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Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337 ± 23 Tg, the ensemble mean burden for 1850 time slice is ~30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: -4% (-16 %) for RCP2.6, 2% (-7 %) for RCP4.5, 1% (-9 %) for RCP6.0, and 7% (18 %) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40-150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly. [ABSTRACT FROM AUTHOR]

The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The modelto- model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry. [ABSTRACT FROM AUTHOR]

An ozone climatology based on ozonesonde measurements taken over the last 17 yr has been constructed for model evaluation and comparisons to other observations. Vertical ozone profiles for 42 stations around the globe have been compiled for the period 1995-20, in pressure and tropopause-referenced altitudes. For each profile, the mean, standard deviation, median, the half-width are provided, as well as information about interannual variability. Regional aggregates are formed in combining stations with similar ozone characteristics. The Hellinger distance is introduced as a new diagnostic to identify stations that describe similar shapes of ozone probability distribution functions (PDFs). In this way, 12 regions were selected covering at least 2 stations and the variability among those stations is discussed. Significant variability with longitude of ozone distributions in the troposphere and lower stratosphere in the northern mid- and high latitudes is found. The representativeness of regional aggregates is discussed for high northern latitudes, Western Europe, Eastern US, Japan, using independent observations from surface stations and MOZAIC aircraft data. Good agreement exists between ozonesondes and aircraft observations in the mid-troposphere and between ozonesondes and surface observations for Western Europe. For Eastern US and high northern latitudes, surface ozone values from ozonesondes are biased 10ppb high compared to independent measurements. An application of the climatology is presented using the NCAR CAM-Chem model. The climatology allows evaluation of the model performance regarding ozone averages, seasonality, interannual variability, the shape of ozone distributions. The new assessment of the key features of ozone distributions gives deeper insights into the performance of models. [ABSTRACT FROM AUTHOR]

The article focuses on the different simulation methods used in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The study introduces several simulation approaches to determine the long-term changes in the atmospheric composition between 1850 and 2100 though the ACCMIP project. It outlines the result of the study, which indicates that the present-day climate diagnostics are consistent with the state-of-the-art climate models.

We have integrated observations of tropospheric ozone, very short-lived (VSL) halocarbons and reactive iodine and bromine species from a wide variety of tropical data sources with the global CAM-Chem chemistry-climate model and offline radiative transfer calculations to compute the contribution of halogen chemistry to ozone loss and associated radiative impact in the tropical marine troposphere. The inclusion of tropospheric halogen chemistry in CAM-Chem leads to an annually averaged depletion of around 10% (∼2.5 Dobson units) of the tropical tropospheric ozone column, with largest effects in the middle to upper troposphere. This depletion contributes approximately -0.10Wm-2 to the radiative flux at the tropical tropopause. This negative flux is of similar magnitude to the ∼0.33Wm-2 contribution of tropospheric ozone to presentday radiative balance as recently estimated from satellite observations. We find that the implementation of oceanic halogen sources and chemistry in climate models is an important component of the natural background ozone budget and we suggest that it needs to be considered when estimating both preindustrial ozone baseline levels and long term changes in tropospheric ozone. [ABSTRACT FROM AUTHOR]

The global chemistry-climate model CAMChem has been extended to incorporate an expanded bromine and iodine chemistry scheme that includes natural oceanic sources of very short-lived (VSL) halocarbons, gas-phase photochemistry and heterogeneous reactions on aerosols. Ocean emissions of five VSL bromocarbons (CHBr3, CH2Br2, CH2BrCl, CHBrCl2, CHBr2Cl) and three VSL iodocarbons (CH2ICl, CH2IBr, CH2I2) have been parameterised by a biogenic chlorophyll-a (chl-a) dependent source in the tropical oceans (20° N-20° S). Constant oceanic fluxes with 2.5 coast-to-ocean emission ratios are separately imposed on four different latitudinal bands in the extratropics (20°-50° and above 50° in both hemispheres). Top-down emission estimates of bromocarbons have been derived using available measurements in the troposphere and lower stratosphere, while iodocarbons have been constrained with observations in the marine boundary layer (MBL). Emissions of CH3I are based on a previous inventory and the longer lived CH3Br is set to a surface mixing ratio boundary condition. The global oceanic emissions estimated for the most abundant VSL bromocarbons - 533 Gg yr-1 for CHBr3 and 67.3 Gg yr-1 for CH2Br2 - are within the range of previous estimates. Overall the latitudinal and vertical distributions of modelled bromocarbons are in good agreement with observations. Nevertheless, we identify some issues such as the reduced number of aircraft observations to validate models in the Southern Hemisphere, the overestimation of CH2Br2 in the upper troposphere - lower stratosphere and the underestimation of CH3I in the same region. Despite the difficulties involved in the global modelling of the shortest lived iodocarbons (CH2ICl, CH2IBr, CH2I2), modelled results are in good agreement with published observations in the MBL. Finally, sensitivity simulations show that knowledge of the diurnal emission cycle for these species, in particular for CH2I2, is key to assess their global source strength. [ABSTRACT FROM AUTHOR]

A continuous tropospheric and stratospheric vertically resolved ozone time series, from 1850 to 2099, has been generated to be used as forcing in global climate models that do not include interactive chemistry. A multiple linear regression analysis of SAGE I+II satellite observations and polar ozonesonde measurements is used for the stratospheric zonal mean dataset during the well-observed period from 1979 to 2009. In addition to terms describing the mean annual cycle, the regression includes terms representing equivalent effective stratospheric chlorine (EESC) and the 11-yr solar cycle variability. The EESC regression fit coefficients, together with pre-1979 EESC values, are used to extrapolate the stratospheric ozone time series backward to 1850. While a similar procedure could be used to extrapolate into the future, coupled chemistry climate model (CCM) simulations indicate that future stratospheric ozone abundances are likely to be significantly affected by climate change, and capturing such effects through a regression model approach is not feasible. Therefore, the stratospheric ozone dataset is extended into the future (merged in 2009) with multimodel mean projections from 13 CCMs that performed a simulation until 2099 under the SRES (Special Report on Emission Scenarios) A1B greenhouse gas scenario and the A1 adjusted halogen scenario in the second round of the Chemistry-Climate Model Validation (CCMVal-2) Activity. The stratospheric zonal mean ozone time series is merged with a three-dimensional tropospheric data set extracted from simulations of the past by two CCMs (CAM3.5 and GISSPUCCINI) and of the future by one CCM (CAM3.5). The future tropospheric ozone time series continues the historical CAM3.5 simulation until 2099 following the four different Representative Concentration Pathways (RCPs). Generally good agreement is found between the historical segment of the ozone database and satellite observations, although it should be noted that total column ozone is overestimated in the southern polar latitudes during spring and tropospheric column ozone is slightly underestimated. Vertical profiles of tropospheric ozone are broadly consistent with ozonesondes and in-situ measurements, with some deviations in regions of biomass burning. The tropospheric ozone radiative forcing (RF) from the 1850s to the 2000s is 0.23Wm-2, lower than previous results. The lower value is mainly due to (i) a smaller increase in biomass burning emissions; (ii) a larger influence of stratospheric ozone depletion on upper tropospheric ozone at high southern latitudes; and possibly (iii) a larger influence of clouds (which act to reduce the net forcing) compared to previous radiative forcing calculations. Over the same period, decreases in stratospheric ozone, mainly at high latitudes, produce a RF of -0.08Wm-2, which is more negative than the central Intergovernmental Panel on Climate Change (IPCC) Fourth Assessment Report (AR4) value of -0.05Wm-2, but which is within the stated range of -0.15 to +0.05Wm-2. The more negative value is explained by the fact that the regression model simulates significant ozone depletion prior to 1979, in line with the increase in EESC and as confirmed by CCMs, while the AR4 assumed no change in stratospheric RF prior to 1979. A negative RF of similar magnitude persists into the future, although its location shifts from high latitudes to the tropics. This shift is due to increases in polar stratospheric ozone, but decreases in tropical lower stratospheric ozone, related to a strengthening of the Brewer-Dobson circulation, particularly through the latter half of the 21st century. Differences in trends in tropospheric ozone among the four RCPs are mainly driven by different methane concentrations, resulting in a range of tropospheric ozone RFs between 0.4 and 0.1Wm-2 by 2100. The ozone dataset described here has been released for the Coupled Model Intercomparison Project (CMIP5) model simulations in netCDF Climate and Forecast (CF) Metadata Convention at the PCMDI website (http://cmip-pcmdi.llnl.gov/). [ABSTRACT FROM AUTHOR]

The article explores the evaluation and description of the global Community Atmosphere Model (CAM) version 4 for atmospheric chemistry in Community Earth System Model (CESM). It reports that the atmospheric chemistry is responsible for the distribution of non-carbon dioxide gases and aerosols which influence the climate and air quality. Details on topics including the offline meteorology, chemical mechanisms, and emissions are discussed.

A comprehensive numerical modeling framework was developed to estimate the effects of collective global changes upon ozone pollution in the US in 2050. The framework consists of the global climate and chemistry models, PCM (Parallel Climate Model) and MOZART-2 (Model for Ozone and Related Chemical Tracers v.2), coupled with regional meteorology and chemistry models, MM5 (Mesoscale Meteorological model) and CMAQ (Community Multi-scale Air Quality model). The modeling system was applied for two 10-year simulations: 1990-1999 as a present-day base case and 2045-2054 as a future case. For the current decade, the daily maximum 8-h moving average (DM8H) ozone mixing ratio distributions for spring, summer and fall showed good agreement with observations. The future case simulation followed the Intergovernmental Panel on Climate Change (IPCC) A2 scenario together with business-as-usual US emission projections and projected alterations in land use, land cover (LULC) due to urban expansion and changes in vegetation. For these projections, US anthropogenic NOx (NO+NO2) and VOC (volatile organic carbon) emissions increased by approximately 6% and 50%, respectively, while biogenic VOC emissions decreased, in spite of warmer temperatures, due to decreases in forested lands and expansion of croplands, grasslands and urban areas. A stochastic model for wildfire emissions was applied that projected 25% higher VOC emissions in the future. For the global and US emission projection used here, regional ozone pollution becomes worse in the 2045-2054 period for all months. Annually, the mean DM8H ozone was projected to increase by 9.6 ppbv (22%). The changes were higher in the spring and winter (25%) and smaller in the summer (17%). The area affected by elevated ozone within the US continent was projected to increase; areas with levels exceeding the 75 ppbv ozone standard at least once a year increased by 38%. In addition, the length of the ozone season was projected to increase with more pollution episodes in the spring and fall. For selected urban areas, the system projected a higher number of pollution events per year and these events had more consecutive days when DM8H ozone exceed 75 ppbv. [ABSTRACT FROM AUTHOR]

Changes in atmospheric ozone have occurred since the preindustrial era as a result of increasing anthropogenic emissions. Within ACCENT, a European Network of Excellence, ozone changes between 1850 and 2000 are assessed for the troposphere and the lower stratosphere (up to 30 km) by a variety of seven chemistry-climate models and three chemical transport models. The modeled ozone changes are taken as input for detailed calculations of radiative forcing. When only changes in chemistry are considered (constant climate) the modeled global-mean tropospheric ozone column increase since preindustrial times ranges from 7.9DU to 13.8DU among the ten participating models, while the stratospheric column reduction lies between 14.1DU and 28.6DU in the models considering stratospheric chemistry. The resulting radiative forcing is strongly dependent on the location and altitude of the modeled ozone change and varies between 0.25Wm-2 and 0.45Wm-2 due to ozone change in the troposphere and -0.123Wm-2 and +0.066Wm-2 due to the stratospheric ozone change. Changes in ozone and other greenhouse gases since preindustrial times have altered climate. Six out of the ten participating models have performed an additional calculation taking into account both chemical and climate change. In most models the isolated effect of climate change is an enhancement of the tropospheric ozone column increase, while the stratospheric reduction becomes slightly less severe. In the three climate-chemistry models with detailed tropospheric and stratospheric chemistry the inclusion of climate change increases the resulting radiative forcing due to tropospheric ozone change by up to 0.10Wm-2, while the radiative forcing due to stratospheric ozone change is reduced by up to 0.034Wm-2. Considering tropospheric and stratospheric change combined, the total ozone column change is negative while the resulting net radiative forcing is positive. [ABSTRACT FROM AUTHOR]