Aircraft pollution: a futuristic view

International audienceImpacts 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

Sulfate geoengineering impact on methane transport and lifetime: results from the Geoengineering Model Intercomparison Project (GeoMIP)

Abstract. Sulfate geoengineering (SG), made by sustained injection of SO2 in the tropical lower stratosphere, may impact the CH4 abundance through several photochemical mechanisms affecting tropospheric OH and hence the methane lifetime. (a) The reflection of incoming solar radiation increases the planetary albedo and cools the surface, with a tropospheric H2O decrease. (b) The tropospheric UV budget is upset by the additional aerosol scattering and stratospheric ozone changes: the net effect is meridionally not uniform, with a net decrease in the tropics, thus producing less tropospheric O(1D). (c) The extratropical downwelling motion from the lower stratosphere tends to increase the sulfate aerosol surface area density available for heterogeneous chemical reactions in the mid-to-upper troposphere, thus reducing the amount of NOx and O3 production. (d) The tropical lower stratosphere is warmed by solar and planetary radiation absorption by the aerosols. The heating rate perturbation is highly latitude dependent, producing a stronger meridional component of the Brewer–Dobson circulation. The net effect on tropospheric OH due to the enhanced stratosphere–troposphere exchange may be positive or negative depending on the net result of different superimposed species perturbations (CH4, NOy, O3, SO4) in the extratropical upper troposphere and lower stratosphere (UTLS). In addition, the atmospheric stabilization resulting from the tropospheric cooling and lower stratospheric warming favors an additional decrease of the UTLS extratropical CH4 by lowering the horizontal eddy mixing. Two climate–chemistry coupled models are used to explore the above radiative, chemical and dynamical mechanisms affecting CH4 transport and lifetime (ULAQ-CCM and GEOSCCM). The CH4 lifetime may become significantly longer (by approximately 16 %) with a sustained injection of 8 Tg-SO2 yr−1 starting in the year 2020, which implies an increase of tropospheric CH4 (200 ppbv) and a positive indirect radiative forcing of sulfate geoengineering due to CH4 changes (+0.10 W m−2 in the 2040–2049 decade and +0.15 W m−2 in the 2060–2069 decade)

A new Geoengineering Model Intercomparison Project (GeoMIP) experiment designed for climate and chemistry models

A new Geoengineering Model Intercomparison Project (GeoMIP) experiment "G4 specified stratospheric aerosols" (short name: G4SSA) is proposed to investigate the impact of stratospheric aerosol geoengineering on atmosphere, chemistry, dynamics, climate, and the environment. In contrast to the earlier G4 GeoMIP experiment, which requires an emission of sulfur dioxide (SO2) into the model, a prescribed aerosol forcing file is provided to the community, to be consistently applied to future model experiments between 2020 and 2100. This stratospheric aerosol distribution, with a total burden of about 2 Tg S has been derived using the ECHAM5-HAM microphysical model, based on a continuous annual tropical emission of 8 Tg SO2 yr−1. A ramp-up of geoengineering in 2020 and a ramp-down in 2070 over a period of 2 years are included in the distribution, while a background aerosol burden should be used for the last 3 decades of the experiment. The performance of this experiment using climate and chemistry models in a multi-model comparison framework will allow us to better understand the impact of geoengineering and its abrupt termination after 50 years in a changing environment. The zonal and monthly mean stratospheric aerosol input data set is available at https://www2.acd.ucar.edu/gcm/geomip-g4-specified-stratospheric-aerosol-data-set

Radiative forcing from aircraft emissions of NOx: model calculations with CH4 surface flux boundary condition

© 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

TRADEOFFs in climate effects through aircraft routing: forcing due to radiatively active gases

We have estimated impacts of alternative aviation routings on the radiative forcing. Changes in ozone and OH have been estimated in four Chemistry Transport Models (CTMs) participating in the TRADEOFF project. Radiative forcings due to ozone and methane have been calculated accordingly. In addition radiative forcing due to CO2 is estimated based on fuel consumption. Three alternative routing cases are investigated; one scenario assuming additional polar routes and two scenarios assuming aircraft cruising at higher (+2000 ft) and lower (−6000 ft) altitudes. Results from the base case in year 2000 are included as a reference. Taking first a steady state backward looking approach, adding the changes in the forcing from ozone, CO2 and CH4, the ranges of the models used in this work are −0.8 to −1.8 and 0.3 to 0.6 m Wm−2 in the lower (−6000 ft) and higher (+2000 ft) cruise levels, respectively. In relative terms, flying 6000ft lower reduces the forcing by 5–10% compared to the current flight pattern, whereas flying higher, while saving fuel and presumably flying time, increases the forcing by about 2–3%. Taking next a forward looking approach we have estimated the integrated forcing (m Wm−2 yr) over 20 and 100 years time horizons. The relative contributions from each of the three climate gases are somewhat different from the backward looking approach. The differences are moderate adopting 100 year time horizon, whereas under the 20 year horizon CO2 naturally becomes less important relatively. Thus the forcing agents impact climate differently on various time scales. Also, we have found significant differences between the models for ozone and methane. We conclude that we are not yet at a point where we can include non-CO2 effects of aviation in emission trading schemes. Nevertheless, the rerouting cases that have been studied here yield relatively small changes in the radiative forcing due to the radiatively active gases

Radiative forcing in the 21st century due to ozone changes in the troposphere and the lower stratosphere

Radiative forcing due to changes in ozone is expected for the 21st century. An assessment on changes in the tropospheric oxidative state through a model intercomparison ("OxComp'') was conducted for the IPCC Third Assessment Report (IPCC-TAR). OxComp estimated tropospheric changes in ozone and other oxidants during the 21st century based on the "SRES'' A2p emission scenario. In this study we analyze the results of 11 chemical transport models (CTMs) that participated in OxComp and use them as input for detailed radiative forcing calculations. We also address future ozone recovery in the lower stratosphere and its impact on radiative forcing by applying two models that calculate both tropospheric and stratospheric changes. The results of OxComp suggest an increase in global-mean tropospheric ozone between 11.4 and 20.5 DU for the 21st century, representing the model uncertainty range for the A2p scenario. As the A2p scenario constitutes the worst case proposed in IPCC-TAR we consider these results as an upper estimate. The radiative transfer model yields a positive radiative forcing ranging from 0.40 to 0.78 W m(-2) on a global and annual average. The lower stratosphere contributes an additional 7.5-9.3 DU to the calculated increase in the ozone column, increasing radiative forcing by 0.15-0.17 W m(-2). The modeled radiative forcing depends on the height distribution and geographical pattern of predicted ozone changes and shows a distinct seasonal variation. Despite the large variations between the 11 participating models, the calculated range for normalized radiative forcing is within 25%, indicating the ability to scale radiative forcing to global-mean ozone column change

Upper tropospheric ice sensitivity to sulfate geoengineering

Aside from the direct surface cooling that sulfate geoengineering (SG) would produce, investigations of the possible side effects of this method are still ongoing, such as the exploration of the effect that SG may have on upper tropospheric cirrus cloudiness. The goal of the present study is to better understand the SG thermodynamical effects on the freezing mechanisms leading to ice particle formation. This is undertaken by comparing SG model simulations against a Representative Concentration Pathway 4.5 (RCP4.5) reference case. In the first case, the aerosol-driven surface cooling is included and coupled to the stratospheric warming resulting from the aerosol absorption of terrestrial and solar near-infrared radiation. In a second SG perturbed case, the surface temperatures are kept unchanged with respect to the reference RCP4.5 case. When combined, surface cooling and lower stratospheric warming tend to stabilize the atmosphere, which decreases the turbulence and updraft velocities (−10&thinsp;% in our modeling study). The net effect is an induced cirrus thinning, which may then produce a significant indirect negative radiative forcing (RF). This RF would go in the same direction as the direct effect of solar radiation scattering by aerosols, and would consequently influence the amount of sulfur needed to counteract the positive RF due to greenhouse gases. In our study, given an 8&thinsp;Tg-SO2&thinsp;yr−1 equatorial injection into the lower stratosphere, an all-sky net tropopause RF of −1.46&thinsp;W&thinsp;m−2 is calculated, of which −0.3&thinsp;W&thinsp;m−2 (20&thinsp;%) is from the indirect effect on cirrus thinning (6&thinsp;% reduction in ice optical depth). When surface cooling is ignored, the ice optical depth reduction is lowered to 3&thinsp;%, with an all-sky net tropopause RF of −1.4&thinsp;W&thinsp;m−2, of which −0.14&thinsp;W&thinsp;m−2 (10&thinsp;%) is from cirrus thinning. Relative to the clear-sky net tropopause RF due to SG aerosols (−2.1&thinsp;W&thinsp;m−2), the cumulative effect of the background clouds and cirrus thinning accounts for +0.6&thinsp;W&thinsp;m−2, due to the partial compensation of large positive shortwave (+1.6&thinsp;W&thinsp;m−2) and negative longwave adjustments (−1.0&thinsp;W&thinsp;m−2). When surface cooling is ignored, the net cloud adjustment becomes +0.8&thinsp;W&thinsp;m−2, with the shortwave contribution (+1.5&thinsp;W&thinsp;m−2) almost twice as much as that of the longwave (−0.7&thinsp;W&thinsp;m−2). This highlights the importance of including all of the dynamical feedbacks of SG aerosols.</p

The potential to narrow uncertainty in projections of stratospheric ozone over the 21st century

Future stratospheric ozone concentrations will be determined both by changes in the concentration of ozone depleting substances (ODSs) and by changes in stratospheric and tropospheric climate, including those caused by changes in anthropogenic greenhouse gases (GHGs). Since future economic development pathways and resultant emissions of GHGs are uncertain, anthropogenic climate change could be a significant source of uncertainty for future projections of stratospheric ozone. In this pilot study, using an "ensemble of opportunity" of chemistry-climate model (CCM) simulations, the contribution of scenario uncertainty from different plausible emissions pathways for ODSs and GHGs to future ozone projections is quantified relative to the contribution from model uncertainty and internal variability of the chemistry-climate system. For both the global, annual mean ozone concentration and for ozone in specific geographical regions, differences between CCMs are the dominant source of uncertainty for the first two-thirds of the 21st century, up-to and after the time when ozone concentrations return to 1980 values. In the last third of the 21st century, dependent upon the set of greenhouse gas scenarios used, scenario uncertainty can be the dominant contributor. This result suggests that investment in chemistry-climate modelling is likely to continue to refine projections of stratospheric ozone and estimates of the return of stratospheric ozone concentrations to pre-1980 levels

Uncertainties and assessments of chemistry-climate models of the stratosphere

In recent years a number of chemistry-climate models have been developed with an emphasis on the stratosphere. Such models cover a wide range of time scales of integration and vary considerably in complexity. The results of specific diagnostics are here analysed to examine the differences amongst individual models and observations, to assess the consistency of model predictions, with a particular focus on polar ozone. For example, many models indicate a significant cold bias in high latitudes, the “cold pole problem”, particularly in the southern hemisphere during winter and spring. This is related to wave propagation from the troposphere which can be improved by improving model horizontal resolution and with the use of non-orographic gravity wave drag. As a result of the widely differing modelled polar temperatures, different amounts of polar stratospheric clouds are simulated which in turn result in varying ozone values in the models. The results are also compared to determine the possible future behaviour of ozone, with an emphasis on the polar regions and mid-latitudes. All models predict eventual ozone recovery, but give a range of results concerning its timing and extent. Differences in the simulation of gravity waves and planetary waves as well as model resolution are likely major sources of uncertainty for this issue. In the Antarctic, the ozone hole has probably reached almost its deepest although the vertical and horizontal extent of depletion may increase slightly further over the next few years. According to the model results, Antarctic ozone recovery could begin any year within the range 2001 to 2008. The limited number of models which have been integrated sufficiently far indicate that full recovery of ozone to 1980 levels may not occur in the Antarctic until about the year 2050. For the Arctic, most models indicate that small ozone losses may continue for a few more years and that recovery could begin any year within the range 2004 to 2019. The start of ozone recovery in the Arctic is therefore expected to appear later than in the Antarctic