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© 2017 The authors. Two independent chemistry-transport models with troposphere-stratosphere coupling are used to quantify the different components of the radiative forcing (RF) from aircraft emissions of NO x , i.e., the University of L'Aquila climate-chemistry model (ULAQ-CCM) and the University of Oslo chemistry-transport model (Oslo-CTM3). The tropospheric NO x enhancement due to aircraft emissions produces a short-term O 3 increase with a positive RF (+17.3mW/m 2 ) (as an average value of the two models). This is partly compensated by the CH 4 decrease due to the OH enhancement (-9.4mW/m 2 ). The latter is a long-term response calculated using a surface CH 4 flux boundary condition (FBC), with at least 50 years needed for the atmospheric CH 4 to reach steady state. The radiative balance is also affected by the decreasing amount of CO 2 produced at the end of the CH 4 oxidation chain: an average CO 2 accumulation change of -2.2 ppbv/yr is calculated on a 50 year time horizon (-1.6mW/m 2 ). The aviation perturbed amount of CH 4 induces a long-term response of tropospheric O 3 mostly due to less HO 2 and CH 3 O 2 being available for O 3 production, compared with the reference case where a constant CH 4 surface mixing ratio boundary condition is used (MBC) (-3.9mW/m 2 ). The CH 4 decrease induces a long-term response of stratospheric H2O (-1.4mW/m 2 ). The latter finally perturbs HO x and NO x in the stratosphere, with a more efficient NO x cycle for mid-stratospheric O 3 depletion and a decreased O 3 production from HO 2 +NO in the lower stratosphere. This produces a long-term stratospheric O 3 loss, with a negative RF (-1.2mW/m 2 ), compared with the CH 4 MBC case. Other contributions to the net NO x RF are those due to NO 2 absorption of UV-A and aerosol perturbations (the latter calculated only in the ULAQ-CCM). These comprise: increasing sulfate due to more efficient oxidation of SO 2 , increasing inorganic and organic nitrates and the net aerosols indirect effect on warm clouds. According to these model calculations, aviation NO x emissions for 2006 produced globally a net cooling effect of -5.7mW/m 2 (-6.2 and -5.1mW/m 2 , from ULAQ and Oslo models, respectively). When the effects of aviation sulfur emissions are taken into account in the atmospheric NO x balance (via heterogeneous chemistry), the model-average net cooling effects of aviation NO x increases to -6.2mW/m 2 . Our study applies to a sustained and constant aviation NO x emission and for the given background NOy conditions. The perturbation picture, however, may look different if an increasing trend in aviation NO x emissions would be allowed.

Air traffic alters the atmospheric composition and thereby contributes to climate change. Here we investigate the trans-Atlantic air traffic for one specific winter day and analyse, which routing changes were required to achieve a reduction in the air traffic's contribution to climate change. We have applied an atmosphere-chemistry model to calculate so-called five dimensional climate cost functions (CCF), which describe the climate effect of a locally confined emission. The five dimensions result from the emission location (3D), time (1D) and the type of emission (1D; carbon dioxide, water vapour, nitrogen oxides). In other words, carbon dioxide (CO2), water vapour (H2O) and nitrogen oxides (NOx) are emitted in amounts typical for aviation at many confined locations and times and their impacts on climate calculated with the atmosphere-chemistry model. The impact on climate results from direct effects, such as the changes in the concentration of the greenhouse gases CO2 and H2O and indirect effects such as contrail cirrus formation and chemical changes of ozone and methane by emissions of NOx. These climate cost functions are used by a flight planning tool to optimise flight routes with respect to their climate impact and economic costs of these routes. The results for this specific winter day show that large reductions in the air traffic’s contribution to climate warming (up to 60%) can be achieved for westbound flights and smaller reductions for eastbound flights (around 25%). Eastbound flights take advantage of the tail winds from the jet stream and hence routings with lower climate impacts have a large fuel penalty, whenever they leave the jet stream. Maximum reduction in climate impact increases the economic costs by 10–15%, due to higher fuel consumption, caused by a longer flight distance and lower flight levels. However, with only small changes to the air traffic routings and flight altitudes, climate reductions up to 25% can be achieved by only small changes in economic costs (less than 0.5%).

In addition to CO2, the climate impact of aviation is strongly influenced by non-CO2 emissions, such as nitrogen oxides, influencing ozone and methane, and water vapour, which can lead to the formation of persistent contrails in ice-supersaturated regions. Because these non-CO2 emission effects are characterised by a short lifetime, their climate impact largely depends on emission location and time; that is to say, emissions in certain locations (or times) can lead to a greater climate impact (even on the global average) than the same emission in other locations (or times). Avoiding these climate-sensitive regions might thus be beneficial to climate. Here, we describe a modelling chain for investigating this climate impact mitigation option. This modelling chain forms a multi-step modelling approach, starting with the simulation of the fate of emissions released at a certain location and time (time-region grid points). This is performed with the chemistry–climate model EMAC, extended via the two submodels AIRTRAC (V1.0) and CONTRAIL (V1.0), which describe the contribution of emissions to the composition of the atmosphere and to contrail formation, respectively. The impact of emissions from the large number of time-region grid points is efficiently calculated by applying a Lagrangian scheme. EMAC also includes the calculation of radiative impacts, which are, in a second step, the input to climate metric formulas describing the global climate impact of the emission at each time-region grid point. The result of the modelling chain comprises a four-dimensional data set in space and time, which we call climate cost functions and which describes the global climate impact of an emission at each grid point and each point in time. In a third step, these climate cost functions are used in an air traffic simulator (SAAM) coupled to an emission tool (AEM) to optimise aircraft trajectories for the North Atlantic region. Here, we describe the details of this new modelling approach and show some example results. A number of sensitivity analyses are performed to motivate the settings of individual parameters. A stepwise sanity check of the results of the modelling chain is undertaken to demonstrate the plausibility of the climate cost functions.

Significant reductions in stratospheric ozone occur inside the polar vortices each spring when chlorine radicals produced by heterogeneous reactions on cold particle surfaces in winter destroy ozone mainly in two catalytic cycles, the ClO dimer cycle and the ClO/BrO cycle. Chlorofluorocarbons (CFCs), which are responsible for most of the chlorine currently present in the stratosphere, have been banned by the Montreal Protocol and its amendments, and the ozone layer is predicted to recover to 1980 levels within the next few decades. During the same period, however, climate change is expected to alter the temperature, circulation patterns and chemical composition in the stratosphere, and possible geo-engineering ventures to mitigate climate change may lead to additional changes. To realistically predict the response of the ozone layer to such influences requires the correct representation of all relevant processes. The European project RECONCILE has comprehensively addressed remaining questions in the context of polar ozone depletion, with the objective to quantify the rates of some of the most relevant, yet still uncertain physical and chemical processes. To this end RECONCILE used a broad approach of laboratory experiments, two field missions in the Arctic winter 2009/10 employing the high altitude research aircraft M55-Geophysica and an extensive match ozone sonde campaign, as well as microphysical and chemical transport modelling and data assimilation. Some of the main outcomes of RECONCILE are as follows: (1) vortex meteorology: the 2009/10 Arctic winter was unusually cold at stratospheric levels during the six-week period from mid-December 2009 until the end of January 2010, with reduced transport and mixing across the polar vortex edge; polar vortex stability and how it is influenced by dynamic processes in the troposphere has led to unprecedented, synoptic-scale stratospheric regions with temperatures below the frost point; in these regions stratospheric ice clouds have been observed, extending over >106km2 during more than 3 weeks. (2) Particle microphysics: heterogeneous nucleation of nitric acid trihydrate (NAT) particles in the absence of ice has been unambiguously demonstrated; conversely, the synoptic scale ice clouds also appear to nucleate heterogeneously; a variety of possible heterogeneous nuclei has been characterised by chemical analysis of the non-volatile fraction of the background aerosol; substantial formation of solid particles and denitrification via their sedimentation has been observed and model parameterizations have been improved. (3) Chemistry: strong evidence has been found for significant chlorine activation not only on polar stratospheric clouds (PSCs) but also on cold binary aerosol; laboratory experiments and field data on the ClOOCl photolysis rate and other kinetic parameters have been shown to be consistent with an adequate degree of certainty; no evidence has been found that would support the existence of yet unknown chemical mechanisms making a significant contribution to polar ozone loss. (4) Global modelling: results from process studies have been implemented in a prognostic chemistry climate model (CCM); simulations with improved parameterisations of processes relevant for polar ozone depletion are evaluated against satellite data and other long term records using data assimilation and detrended fluctuation analysis. Finally, measurements and process studies within RECONCILE were also applied to the winter 2010/11, when special meteorological conditions led to the highest chemical ozone loss ever observed in the Arctic. In addition to quantifying the 2010/11 ozone loss and to understand its causes including possible connections to climate change, its impacts were addressed, such as changes in surface ultraviolet (UV) radiation in the densely populated northern mid-latitudes.

Recent laboratory measurements have shown the existence of a HNO3 forming branch of the HO2 + NO reaction. This reaction is the main source of tropospheric O3, through the subsequent photolysis of NO2, as well as being a major source of OH. The branching of the reaction to HNO3 reduces the formation of these species significantly, affecting O3 abundances, radiative forcing and the oxidation capacity of the troposphere. The Oslo CTM2, a three-dimensional chemistry transport model, is used to calculate atmospheric composition and trends with and without the new reaction branch. Results for the present day atmosphere, when both temperature and pressure effects on the branching ratio are accounted for, show an 11 % reduction in the calculated tropospheric burden of O3, with the main contribution from the tropics. An increase of the global, annual mean methane lifetime by 10.9 %, resulting from a 14.1 % reduction in the global, annual mean OH concentration is also found. Comparisons with measurements show that including the new branch improves the modelled O3 in the Oslo CTM2, but that it is not possible to conclude whether the NOy distribution improves. We model an approximately 11 % reduction in the tropical tropospheric O3 increase since pre-industrial times, and a 4 % reduction of the increase in total tropospheric burden. Also, an 8 % decrease in the trend of OH concentrations is calculated, when the new branch is accounted for. The radiative forcing due to changes in O3 over the industrial era was calculated as 0.33 W m−2, reducing to 0.26 W m−2 with the new reaction branch. These results are significant, and it is important that this reaction branching is confirmed by other laboratory groups.

The evolution of Arctic stratospheric O3 throughout the winter and spring of 2006/2007 is estimated by a state-of-the-art chemical transport model (CTM) and by a 3D-Var assimilation system using O3 data from the Earth Observing System (EOS) Microwave Limb Sounder (MLS) and Solar Backscatter Ultraviolet Radiometer (SBUV/2) satellites. Modelled and assimilated O3 compare well with MLS measurements. The aim of this article is to compare O3 loss estimates derived from the CTM and data-assimilation results, and as a result point to further developments in the method of inferring O3 loss using data assimilation. The methods for inferring O3 loss are discussed and compared with other published methods. The assimilation-system vertical transport is found to be too fast, in agreement with an earlier study, although this affects only the O3 reference field used for the loss estimation. Improving the O3 reference in the assimilation method used here provides a maximum vortex average O3 loss range of 0.8‐1.2 ppmv at 68hPa and 1.0‐1.5ppmv at 46hPa, peaking at the beginning of March. The corresponding CTM values are 1.4 and 1.6ppmv,respectively, withthe peak lagging the assimilation by a few days at 46hPa. We show that using a passive tracer as reference forO3 lossdoesnotprovidethebestestimateforpolarstratosphericcloud (PSC)-related loss for this winter; up to 40% of total O3 loss is shown not to be related to PSCs or heterogenous chemistry. Hence, the use of a passive O3 reference for estimating PSC-related O3 loss should be made with care. In addition to the vortex average losses, we estimate an innermost vortex O3 loss of 1.4ppmv due to PSCs only. Transport effects and differences between the CTM and the assimilation system are discussed, and possible improvements for both models are suggested. Copyright c � 2011 Royal Meteorological Society

Observations at surface sites show an increase in global mean surface methane (CH4) of about 180 parts per billion (ppb) (above 10 %) over the period 1984–2012. Over this period there are large fluctuations in the annual growth rate. In this work, we investigate the atmospheric CH4 evolution over the period 1970–2012 with the Oslo CTM3 global Chemical Transport Model (CTM) in a bottom-up approach. We thoroughly assess data from surface measurement sites in international networks and select a subset suited for comparisons with the output from the CTM. We compare model results and observations to understand causes both for long-term trends and short-term variations. Employing the Oslo CTM3 model we are able to reproduce the seasonal and year to year variations and shifts between years with consecutive growth and stagnation, both at global and regional scales. The overall CH4 trend over the period is reproduced, but for some periods the model fails to reproduce the strength of the growth. The observed growth after 2006 is overestimated by the model in all regions. This seems to be explained by a too strong increase in anthropogenic emissions in Asia, having global impact. Our findings confirm other studies questioning the timing or strength of the emission changes in Asia in the EDGAR v4.2 emission inventory over the last decades. The evolution of CH4 is not only controlled by changes in sources, but also by changes in the chemical loss in the atmosphere and soil uptake. We model a large growth in atmospheric oxidation capacity over the period 1970–2012. In our simulations, the CH4 lifetime decreases by more than 8 % from 1970 to 2012, a significant shortening of the residence time of this important greenhouse gas. This results in substantial growth in the chemical CH4 loss (relative to its burden) and dampens the CH4 growth. The change in atmospheric oxidation capacity is driven by complex interactions between a number of chemical components and meteorological factors. In our analysis, we are able to detach the key factors and provide simple prognostic equations for the relations between these and the atmospheric CH4 lifetime.

Three global chemistry-transport models (CTM) are used to quantify the radiative forcing (RF) from aviation NOx emissions, and the resultant reductions in RF from coupling NOx to aerosols via heterogeneous chemistry. One of the models calculates the changes due to aviation black carbon (BC) and sulphate aerosols and their direct RF, as well as the BC indirect effect on cirrus cloudiness. The surface area density of sulphate aerosols is then passed to the other models to compare the resulting photochemical perturbations on NOx through heterogeneous chemical reactions. The perturbation on O3 and CH4 (via OH) is finally evaluated, considering both short- and long-term O3 responses. Ozone RF is calculated using the monthly averaged output of the three CTMs in two independent radiative transfer codes. According to the models, column ozone and CH4 lifetime changes due to coupled NOx/aerosol emissions are, on average, +0.56 Dobson Units (DU) and −1.1 months, respectively, for atmospheric conditions and aviation emissions representative of the year 2006, with an RF of +16.4 and −10.2 mW/m2 for O3 and CH4, respectively. Sulphate aerosol induced changes on ozone column and CH4 lifetime account for −0.028 DU and +0.04 months, respectively, with corresponding RFs of −0.63 and +0.36 mW/m2. Soot-cirrus forcing is calculated to be 4.9 mW/m2.

The lifetime of nitrous oxide, the third-most-important human-emitted greenhouse gas, is based to date primarily on model studies or scaling to other gases. This work calculates a semiempirical lifetime based on Microwave Limb Sounder satellite measurements of stratospheric profiles of nitrous oxide, ozone, and temperature; laboratory cross-section data for ozone and molecular oxygen plus kinetics for O(1D); the observed solar spectrum; and a simple radiative transfer model. The result is 116 ± 9 years. The observed monthly-to-biennial variations in lifetime and tropical abundance are well matched by four independent chemistry-transport models driven by reanalysis meteorological fields for the period of observation (2005-2010), but all these models overestimate the lifetime due to lower abundances in the critical loss region near 32 km in the tropics. These models plus a chemistry-climate model agree on the nitrous oxide feedback factor on its own lifetime of 0.94 ± 0.01, giving N2O perturbations an effective residence time of 109 years. Combining this new empirical lifetime with model estimates of residence time and preindustrial lifetime (123 years) adjusts our best estimates of the human-natural balance of emissions today and improves the accuracy of projected nitrous oxide increases over this century. Key Points Nitrous oxide lifetime is computed empirically from MLS satellite data Empirical N2O lifetimes compared with models including interannual variability Results improve values for present anthropogenic and preindustrial emissions.© 2015. The Authors., Research at UCI was supported by NASA grants NNX09AJ47G and NNX13AL12G and DOE awards DE-SC0007021 and DE-SC0012536. N.M.D. was supported by UCI NSF REU 1005042. The GEOSCCM contribution was supported by the NASA MAP program. B.F. was supported by the Spanish MCINN under grant AYA2011-23552 and EC FEDER funds. Work at the Jet Propulsion Laboratory was performed under contract with NASA. The assistance of Ryan Fuller (at JPL) for the creation of MLS data sets used here is acknowledged. The GSFC 2-D model contribution was supported by the NASA Atmospheric Composition: Modeling and Analysis Program.

Within the EU-project TRADEOFF, the impact of NOx (=NO+NO2) emissions from subsonic aviation upon the chemical composition of the atmosphere has been calculated with focus on changes in reactive nitrogen and ozone. We apply a 3-D chemical transport model that includes comprehensive chemistry for both the troposphere and the stratosphere and uses various aircraft emission scenarios developed during TRADEOFF for the year 2000. The environmental effects of enhanced air traffic along polar routes and of possible changes in cruising altitude are investigated, taking into account effects of flight route changes on fuel consumption and emissions. In a reference case including both civil and military aircraft the model predicts aircraft-induced maximum increases of zonal-mean NOy (=total reactive nitrogen) between 156 pptv (August) and 322 pptv (May) in the tropopause region of the Northern Hemisphere. Resulting maximum increases in zonal-mean ozone vary between 3.1 ppbv in September and 7.7 ppbv in June. Enhanced use of polar routes implies substantially larger zonal-mean ozone increases in high Northern latitudes during summer, while the effect is negligible in winter. Lowering the flight altitude leads to smaller ozone increases in the lower stratosphere and upper troposphere, and to larger ozone increases at altitudes below. Regarding total ozone change, the degree of cancellation between these two effects depends on latitude and season, but annually and globally averaged the contribution from higher altitudes dominates, mainly due to washout of NOy in the troposphere, which weakens the tropospheric increase. Raising flight altitudes increases the ozone burden both in the troposphere and the lower stratosphere, primarily due to a more efficient accumulation of pollutants in the stratosphere.

The vapour phase reactions of 2-fluoroethanol, 2,2-difluoroethanol, and 2,2,2-trifluoroethanol with OH radicals and Cl atoms were studied at 298 K and 1013 mbar using long-path FTIR detection. The following reaction rate coefficients were determined by the relative rate method: k298(OH+CH2FCH2OH)=(1.42±0.11)×10−12, k298(OH+CHF2CH2OH)=(4.51±0.06)×10−13, k298(OH+CF3CH2OH)=(1.23±0.06)×10−13, k298(Cl+CH2FCH2OH)=(2.67±0.3)×10−11, k298(Cl+CHF2CH2OH)=(3.12±0.06)×10−12, and k298(Cl+CF3CH2OH)=(7.42±0.12)×10−13 cm3 molecule−1 s−1; the reported uncertainties represent 3 σ from the statistical analyses and do not include any systematic errors or uncertainties in the reference rate coefficients. Quantitative infrared cross-sections of the title compounds at 298 K are reported in the 4000–50 cm−1 region. A 3D chemistry transport model was applied to calculate the atmospheric distributions and lifetimes of the title compounds; the global and yearly averaged lifetimes were calculated as 20 days for CH2FCH2OH, 40 days for CHF2CH2OH, and 117 days for CF3CH2OH. Radiative forcing calculations were carried out assuming either constant vertical profiles or the distribution derived from the chemistry transport model. The Global Warming Potentials for the title compounds are insignificant compared to, e.g. CFC-11 (CCl3F).

Ozone and methane are chemically active climate-forcing agents affected by climate–chemistry interactions in the atmosphere. Key chemical reactions and processes affecting ozone and methane are presented. It is shown that climate-chemistry interactions have a significant impact on the two compounds. Ozone, which is a secondary compound in the atmosphere, produced and broken down mainly in the troposphere and stratosphre through chemical reactions involving atomic oxygen (O), NOx compounds (NO, NO2), CO, hydrogen radicals (OH, HO2), volatile organic compounds (VOC) and chlorine (Cl, ClO) and bromine (Br, BrO). Ozone is broken down through changes in the atmospheric distribution of the afore mentioned compounds. Methane is a primary compound emitted from different sources (wetlands, rice production, livestock, mining, oil and gas production and landfills).Methane is broken down by the hydroxyl radical (OH). OH is significantly affected by methane emissions, defined by the feedback factor, currently estimated to be in the range 1.3 to 1.5, and increasing with increasing methane emission. Ozone and methane changes are affected by NOx emissions. While ozone in general increase with increases in NOx emission, methane is reduced, due to increases in OH. Several processes where current and future changes have implications for climate-chemistry interactions are identified. It is also shown that climatic changes through dynamic processes could have significant impact on the atmospheric chemical distribution of ozone and methane, as we can see through the impact of Quasi Biennial Oscillation (QBO). Modeling studies indicate that increases in ozone could be more pronounced toward the end of this century. Thawing permafrost could lead to important positive feedbacks in the climate system. Large amounts of organic material are stored in the upper layers of the permafrost in the yedoma deposits in Siberia, where 2 to 5% of the deposits could be organic material. During thawing of permafrost, parts of the organic material that is deposited could be converted to methane. Furthermore, methane stored in deposits under shallow waters in the Arctic have the potential to be released in a future warmer climate with enhanced climate impact on methane, ozone and stratospheric water vapor. Studies performed by several groups show that the transport sectors have the potential for significant impacts on climate-chemistry interactions. There are large uncertainties connected to ozone and methane changes from the transport sector, and to methane release and climate impact during permafrost thawing.

The atmospheric impact of aircraft NOx emissions are studied using updated aircraft inventories for the year 2006, in order to estimate the photochemistry-related mitigation potential of shifting cruise altitudes higher or lower by 2000 ft. Applying three chemistry-transport models (CTM) and two climatechemistry models (CCM) in CTM mode, all including detailed tropospheric and stratospheric chemistry, we estimate the short-lived radiative forcing (RF) from O3 to range between 16.4 and 23.5 mW m 2, with a mean value of 19.5 mW m 2. Including the long-lived RF caused by changes in CH4, the total NOxrelated RF is estimated to about 5 mW m 2, ranging 1e8 mW m 2. Cruising at 2000 ft higher altitude increases the total RF due to aircraft NOx emissions by 2 ± 1 mW m 2, while cruising at 2000 ft lower altitude reduces RF by 2 ± 1 mWm 2. This change is mainly controlled by short-lived O3 and show that chemical NOx impact of contrail avoiding measures is likely small.

Accurate prediction of future methane abundances following a climate scenario requires understanding the lifetime changes driven by anthropogenic emissions, meteorological factors, and chemistry-climate feedbacks. Uncertainty in any of these influences or the underlying processes implies uncertainty in future abundance and radiative forcing. We simulate methane lifetime in three chemical transport models (CTMs) – UCI CTM, GEOS-Chem, and Oslo CTM3 – over the period 1997–2009 and compare the models' year-to-year variability against constraints from global methyl chloroform observations. Using sensitivity tests, we find that temperature, water vapor, stratospheric ozone column, biomass burning and lightning NOx are the dominant sources of interannual changes in methane lifetime in all three models. We also evaluate each model's response to forcings that have impacts on decadal time scales, such as methane feedback, and anthropogenic emissions. In general, these different CTMs show similar sensitivities to the driving variables. We construct a parametric model that reproduces most of the interannual variability of each CTM and use it to predict methane lifetime from 1980 through 2100 following a specified emissions and climate scenario (RCP 8.5). The parametric model propagates uncertainties through all steps and provides a foundation for predicting methane abundances in any climate scenario. Our sensitivity tests also enable a new estimate of the methane global warming potential (GWP), accounting for stratospheric ozone effects, including those mediated by water vapor. We estimate the 100-yr GWP to be 32, which is 25% larger than past assessments.

In addition to CO2, the climate impact of aviation is strongly influenced by non-CO2 emissions, such as nitrogen oxides, influencing ozone and methane, and water vapour, forming contrails. Because these non-CO2 emission effects are characterised by a short lifetime, their climate impact largely depends on emission location and time, i.e. emissions in certain locations (or times) can lead to a greater climate impact (even on the global average) than the same emission in other locations (or times). Avoiding these climate sensitive regions might thus be beneficial to climate. Here, we describe a modelling chain for investigating this climate impact mitigation option. It forms a multi-step modelling approach, starting with the simulation of the fate of emissions released at a certain location and time (time-region). This is performed with the chemistry–climate model EMAC, extended by the two submodels AIRTRAC 1.0 and CONTRAIL 1.0, which describe the contribution of emissions to the composition of the atmosphere and the contrail formation. Numerous time-regions are efficiently calculated by applying a Lagrangian scheme. EMAC also includes the calculation of radiative impacts, which are, in a second step, the input to climate metric formulas describing the climate impact of the time-region emission. The result of the modelling chain comprises a four dimensional dataset in space and time, which we call climate cost functions, and which describe at each grid point and each point in time, the climate impact of an emission. In a third step, these climate cost functions are used in a traffic simulator (SAAM), coupled to an emission tool (AEM) to optimise aircraft trajectories for the North Atlantic region. Here, we describe the details of this new modelling approach and show some example results. A number of sensitivity analyses are performed to motivate the settings of individual parameters. A stepwise sanity check of the results of the modelling chain is undertaken to demonstrate the plausibility of the climate cost functions.

Arctic column ozone reached record low values (∼310 DU) during March of 2011, exposing Arctic ecosystems to enhanced UV-B. We identify the cause of this anomaly using the Oslo CTM2 atmospheric chemistry model driven by ECMWF meteorology to simulate Arctic ozone from 1998 through 2011. CTM2 successfully reproduces the variability in column ozone, from week to week, and from year to year, correctly identifying 2011 as an extreme anomaly over the period. By comparing parallel model simulations, one with all Arctic ozone chemistry turned off on January 1, we find that chemical ozone loss in 2011 is enhanced relative to previous years, but it accounted for only 23% of the anomaly. Weakened transport of ozone from middle latitudes, concurrent with an anomalously strong polar vortex, was the primary cause of the low ozone When the zonal winds relaxed in mid-March 2011, Arctic column ozone quickly recovered.

We present here the global chemical transport model Oslo CTM3, an update of the Oslo CTM2. The update comprises a faster transport scheme, an improved wet scavenging scheme for large scale rain, updated photolysis rates and a new lightning parameterization. Oslo CTM3 is better parallelized and allows for stable, large time steps for advection, enabling more complex or high spatial resolution simulations. A new treatment of the horizontal distribution of lightning is presented and found to compare well with measurements. The vertical distribution of lightning is updated and found to be a large contributor to CTM2–CTM3 differences, producing more NOx in the tropical middle troposphere, and less at the surface and at high altitudes. Compared with Oslo CTM2, Oslo CTM3 is faster, more capable and has better conceptual models for scavenging, vertical transport and fractional cloud cover. CTM3 captures stratospheric O3 better than CTM2, but shows minor improvements in terms of matching atmospheric observations in the troposphere. Use of the same meteorology to drive the two models shows that some features related to transport are better resolved by the CTM3, such as polar cap transport, while features like transport close to the vortex edge are resolved better in the Oslo CTM2 due to its required shorter transport time step. The longer transport time steps in CTM3 result in larger errors, e.g., near the jets, and when necessary the errors can be reduced by using a shorter time step. Using a time step of 30 min, the new transport scheme captures both large-scale and small-scale variability in atmospheric circulation and transport, with no loss of computational efficiency. We present a version of the new transport scheme which has been specifically tailored for polar studies, resulting in more accurate polar cap transport than the standard CTM3 transport, confirmed by comparison to satellite observations. Inclusion of tropospheric sulfur chemistry and nitrate aerosols in CTM3 is shown to be important to reproduce tropospheric O3, OH and the CH4 lifetime well.

Recent laboratory measurements have shown the existence of a HNO3 forming branch of the HO2 + NO reaction. This reaction is the main source of atmospheric O3, through the subsequent photolysis of NO2, as well as being a major source of OH. The branching of the reaction to HNO3 reduces the formation of these species significantly, affecting O3 abundances, climate and the oxidation capacity of the troposphere. The Oslo CTM2, a three-dimensional chemistry transport model, is used to calculate atmospheric composition and trends with and without the new reaction branch. Results for the present day atmosphere, when both temperature and pressure effects on the branching ratio are accounted for, show an increase of the global, annual mean methane lifetime by 10.9 %, resulting from a 14.1 % reduction in the global, annual mean OH concentration. Comparisons with measurements show that including the new branch improves the modelled O3, but that it is not possible to conclude whether the NOy distribution improves. We model an approximately 11 % reduction in the tropical tropospheric O3 increase since pre-industrial times, as well as an 8 % decrease in the trend of OH concentration, when the new branch is accounted for. The radiative forcing due to changes in O3 over the industrial era was calculated as 0.33 W m−2, reducing to 0.26 W m−2 with the new reaction branch. These results are significant, and it is important that this reaction branching is confirmed by other laboratory groups.

This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and European surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, then deposition velocity and surface emissions and finally, deposition velocity, biomass burning, anthropogenic and N2 fixation-related emissions were simultaneously inverted in several scenarios. These scenarios have focused on the sensibility of the soil uptake value to different spatio-temporal distributions. The range of variations of these diverse inversion sets generate an estimate of the uncertainty for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between −8 and +8 Tg yr−1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on bottom-up and top-down estimations. Our estimate of global H2 soil uptake is −59±9 Tg yr−1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions within the range of their respective uncertainties. Additional constraints, such as isotopic measurements would be needed to infer a more robust partition of H2 sources and sinks.

[1] The global chemical transport model Oslo CTM2, driven by European Centre for Medium-Range Weather Forecasts international Integrated Forecast System meteorology and including tropospheric and stratospheric chemistry, is described and evaluated against measurements by satellite-based instruments, ozone sondes, and aircraft. A new heterogeneous chemistry and microphysics scheme capable of reproducing severe ozone depletion events is described. The Oslo CTM2 simulates ozone measurements well, overestimating by less than 20% in the lowermost stratosphere, while underestimating slightly at higher altitudes. In the upper troposphere, the spatial and temporal variation is well simulated, although a 30–50% overestimation is seen. In order to demonstrate ozone depletion in the Arctic by heterogeneous processes, the ozone loss during the cold 2004/2005 Arctic winter stratosphere is compared to the warm 2000/2001 Arctic winter. Enhanced ozone loss is shown to have occurred at eight Arctic stations. From January to March the accumulated ozone loss amounts to up to 1 ppmv, with a maximum ozone loss rate of 32 ppb/d. Ozone sonde measurements are well reproduced for both years.

The demand for intercontinental transportation is increasing and people are requesting short travel times, which supersonic air transportation would enable. However, besides noise and sonic boom issues, which we are not referring to in this investigation, emissions from supersonic aircraft are known to alter the atmospheric composition, in particular the ozone layer, and hence affect climate significantly more than subsonic aircraft. Here, we suggest a metric to quantitatively assess different options for supersonic transport with regard to the potential destruction of the ozone layer and climate impacts. Options for fleet size, engine technology (nitrogen oxide emission level), cruising speed, range, and cruising altitude, are analyzed, based on SCENIC emission scenarios for 2050, which underlay the requirements to be as realistic as possible in terms of e.g., economic markets and profitable market penetration. This methodology is based on a number of atmosphere-chemistry and climate models to reduce model dependencies. The model results differ significantly in terms of the response to a replacement of subsonic aircraft by supersonic aircraft, e.g., concerning the ozone impact. However, model differences are smaller when comparing the different options for a supersonic fleet. Those uncertainties were taken into account to make sure that our findings are robust. The base case scenario, where supersonic aircraft get in service in 2015, a first fleet fully operational in 2025 and a second in 2050, leads in our simulations to a near surface temperature increase in 2050 of around 7 mK and with constant emissions afterwards to around 21 mK in 2100. The related total radiative forcing amounts to 22 mWm2 in 2050, with an uncertainty between 9 and 29 mWm2. A reduced supersonic cruise altitude or speed (from Mach 2 to Mach 1.6) reduces both, climate impact and ozone destruction, by around 40%. An increase in the range of the supersonic aircraft leads to more emissions at lower latitudes since more routes to SE Asia are taken into account, which increases ozone depletion, but reduces climate impact compared to the base case.

International audience; Impacts of NOx, H2O and aerosol emissions from a projected 2050 aircraft fleet, provided in the EU project SCENIC, are investigated using the Oslo CTM2, a 3-D chemical transport model including comprehensive chemistry for the stratosphere and the troposphere. The aircraft emission scenarios comprise emissions from subsonic and supersonic aircraft. The increases in NOy due to emissions from the mixed fleet are comparable for subsonic (at 11–12 km) and supersonic (at 18–20 km) aircraft, with annual zonal means of 1.35 ppbv and 0.83 ppbv, respectively. H2O increases are also comparable at these altitudes: 630 and 599 ppbv, respectively. The aircraft emissions increase tropospheric ozone by about 10 ppbv in the Northern Hemisphere due to increased ozone production, mainly because of subsonic aircraft. Supersonic aircraft contribute to a reduction of stratospheric ozone due to increased ozone loss at higher altitudes. In the Northern Hemisphere the reduction is about 39 ppbv, but also in the Southern Hemisphere a 22 ppbv stratospheric decrease is modeled due to transport of supersonic aircraft emissions and ozone depleted air. The total ozone column is increased in lower and Northern mid-latitudes, otherwise the increase of ozone loss contributes to a decrease of the total ozone column. Two exceptions are the Northern Hemispheric spring, where the ozone loss increase is small due to transport processes, and tropical latitudes during summer where the effect of subsonic aircraft is low due to a high tropopause. Aerosol particles emitted by aircraft reduce both aircraft and background NOx, more than counterweighting the effect of NOx and H2O aircraft emissions in the stratosphere. Above about 20 km altitude, the NOx (and thus ozone loss) reduction is large enough to give an increase in ozone due to aircraft emissions. This effect is comparable in the Northern and Southern Hemisphere. At 11–20 km altitude, however, ozone production is reduced due to less NOx. Also ClONO2 is increased at this altitude due to enhanced heterogeneous reactions (lowered HCl), and ClO is increased due to less NOx, further enhancing ozone loss in this region. This results in a 14 ppbv further reduction of ozone. Mainly, this results in an increase of the total ozone column due to a decrease in ozone loss caused by the NOx cycle (at the highest altitudes). At the lowermost latitudes, the reduced loss due to the NOx cycle is small. However, ozone production at lower altitudes is reduced and the loss due to ClO is increased, giving a decrease in the total ozone column. Also, at high latitudes during spring the heterogeneous chemistry is more efficient on PSCs, increasing the ozone loss.

In this work we focus on the direct radiative forcing (RF) of black carbon (BC) and sulphuric acid particles emitted by future supersonic aircraft, as well as on the ozone RF due to changes produced by emissions of both gas species (NOx, H2O) and aerosol particles capable of affecting stratospheric ozone chemistry. Heterogeneous chemical reactions on the surface of sulphuric acid stratospheric particles (SSA-SAD) are the main link between ozone chemistry and supersonic aircraft emissions of sulphur precursors (SO2) and particles (H2O–H2SO4). Photochemical O3 changes are compared from four independent 3-D atmosphere-chemistry models (ACMs), using as input the perturbation of SSA-SAD calculated in the University of L'Aquila model, which includes on-line a microphysics code for aerosol formation and growth. The ACMs in this study use aircraft emission scenarios for the year 2050 developed by AIRBUS as a part of the EU project SCENIC, assessing options for fleet size, engine technology (NOx emission index), Mach number, range and cruising altitude. From our baseline modeling simulation, the impact of supersonic aircraft on sulphuric acid aerosol and BC mass burdens is 53 and 1.5 μg/m2, respectively, with a direct RF of −11.4 and 4.6 mW/m2 (net RF=−6.8 mW/m2). This paper discusses the similarities and differences amongst the participating models in terms of changes to O3 precursors due to aircraft emissions (NOx, HOx,Clx,Brx) and the stratospheric ozone sensitivity to them. In the baseline case, the calculated global ozone change is −0.4 ±0.3 DU, with a net radiative forcing (IR+UV) of −2.5± 2 mW/m2. The fraction of this O3-RF attributable to SSA-SAD changes is, however, highly variable among the models, depending on the NOx removal efficiency from the aircraft emission regions by large scale transport.