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The general objective of this series of papers is to evaluate long duration limited area simulations with idealised tracers as a tool to assess tracer transport in chemistry-transport models (CTMs). In this first paper, we analyse the results of six simulations using different convection closures and parameterizations. The simulations are using the Grell and Dévényi (2002) mass-flux framework for the convection parameterization with different closures (Grell = GR, Arakawa-Shubert = AS, Kain-Fritch = KF, Low omega = LO, Moisture convergence = MC) and an ensemble parameterization (EN) based on the other five closures. The simulations are run for one month during the SCOUT-O3 field campaign lead from Darwin (Australia). They have a 60 km horizontal resolution and a fine vertical resolution in the upper troposphere/lower stratosphere. Meteorological results are compared with satellite products, radiosoundings and SCOUT-O3 aircraft campaign data. They show that the model is generally in good agreement with the measurements with less variability in the model. Except for the precipitation field, the differences between the six simulations are small on average with respect to the differences with the meteorological observations. The comparison with TRMM rainrates shows that the six parameterizations or closures have similar behaviour concerning convection triggering times and locations. However, the 6 simulations provide two different behaviours for rainfall values, with the EN, AS and KF parameterizations (Group 1) modelling better rain fields than LO, MC and GR (Group 2). The vertical distribution of tropospheric tracers is very different for the two groups showing significantly more transport into the TTL for Group 1 related to the larger average values of the upward velocities. Nevertheless the low values for the Group 1 fluxes at and above the cold point level indicate that the model does not simulate significant overshooting. For stratospheric tracers, the differences between the two groups are small indicating that the downward transport from the stratosphere is more related to the turbulent mixing parameterization than to the convection parameterization.

The general objective of this series of two papers is to evaluate long duration limited-area simulations with idealised tracers as a possible tool to assess the tracer transport in chemistry-transport models (CTMs). In this second paper we analyse the results of three simulations using different horizontal and vertical resolutions. The goal is to study the impact of the model spatial resolution on convective transport of idealized tracer in the tropics. The reference simulation (REF) uses a 60 km horizontal resolution and 300 m vertically in the upper troposphere/lower stratosphere (UTLS). A 20 km horizontal resolution simulation (HR) is run as well as a simulation with 850 m vertical resolution in the UTLS (CVR). The simulations are run for one month during the SCOUT-O3 field campaign. Aircraft data, TRMM rainrate estimates and radiosoundings have been used to evaluate the simulations. They show that the HR configuration gives generally a better agreement with the measurements than the REF simulation. The CVR simulation gives generally the worst results. The vertical distribution of the tropospheric tracers for the simulations has a similar shape with a ~15 km altitude maximum for the 6h-lifetime tracer of 0.4 ppbv for REF, 1.2 for HR and 0.04 for CVR. These differences are related to the dynamics produced by the three simulations that leads to larger values of the upward velocities on average for HR and lower for CVR compared to REF. HR simulates more frequent and stronger convection leading to enhanced fluxes compared to REF and higher detrainment levels compared to CVR. HR provides also occasional overshoots over the cold point dynamical barrier. For the stratospheric tracers the differences between the three simulations are small. The diurnal cycle of the fluxes of all tracers in the Tropical Tropopause Layer exhibits a maximum linked to the maximum of convective activity.

Light-weight microlidar and water vapour measurements were taken on-board a stratospheric balloon during the HIBISCUS 2004 campaign, held in Bauru, Brazil (49° W, 22° S). Cirrus clouds were observed throughout the flight between 12 and 15 km height with a high mesoscale variability in optical and microphysical properties. It was found that the cirrus clouds were composed of different layers characterized by marked differences in height, thickness and optical properties. Simultaneous water vapour observations show that the different layers are characterized by different values of the saturation with respect to ice. A mesoscale simulation and a trajectory analysis clearly revealed that the clouds had formed in the outflow of a large and persistent convective region and that the observed variability of the optical properties and of the cloud structure is likely linked to the different residence times of the convectively-processed air in the upper troposphere.

In this study, we evaluate the ability of the BRAMS (Brazilian Regional Atmospheric Modeling System) mesoscale model compared to ECMWF global analysis to simulate the observed vertical variations of water vapour in the tropical upper troposphere and lower stratosphere (UTLS). The observations are balloon-borne measurements of water vapour mixing ratio and temperature from micro-SDLA (Tunable Diode Laser Spectrometer) instrument. Data from two balloon flights performed during the 2004 HIBISCUS field campaign are used to compare with the mesoscale simulations and to the ECMWF analysis. The observations exhibit fine scale vertical structures of water vapour of a few hundred meters height. The ECMWF vertical resolution (~1 km) is too coarse to capture these vertical structures in the UTLS. With a vertical resolution similar to ECMWF, the mesoscale model performs better than ECMWF analysis for water vapour in the upper troposphere and similarly or slightly worse for temperature. The BRAMS model with 250 m vertical resolution is able to capture more of the observed fine scale vertical variations of water vapour compared to runs with a coarser vertical resolution. This is mainly related to: (i) the enhanced vertical resolution in the UTLS and (ii) to the more detailed microphysical parameterization providing ice supersaturations as in the observations. In near saturated or supersaturated layers, the mesoscale model predicted relative humidity with respect to ice saturation is close to observations provided that the temperature profile is realistic. For temperature, the ECMWF analysis gives good results partly attributed to data assimilation. The analysis of the mesoscale model results showed that the vertical variations of the water vapour profile depends on the dynamics in unsaturated layer while the microphysical processes play a major role in saturated/supersaturated layers. In the lower stratosphere, the ECMWF model and the BRAMS model give very similar water vapour profiles that are significantly drier than micro-SDLA measurements. This similarity comes from the fact that BRAMS is initialised using ECMWF analysis and that no mesoscale process acts in the stratosphere leading to no modification of the BRAMS results with respect to ECMWF analysis.

In this second part of a series of two papers which aim to study the local impact of deep convection on the chemical composition of the Upper Troposphere and Lower Stratosphere (UTLS), we focus on ozone simulation results using a mesoscale model that includes on-line chemistry. A severe convective system observed on 8 February 2001 at Bauru, Brazil, is studied. This unorganised convective system is composed of several convective cells that interact with each other. We show that there is an increase in the ozone concentration in the tropical transitional layer (TTL) in the model during this event, which is compatible with ozone sonde observations from Bauru during the 2004 convective season. The model horizontal variability of ozone in this layer is comparable with the variability of the ozone sonde observations in the same area. The calculation of the ozone budget in the TTL during a 24 h period in the area of the convective system shows that the ozone behaviour in this layer is mainly driven by dynamics. The horizontal flux at a specific time is the main contribution in the budget, since it drives the sign and the magnitude of the total ozone flux. However, when averaged over the 24 h period, the horizontal flux is smaller than the vertical fluxes, and leads to a net decrease of ozone molecule number of 23%. The upward motions at the bottom of the TTL, related to the convection activity is the main contributor to the budget over the 24h period since it can explain 70% of the total ozone increase in the TTL, while the chemical ozone production inside the TTL is estimated to be 29% of the ozone increase, if NOx production by lightning (LNOx) is taken into account. It is shown that downward motion at the tropopause induced by gravity waves generated by deep convection is non negligible in the TTL ozone budget, since it represents 24% of the ozone increase. The flux analysis shows the importance of the vertical contributions during the life time of the convective event (about 8 h). The TTL ozone is driven out of the domain horizontally by the convective outflow during this period, limiting the ozone increase in this layer.

The aim of this work is to study the local impact on the upper troposphere/lower stratosphere air composition of an extreme deep convective system. For this purpose, we performed a simulation of a convective cluster composed of many individual deep convective cells that occurred near Bauru (Brazil). The simulation is performed using the 3-D mesoscale model RAMS coupled on-line with a chemistry model. The comparisons with meteorological measurements show that the model produces meteorological fields generally consistent with the observations. The present paper (part I) is devoted to the analysis of the ozone precursors (CO, NOx and non-methane volatile organic compounds) and HOx in the UTLS. The simulation results show that the distribution of CO with altitude is closely related to the upward convective motions and consecutive outflow at the top of the convective cells leading to a bulge of CO between 7 km altitude and the tropopause (around 17 km altitude). The model results for CO are consistent with satellite-borne measurements at 700 hPa. The simulation also indicates enhanced amounts of NOx up to 2 ppbv in the 7–17 km altitude layer mainly produced by the lightning associated with the intense convective activity. For insoluble non-methane volatile organic compounds, the convective activity tends to significantly increase their amount in the 7–17 km layer by dynamical effects. During daytime in the presence of lightning NOx, this bulge is largely reduced in the upper part of the layer for reactive species (e.g. isoprene, ethene) because of their reactions with OH that is increased on average during daytime. Lightning NOx also impacts on the oxydizing capacity of the upper troposphere by reducing on average HOx, HO2, H2O2 and organic hydroperoxides. During the simulation time, the impact of convection on the air composition of the lower stratosphere is negligible for all ozone precursors although several of the simulated convective cells nearly reach the tropopause. There is no significant transport from the upper troposphere to the lower stratosphere, the isentropic barrier not being crossed by convection. The impact of the increase of ozone precursors and HOx in the upper troposphere on the ozone budget in the LS is discussed in part II of this series of papers.

We have derived values of the Ultraviolet Index (UVI) at solar noon using the Tropospheric Ultraviolet Model (TUV) driven by ozone, temperature and aerosol fields from climate simulations of the first phase of the Chemistry-Climate Model Initiative (CCMI-1). Since clouds remain one of the largest uncertainties in climate projections, we simulated only the clear-sky UVI. We compared the modelled UVI climatologies against present-day climatological values of UVI derived from both satellite data (the OMI-Aura OMUVBd product) and ground-based measurements (from the NDACC network). Depending on the region, relative differences between the UVI obtained from CCMI/TUV calculations and the ground-based measurements ranged between -5.9% and 10.6%. We then calculated the UVI evolution throughout the 21st century for the four Representative Concentration Pathways (RCPs 2.6, 4.5, 6.0 and 8.5). Compared to 1960s values, we found an average increase in the UVI in 2100 (of 2-4%) in the tropical belt (30°N-30°S). For the mid-latitudes, we observed a 1.8 to 3.4 % increase in the Southern Hemisphere for RCP 2.6, 4.5 and 6.0, and found a 2.3% decrease in RCP 8.5. Higher increases in UVI are projected in the Northern Hemisphere except for RCP 8.5. At high latitudes, ozone recovery is well identified and induces a complete return of mean UVI levels to 1960 values for RCP 8.5 in the Southern Hemisphere. In the Northern Hemisphere, UVI levels in 2100 are higher by 0.5 to 5.5% for RCP 2.6, 4.5 and 6.0 and they are lower by 7.9% for RCP 8.5. We analysed the impacts of greenhouse gases (GHGs) and ozone-depleting substances (ODSs) on UVI from 1960 by comparing CCMI sensitivity simulations (1960-2100) with fixed GHGs or ODSs at their respective 1960 levels. As expected with ODS fixed at their 1960 levels, there is no large decrease in ozone levels and consequently no sudden increase in UVI levels. With fixed GHG, we observed a delayed return of ozone to 1960 values, with a corresponding pattern of change observed on UVI, and looking at the UVI difference between 2090s values and 1960s values, we found an 8 % increase in the tropical belt during the summer of each hemisphere. Finally we show that, while in the Southern Hemisphere the UVI is mainly driven by total ozone column, in the Northern Hemisphere both total ozone column and aerosol optical depth drive UVI levels, with aerosol optical depth having twice as much influence on the UVI as total ozone column does.