ALBERT

Description: 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.

Description: We present a "nudged" version of the Met Office general circulation model, the Unified Model. We constrain this global climate model using ERA-40 re-analysis data with the aim of reproducing the observed "weather" over a year from September 1999. Quantitative assessments are made of its performance, focusing on dynamical aspects of nudging and demonstrating that the "weather" is well simulated.

Description: We examine the effects of ozone precursor emissions from megacities on present-day air quality using the global chemistry–climate model UM-UKCA (UK Met Office Unified Model coupled to the UK Chemistry and Aerosols model). The sensitivity of megacity and regional ozone to local emissions, both from within the megacity and from surrounding regions, is important for determining air quality across many scales, which in turn is key for reducing human exposure to high levels of pollutants. We use two methods, perturbation and tagging, to quantify the impact of megacity emissions on global ozone. We also completely redistribute the anthropogenic emissions from megacities, to compare changes in local air quality going from centralised, densely populated megacities to decentralised, lower density urban areas. Focus is placed not only on how changes to megacity emissions affect regional and global NOx and O3, but also on changes to NOy deposition and to local chemical environments which are perturbed by the emission changes. The perturbation and tagging methods show broadly similar megacity impacts on total ozone, with the perturbation method underestimating the contribution partially because it perturbs the background chemical environment. The total redistribution of megacity emissions locally shifts the chemical environment towards more NOx-limited conditions in the megacities, which is more conducive to ozone production, and monthly mean surface ozone is found to increase up to 30% in megacities, depending on latitude and season. However, the displacement of emissions has little effect on the global annual ozone burden (0.12% change). Globally, megacity emissions are shown to contribute ~3% of total NOy deposition. The changes in O3, NOx and NOy deposition described here are useful for quantifying megacity impacts and for understanding the sensitivity of megacity regions to local emissions. The small global effects of the 100% redistribution carried out in this study suggest that the distribution of emissions on the local scale is unlikely to have large implications for chemistry–climate processes on the global scale.

Description: 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.

Description: In the 1990s the rates of increase of greenhouse gas concentrations, most notably of methane, were observed to change, for reasons that have yet to be fully determined. This period included the eruption of Mt. Pinatubo and an El Niño warm event, both of which affect biogeochemical processes, by changes in temperature, precipitation and radiation. We examine the impact of these changes in climate on global isoprene emissions and the effect these climate dependent emissions have on the hydroxy radical, OH, the dominant sink for methane. We model a reduction of isoprene emissions in the early 1990s, with a maximum decrease of 40 Tg(C)/yr in late 1992 and early 1993, a change of 9%. This reduction is caused by the cooler, drier conditions following the eruption of Mt. Pinatubo. Isoprene emissions are reduced both directly, by changes in temperature and a soil moisture dependent suppression factor, and indirectly, through reductions in the total biomass. The reduction in isoprene emissions causes increases of tropospheric OH which lead to an increased sink for methane of up to 5 Tg(CH4)/year, comparable to estimated source changes over the time period studied. There remain many uncertainties in the emission and oxidation of isoprene which may affect the exact size of this effect, but its magnitude is large enough that it should remain important.

Description: Evaluation of the aerosol schemes in current climate models is dependent upon the available observational data. In-situ observations from flight campaigns can provide valuable data about the vertical distribution of aerosol that is difficult to obtain from satellite or ground-based platforms, although they are localised in space and time. Using single-particle soot-photometer (SP2) measurements from the HIAPER Pole-to-Pole Observations (HIPPO) campaign, which consists of many vertical profiles over a large region of the Pacific, we evaluate the meridional and vertical distribution of black carbon (BC) aerosol simulated by the HadGEM3–UKCA and ECHAM5–HAM2 models. Both models show a similar pattern of overestimating the BC column burden compared to that derived from the observations, in many areas by an order of magnitude. However, by sampling the simulated BC mass mixing ratio along the flight track and comparing to the observations, we show that this discrepancy has a rather different vertical structure in the two models: in HadGEM3–UKCA the discrepancy is dominated by excess aerosol in the tropical upper troposphere, while in ECHAM5–HAM2 areas of discrepancy are spread across many different latitudes and altitudes. Using this methodology, we conduct sensitivity tests on two specific elements of the models: biomass-burning emissions and scavenging by convective precipitation. We show that, by coupling the convective scavenging more tightly with convective transport, both the column burden and vertical distribution of BC in HadGEM3–UKCA are much improved with respect to the observations, with a substantial and statistically significant increase in correlation – this demonstrates the importance of a realistic representation of this process. In contrast, updating from GFED2 to GFED3.1 biomass-burning emissions makes a more modest improvement in both models, which is not statistically significant. By comparing our results with a more traditional approach using regional- and monthly-mean vertical profile curves, we show that the point-by-point analysis allows the model improvements to be demonstrated more clearly. We also demonstrate the important role that nudged simulations (where the large-scale model dynamics are continuously relaxed towards a reanalysis) can play in this type of evaluation, allowing statistically significant differences between configurations of the aerosol scheme to be seen where the differences between the corresponding free-running simulations would not be significant.

Description: 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), chemical transport, and chemistry-climate 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 h) 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 be different 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 modelling the halogen burden of the lowermost stratosphere through transport of species such as bromoform, or short-lived hydrocarbons into the lowermost stratosphere. The modelled tracer profiles are strongly influenced by the convective transport parameterisations, and different boundary layer mixing parameterisations also have a large impact on the modelled tracer profiles. Preferential locations for rapid transport from the surface into the upper troposphere are similar in all models, and are mostly concentrated over the western Pacific, the Maritime Continent and the Indian Ocean. In contrast, models do not indicate that upward transport is highest over western Africa.

Description: The correlation between measured tropospheric ozone (O3) and carbon monoxide (CO) has been used extensively in tropospheric chemistry studies to explore the photochemical characteristics of different regions and to evaluate the ability of models to capture these characteristics. Here, we present the first study that uses multi-year, global, vertically resolved, simultaneous and collocated O3 and CO satellite (Tropospheric Emission Spectrometer) measurements, to determine this correlation in the middle/lower free troposphere for two different seasons, and to evaluate two chemistry-climate models. We find results that are fairly robust across different years, altitudes and timescales considered, which indicates that the correlation maps presented here could be used in future model evaluations. The highest positive correlations (around 0.8) are found in the northern Pacific during summer, which is a common feature in the observations and the G-PUCCINI model. We make quantitative comparisons between the models using a single-figure metric (C), which we define as the correlation coefficient between the modeled and the observed O3-CO correlations for different regions of the globe. On a global scale, the G-PUCCINI model shows a good performance in the summer (C=0.71) and a satisfactory performance in the winter (C=0.52). It captures midlatitude features very well, especially in the summer, whereas the performance in regions like South America or Central Africa is weaker. The UKCA model (C=0.46/0.15 for July–August/December–January on a global scale) performs better in certain regions, such as the tropics in winter, and it captures some of the broad characteristics of summer extratropical correlations, but it systematically underestimates the O3-CO correlations over much of the globe. It is noteworthy that the correlations look very different in the two models, even though the ozone distributions are similar. This demonstrates that this technique provides a powerful global constraint for understanding modeled tropospheric chemical processes. We investigated the sources of the correlations by performing a series of sensitivity experiments. In these, the sign of the correlation is, in most cases, insensitive to removing different individual emissions, but its magnitude changes downwind of emission regions when applying such perturbations. Interestingly, we find that the O3-CO correlation does not solely reflect the strength of O3 photochemical production, as often assumed by earlier studies, but is more complicated and may reflect a mixture of different processes such as transport.

Description: Naturally produced very short-lived substances (VSLS) account for almost a quarter of the current stratospheric inorganic bromine, Bry. Following VSLS oxidation, bromine radicals (Br and BrO) can catalytically destroy ozone. The extent to which possible increases in surface emissions or transport of these VSLS bromocarbons to the stratosphere could counteract the effect of halogen reductions under the Montreal Protocol is an important policy question. Here, by using a chemistry–climate model, UM-UKCA, we investigate the impact of a hypothetical doubling (an increase of 5 ppt Bry) of VSLS bromocarbons on ozone and how the resulting ozone changes depend on the background concentrations of chlorine and bromine. Our model experiments indicate that for the 5 ppt increase in Bry from VSLS, the ozone decrease in the lowermost stratosphere of the Southern Hemisphere (SH) may reach up to 10% in the annual mean; the ozone decrease in the Northern Hemisphere (NH) is smaller (4–6%). The largest impact on the ozone column is found in the Antarctic spring. There is a significantly larger ozone decrease following the doubling of the VSLS burden under a high stratospheric chlorine background than under a low chlorine background, indicating the importance of the inter-halogen reactions. For example, the decline in the high-latitude, lower-stratospheric ozone concentration as a function of Bry is higher by about 30–40% when stratospheric Cly is ~ 3 ppb (present day), compared with Cly of ~ 0.8 ppb (a pre-industrial or projected future situation). Bromine will play an important role in the future ozone layer. However, even if bromine levels from natural VSLS were to increase significantly later this century, changes in the concentration of ozone will likely be dominated by the decrease in anthropogenic chlorine. Our calculation suggests that for a 5 ppt increase in Bry from VSLS, the Antarctic ozone hole recovery date could be delayed by approximately 6–8 years, depending on Cly levels.