of different reanalysis products; rather, we show they are associated with how the simulations were implemented, by which we refer both to how the large-scale flow was prescribed and to biases in the underlying free-running models. In most cases these differences are shown to be as large or even larger than the differences exhibited by free-running simulations produced using the exact same models, which are also shown to be more dynamically consistent. Overall, our results suggest that care must be taken when using specified-dynamics simulations to examine the influence of large-scale dynamics on composition

The Impact of Recent European Droughts and Heatwaves on Trace Gas Surface Fluxes: Insights from Land Surface Data Assimilation

Heatwave and drought extremes can have significant impacts on vegetation, which can in turn lead to important effects on reactive trace gas fluxes at the land-atmosphere interface that can ultimately alter atmospheric composition. We present results from the EU-funded Sentinel EObased Emission and Deposition Service (SEEDS) project, which aimed at developing upgrades to the existing Copernicus Atmospheric Monitoring Service (CAMS) component on European air quality. In this work, we used land surface modelling (SURFEX – Surface Externalisée) combined with data assimilation (Extended Kalman Filter - EKF) of satellite leaf area index (LAI) to deliver improved estimation of the land surface state. The land surface model is coupled with an online model for dry deposition and an offline model (MEGANv3.1) for biogenic volatile organic compounds (BVOCs) to estimate trace gas losses and emissions, respectively. This approach exploits methods at the forefront of land surface modelling (dynamic vegetation simulation and data assimilation) and combines them with the latest algorithms to estimate trace gas fluxes at the surface. We present findings from two extreme events in Europe: the 2018 drought and the 2019 June/July heat waves. SURFEX was forced using ECMWF meteorology at 0.1° × 0.1° resolution that captured both events. Both extreme events provoked strong responses in the models for dry deposition velocity and BVOC emissions. The 2018 drought began in spring and endured through summer, during which dry deposition velocities declined steadily beyond seasonal norms due to increased stomatal resistance forced by the vegetation response to drought. Over continental Europe, BVOCs initially increased in the early phase of the drought, but then sharply declined into July in the worst-affected regions in Germany, Denmark, and Poland. Meanwhile, BVOCs increased in Scandinavia relative to seasonal norms due to the warmer-than-average conditions. The first episode of severe heat in 2019 arrived in late June, which initially caused a large increase in BVOC emissions compared to seasonal norms. Then drought set in during July and despite a second large heat wave BVOC emissions were lower overall compared to seasonal norms. In fact, the European-wide BVOC emissions were higher in June compared to July due to the drought effects that commenced later in the heat wave cycle. This reverses the normal seasonal cycle in BVOC emissions, and drought impacts on vegetation were the primary driver behind this. Dry deposition velocities are reduced during both heat waves, but we see a larger decline in the second heat wave in July when drought conditions are more severe. Our findings suggest that these impacts on trace gas surface fluxes would have a strong effect on atmospheric composition, and on photochemical ozone formation. We, therefore, conclude that these effects likely played a contributory role to the ozone pollution episodes that occurred coincidentally in time with the heat wave events in both 2018 and 2019. The project aim within SEEDS is to eventually test the BVOC emissions and dry deposition velocities within a chemical transport model participating within the CAMS regional ensemble (MOCAGE) and to therefore evaluate the impact on ozone

First implementation of secondary inorganic aerosols in the MOCAGE version R2.15.0 chemistry transport model

In this study we develop a secondary inorganic aerosol (SIA) module for the MOCAGE chemistry transport model developed at CNRM. The aim is to have a module suitable for running at different model resolutions and for operational applications with reasonable computing times. Based on the ISORROPIA II thermodynamic equilibrium module, the new version of the model is presented and evaluated at both the global and regional scales. The results show high concentrations of secondary inorganic aerosols in the most polluted regions: Europe, Asia and the eastern part of North America. Asia shows higher sulfate concentrations than other regions thanks to emission reductions in Europe and North America. Using two simulations, one with and the other without secondary inorganic aerosol formation, the global model outputs are compared to previous studies, to MODIS AOD retrievals, and also to in situ measurements from the HTAP database. The model shows a better agreement with MODIS AOD retrievals in all geographical regions after introducing the new SIA scheme. It also provides a good statistical agreement with in situ measurements of secondary inorganic aerosol composition: sulfate, nitrate and ammonium. In addition, the simulation with SIA generally gives a better agreement with observations for secondary inorganic aerosol precursors (nitric acid, sulfur dioxide, ammonia), in particular with a reduction of the modified normalized mean bias (MNMB). At the regional scale, over Europe, the model simulation with SIA is compared to the in situ measurements from the EMEP database and shows a good agreement with secondary inorganic aerosol composition. The results at the regional scale are consistent with those obtained from the global simulations. The AIRBASE database was used to compare the model to regulated air quality pollutants: particulate matter, ozone and nitrogen dioxide concentrations. Introduction of the SIA in MOCAGE provides a reduction in the PM2.5 MNMB of 0.44 on a yearly basis and up to 0.52 for the 3 spring months (March, April, May) when SIAs are at their maximum

Tropospheric chemistry in the Integrated Forecasting System of ECMWF

A representation of atmospheric chemistry has been included in the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The new chemistry modules complement the aerosol modules of the IFS for atmospheric composition, which is named C-IFS. C-IFS for chemistry supersedes a coupled system in which chemical transport model (CTM) Model for OZone and Related chemical Tracers 3 was two-way coupled to the IFS (IFS-MOZART). This paper contains a description of the new on-line implementation, an evaluation with observations and a comparison of the performance of C-IFS with MOZART and with a re-analysis of atmospheric composition produced by IFS-MOZART within the Monitoring Atmospheric Composition and Climate (MACC) project. The chemical mechanism of C-IFS is an extended version of the Carbon Bond 2005 (CB05) chemical mechanism as implemented in CTM Transport Model 5 (TM5). CB05 describes tropospheric chemistry with 54 species and 126 reactions. Wet deposition and lightning nitrogen monoxide (NO) emissions are modelled in C-IFS using the detailed input of the IFS physics package. A 1 year simulation by C-IFS, MOZART and the MACC re-analysis is evaluated against ozonesondes, carbon monoxide (CO) aircraft profiles, European surface observations of ozone (O3), CO, sulfur dioxide (SO2) and nitrogen dioxide (NO2) as well as satellite retrievals of CO, tropospheric NO2 and formaldehyde. Anthropogenic emissions from the MACC/CityZen (MACCity) inventory and biomass burning emissions from the Global Fire Assimilation System (GFAS) data set were used in the simulations by both C-IFS and MOZART. C-IFS (CB05) showed an improved performance with respect to MOZART for CO, upper tropospheric O3, and wintertime SO2, and was of a similar accuracy for other evaluated species. C-IFS (CB05) is about 10 times more computationally efficient than IFS-MOZAR

Tropical deep convection and its impact on composition in global and mesoscale models - Part 2: Tracer transport

The tropical transport processes of 14 different models or model versions were compared, within the framework of the SCOUT-O3 (Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere) project. The tested models range from the regional to the global scale, and include numerical weather prediction (NWP), chemistry transport, and climate chemistry models. Idealised tracers were used in order to prevent the model's chemistry schemes from influencing the results substantially, so that the effects of modelled transport could be isolated. We find large differences in the vertical transport of very short lived tracers (with a lifetime of 6 hours) within the tropical troposphere. Peak convective outflow altitudes range from around 300 hPa to almost 100 hPa among the different models, and the upper tropospheric tracer mixing ratios differ by up to an order of magnitude. The timing of convective events is found to differ between the models, even among those which source their forcing data from the same NWP model (ECMWF). The differences are less pronounced for longer lived tracers, however they could have implications for the modelling of the halogen burden of the lowermost stratosphere through species such as bromoform, or for the transport of short lived hydrocarbons into the lowermost stratosphere. The modelled tracer profiles are found to be strongly influenced by the convective transport parameterisations, and boundary layer mixing parameterisations of the models. The location of rapid transport into the upper troposphere is similar among the models, and is mostly concentrated over the western Pacific, the Maritime Continent and the Indian Ocean. In contrast, none of the models indicates significant enhancement in upward transport over western Africa. The mean mixing ratios of an idealised CO like tracer in the upper tropical troposphere are found to be sensitive to the surface CO mixing ratios in the regions with the most active convection, revealing the importance of correctly modelling both the location of convective transport and the geographical pollutant emission patterns