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We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north–south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34%). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6%) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change in global mean tropospheric CO and NOx burdens (ΔCO/ΔNOx, approximately represents changes in OH sinks versus changes in OH sources) in the models, pointing to a need for better constraints on natural precursor emissions and on the chemical mechanisms in the current generation of chemistry-climate models. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH (3.5 ± 2.2%) leads to a 4.3 ± 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present-day climate change decreased the methane lifetime by about four months, representing a negative feedback on the climate system. Further, we analysed attribution experiments performed by a subset of models relative to 2000 conditions with only one precursor at a time set to 1860 levels. We find that global mean OH increased by 46.4 ± 12.2% in response to preindustrial to present-day anthropogenic NOx emission increases, and decreased by 17.3 ± 2.3%, 7.6 ± 1.5%, and 3.1 ± 3.0% due to methane burden, and anthropogenic CO, and NMVOC emissions increases, respectively.

We quantify the concentrations changes and Radiative Forcing (RF) of short-lived atmospheric pollutants due to shipping emissions of NOx, SOx, CO, NMVOCs, BC and OC. We use high resolution ship emission inventories for the Arctic that are more suitable for regional scale evaluation than those used in former studies. A chemical transport model and a RF model are used to evaluate the time period 2004–2030, when we expect increasing traffic in the Arctic region. Two datasets for ship emissions are used that characterize the potential impact from shipping and the degree to which shipping controls may mitigate impacts: a high (HIGH) scenario and a low scenario with Maximum Feasible Reduction (MFR) of black carbon in the Arctic. In MFR, BC emissions in the Arctic are reduced with 70% representing a combination technology performance and/or reasonable advances in single-technology performance. Both scenarios result in moderate to substantial increases in concentrations of pollutants both globally and in the Arctic. Exceptions are black carbon in the MFR scenario, and sulfur species and organic carbon in both scenarios due to the future phase-in of current regulation that reduces fuel sulfur content. In the season with potential transit traffic through the Arctic in 2030 we find increased concentrations of all pollutants in large parts of the Arctic. Net global RFs from 2004–2030 of 53 mW m−2 (HIGH) and 73 mW m−2 (MFR) are similar to those found for preindustrial to present net global aircraft RF. The found warming contrasts with the cooling from historical ship emissions. The reason for this difference and the higher global forcing for the MFR scenario is mainly the reduced future fuel sulfur content resulting in less cooling from sulfate aerosols. The Arctic RF is largest in the HIGH scenario. In the HIGH scenario ozone dominates the RF during the transit season (August–October). RF due to BC in air, and snow and ice becomes significant during Arctic spring. For the HIGH scenario the net Arctic RF during spring is 5 times higher than in winter.

Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (±1 standard deviation) in RFs of ±17%. Three different radiation schemes were used – we find differences in RFs between schemes (for the same ozone fields) of ±10%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44±12%), nitrogen oxides (31 ± 9%), carbon monoxide (15 ± 3%) and non-methane volatile organic compounds (9 ± 2%); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m−2 DU−1, a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m−2; relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

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.

Shipping is a growing sector in the global economy, and it contributions to global CO2 emissions are expected to increase. CO2 emissions from the world shipping fleet will likely be regulated in the near future, and studies have shown that significant emission reductions can be achieved at low cost. Regulations are being discussed for both existing ships as well as for future additions to the fleet. In this study a plausible CO2 emission reduction inventory is constructed for the cargo fleet existing in 2010, as well as for container ships, bulk ships and tankers separately. In the reduction inventories, CO2 emissions are reduced by 25–32% relative to baseline by applying 15 technical and operational emission reduction measures in accordance with a ship-type-specific cost-effectiveness criterion, and 9 other emission compounds are changed as a technical implication of reducing CO2. The overall climate and environmental effects of the changes to all 10 emission components in the reduction inventory are assessed using a chemical transport model, radiative forcing (RF) models and a simple climate model. We find substantial environmental and health benefits with up to 5% reduction in surface ozone levels, 15% reductions in surface sulfate and 10% reductions in wet deposition of sulfate in certain regions exposed to heavy ship traffic. The major ship types show distinctly different contributions in specific locations. For instance, the container fleet contributes 50% of the sulfate decline on the west coast of North America. The global radiative forcing from a 1 yr emission equal to the difference between baseline and reduction inventory shows an initial strong positive forcing from non-CO2 compounds. This warming effect is due to reduced cooling by aerosols and methane. After approximately 25 yr, the non-CO2 forcing is balanced by the CO2 forcing. For the global mean temperature change, we find a shift from warming to cooling after approximately 60 yr. The major ship types show significant differences in the short-term radiative forcing. For instance, the direct SO4 forcing from tankers is 30% higher than for container and bulk. The net long-term effects on RF are similar due to similar CO2 forcing. We assess an emission scenario where the reduction inventory is sustained on the fleet as it steadily diminishes over time due to scrapping and disappears in 2040. We find a net temperature increase lasting until approximately 2080. We conclude that changes in non-CO2 emission does matter significantly if reductions of CO2 emissions are made on the year 2010 cargo shipping fleet. In sum, we find that emission changes motivated by CO2 reductions in shipping will be beneficial from a long-term climate perspective, and that there are positive environmental and health effects identified as concentrations of key short-lived pollutants are reduced.

We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5–20 ppb) in the Southern Hemisphere (SH) and modest high bias (5–10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005–2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120 mW m−2 OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39 ± 41 m Wm−2 relative to TES data. We show that there is a correlation (R2 = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750–2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100 m Wm−2. Removing these models leads to a mean ozone radiative forcing of 394 ± 42 m Wm−2. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 ± 60 m Wm−2 derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

Results from simulations performed for the Atmospheric Chemistry and Climate Modeling Intercomparison Project (ACCMIP) are analysed to examine how OH and methane lifetime may change from present day to the future, under different climate and emissions scenarios. Present day (2000) mean tropospheric chemical lifetime derived from the ACCMIP multi-model mean is 9.8 ± 1.6 yr (9.3 ± 0.9 yr when only including selected models), lower than a recent observationally-based estimate, but with a similar range to previous multi-model estimates. Future model projections are based on the four Representative Concentration Pathways (RCPs), and the results also exhibit a large range. Decreases in global methane lifetime of 4.5 ± 9.1% are simulated for the scenario with lowest radiative forcing by 2100 (RCP 2.6), while increases of 8.5 ± 10.4% are simulated for the scenario with highest radiative forcing (RCP 8.5). In this scenario, the key driver of the evolution of OH and methane lifetime is methane itself, since its concentration more than doubles by 2100 and it consumes much of the OH that exists in the troposphere. Stratospheric ozone recovery, which drives tropospheric OH decreases through photolysis modifications, also plays a partial role. In the other scenarios, where methane changes are less drastic, the interplay between various competing drivers leads to smaller and more diverse OH and methane lifetime responses, which are difficult to attribute. For all scenarios, regional OH changes are even more variable, with the most robust feature being the large decreases over the remote oceans in RCP8.5. Through a regression analysis, we suggest that differences in emissions of non-methane volatile organic compounds and in the simulation of photolysis rates may be the main factors causing the differences in simulated present day OH and methane lifetime. Diversity in predicted changes between present day and future OH was found to be associated more strongly with differences in modelled temperature and stratospheric ozone changes. Finally, through perturbation experiments we calculated an OH feedback factor (F) of 1.24 from present day conditions (1.50 from 2100 RCP8.5 conditions) and a climate feedback on methane lifetime of 0.33 ± 0.13 yr K−1, on average. Models that did not include interactive stratospheric ozone effects on photolysis showed a stronger sensitivity to climate, as they did not account for negative effects of climate-driven stratospheric ozone recovery on tropospheric OH, which would have partly offset the overall OH/methane lifetime response to climate change.

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.

Emissions of short-lived climate forcers (SLCF) in the Arctic region are expected to increase, notably from shipping and petroleum extraction. We here discuss changes in atmospheric SLCF concentrations and resulting radiative forcing (RF) from present day shipping and petroleum activities in the Arctic. The three-dimensional chemistry transport OsloCTM2 and a state of the art radiative forcing model are used, based on a coherent dataset of present day Arctic emissions. We find that the net RF of SLCF of shipping in the Arctic region is negative, mainly due to the direct and indirect RF effects of sulphate emissions, while the net RF of SLCF of petroleum extraction is positive, mainly due to the effects of black carbon aerosols in the air and deposited on snow. Strong seasonal variations of the sensitivities to emissions are found. In terms of annual mean values we find that the Arctic sensitivities to SLCF is similar to global average sensitivities. One exception to this is the stronger snow/ice albedo effect from BC emissions.

A reliable and up-to-date ship emission inventory is essential for atmospheric scientists quantifying the impact of shipping and for policy makers implementing regulations and incentives for emission reduction. The emission modelling in this study takes into account ship type and size dependent input data for 15 ship types and 7 size categories. Global port arrival and departure data for more than 32 000 merchant ships are used to establish operational profiles for the ship segments. The modelled total fuel consumption amounts to 217 Mt in 2004 of which 11 Mt is consumed in in-port operations. This is in agreement with international sales statistics. The modelled fuel consumption is applied to develop global emission inventories for CO2, NO2, SO2, CO, CH4, VOC (Volatile Organic Compounds), N2O, BC (Black Carbon) and OC (Organic Carbon). The global emissions from ships at sea and in ports are distributed geographically, applying extended geographical data sets covering about 2 million global ship observations and global port data for 32 000 ships. In addition to inventories for the world fleet, inventories are produced separately for the three dominating ship types, using ship type specific emission modelling and traffic distributions. A global Chemical Transport Model (CTM) was used to calculate the environmental impacts of the emissions. We find that ship emissions is a dominant contributor over much of the world oceans to surface concentrations of NO2 and SO2. The contribution is also large over some coastal zones. For surface ozone the contribution is high over the oceans but clearly also of importance over Western North America (contribution 15–25%) and Western Europe (5–15%). The contribution to tropospheric column ozone is up to 5–6%. The overall impact of ship emissions on global methane lifetime is large due to the high NOx emissions. With regard to acidification we find that ships contribute 11% to nitrate wet deposition and 4.5% to sulphur wet deposition globally. In certain coastal regions the contributions may be in the range 15–50%. In general we find that ship emissions have a large impact on acidic deposition and surface ozone in Western North America, Scandinavia, Western Europe, western North Africa and Malaysia/Indonesia. For most of these regions container traffic, the largest emitter by ship type, has the largest impact. This is the case especially for the Pacific and the related container trade routes between Asia and North America. However, the contributions from bulk ships and tank vessels are also significant in the above mentioned impact regions. Though the total ship impact at low latitudes is lower, the tank vessels have a quite large contribution at low latitudes and near the Gulf of Mexico and Middle East. The bulk ships are characterized by large impact in Oceania compared to other ship types. In Scandinavia and north-Western Europe, one of the major ship impact regions, the three largest ship types have rather small relative contributions. The impact in this region is probably dominated by smaller ships operating closer to the coast. For emissions in ports impacts on NO2 and SO2 seem to be of significance. For most ports the contribution to the two components is in the range 0.5–5%, for a few ports it exceeds 10%. The approach presented provides an improvement in characterizing fleet operational patterns, and thereby ship emissions and impacts. Furthermore, the study shows where emission reductions can be applied to most effectively minimize the impacts by different ship types.

No abstract available.