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.
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 for both long-term trends and short-term variations. Employing Oslo CTM3 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 model overestimates the observed growth after 2006 in all regions. This seems to be explained by an overly 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 recent 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. The atmospheric CH4 lifetime is an indicator of the CH4 loss. In our simulations, the atmospheric CH4 lifetime decreases by more than 8 % from 1970 to 2012, a significant reduction of the residence time of this important greenhouse gas. Changes in CO and NOx emissions, specific humidity, and ozone column drive most of this, and we provide simple prognostic equations for the relations between those and the CH4 lifetime. The reduced lifetime results in substantial growth in the chemical CH4 loss (relative to its burden) and dampens the CH4 growth.
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.
Key Points
Good model agreement with observations
The model reproduces the Arctic ozone deficit in 2011
Dynamics play a major role for the ozone deficit in 2011
The chemical transport model Oslo CTM3 Søvde, O. A; Prather, M. J; Isaksen, I. S. A ...
Geoscientific Model Development,
11/2012, Letnik:
5, Številka:
6
Journal Article
Recenzirano
Odprti dostop
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 NO sub(X) 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 O sub(3) 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 O sub(3), OH and the CH sub(4) 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 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.
Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This ...makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.
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.
This work describes observational and modelling results of the ozone depletion which took place during the winter/spring of 2011 in the Arctic stratosphere. Assimilated total ozone data from GOME‐2 ...were used to estimate the integrated ozone mass deficit at polar latitudes and the Oslo CTM2 model calculated low winter/spring ozone values over the Arctic, which compare well with the satellite observations. Model runs with and without chemistry in the Arctic during the winter/spring of 2011 show that the very low Arctic stratospheric air temperatures led to significant chemical ozone loss. The calculated winter/spring ozone mass deficit (O3MD) reached extreme high values in 2011 (2700 Mt) and the seasonal zonal mean total ozone extreme low values of 333DU. Dynamics have set up the conditions for cold temperatures in the lower stratosphere in winter/spring of 2011. Comparison of ozone columns with the previous 13 years shows record low ozone column values during winter/spring in the Arctic in 2011. A comparison is also given with similar model studies for the overall warmer winter/spring of 2010 which show higher ozone column values and significantly less chemical ozone loss. The interannual variability of column ozone over the northern polar region is, as expected, highly correlated with the corresponding year‐to‐year variability of the seasonally‐averaged temperatures in the lower stratosphere.
Key Points
Record low ozone decline over the Arctic
Good agreement between model and observations
High correlation between stratospheric temperatures and total ozone
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
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.
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