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We document the ability of the new-generation Oslo chemistry-transport model, Oslo CTM3, to accurately simulate present-day aerosol distributions. The model is then used with the new Community Emission Data System (CEDS) historical emission inventory to provide updated time series of anthropogenic aerosol concentrations and consequent direct radiative forcing (RFari) from 1750 to 2014.Overall, Oslo CTM3 performs well compared with measurements of surface concentrations and remotely sensed aerosol optical depth. Concentrations are underestimated in Asia, but the higher emissions in CEDS than previous inventories result in improvements compared to observations. The treatment of black carbon (BC) scavenging in Oslo CTM3 gives better agreement with observed vertical BC profiles relative to the predecessor Oslo CTM2. However, Arctic wintertime BC concentrations remain underestimated, and a range of sensitivity tests indicate that better physical understanding of processes associated with atmospheric BC processing is required to simultaneously reproduce both the observed features. Uncertainties in model input data, resolution, and scavenging affect the distribution of all aerosols species, especially at high latitudes and altitudes. However, we find no evidence of consistently better model performance across all observables and regions in the sensitivity tests than in the baseline configuration.Using CEDS, we estimate a net RFari in 2014 relative to 1750 of-0.17 W m-2, significantly weaker than the IPCC AR5 2011–1750 estimate. Differences are attributable to several factors, including stronger absorption by organic aerosol, updated parameterization of BC absorption, and reduced sulfate cooling. The trend towards a weaker RFari over recent years is more pronounced than in the IPCC AR5, illustrating the importance of capturing recent regional emission changes.

High concentrations of ozone in ambient air are hazardous not only to humans but to the ecosystem in general. The impact of ozone damage on vegetation and agricultural plants in combination with advancing climate change may affect food security in the future. While the future scenarios in themselves are uncertain, there are limiting factors constraining the accuracy of surface ozone modeling also at present: the distribution and amount of ozone precursors and ozone-depleting substances, the stratosphere–troposphere exchange, as well as scavenging processes. Removal of any substance through gravitational settling or by uptake by plants and soil is referred to as dry deposition. The process of dry deposition is important for predicting surface ozone concentrations and understanding the observed amount and increase of tropospheric background ozone. The conceptual dry deposition velocities are calculated following a resistance-analogous approach, wherein aerodynamic, quasi-laminar, and canopy resistance are key components, but these are hard to measure explicitly. We present an update of the dry deposition scheme implemented in Oslo CTM3. We change from a purely empirical dry deposition parameterization to a more process-based one which takes the state of the atmosphere and vegetation into account. We examine the sensitivity of the scheme to various parameters, e.g., the stomatal conductance-based description of the canopy resistance and the choice of ozone surface resistance, and evaluate the resulting modeled ozone dry deposition with respect to observations and multi-model studies. Individual dry deposition velocities are now available for each land surface type and agree generally well with observations. We also estimate the impact on the modeled ozone concentrations at the surface. We show that the global annual total ozone dry deposition decreases with respect to the previous model version (-37 %), leading to an increase in surface ozone of more than 100% in some regions. While high sensitivity to changes in dry deposition to vegetation is found in the tropics and the Northern Hemisphere, the largest impact on global scales is associated with the choice of prescribed ozone surface resistance over the ocean and deserts.

In the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) exercise, a range of global atmospheric general circulation and chemical transport models performed coordinated perturbation experiments with 20 % reductions in emissions of anthropogenic aerosols, or aerosol precursors, in a number of source regions. Here, we compare the resulting changes in the atmospheric load and vertically resolved profiles of black carbon (BC), organic aerosols (OA) and sulfate (SO4) from 10 models that include treatment of aerosols. We use a set of temporally, horizontally and vertically resolved profiles of aerosol forcing efficiency (AFE) to estimate the impact of emission changes in six major source regions on global radiative forcing (RF) pertaining to the direct aerosol effect, finding values between. 51.9 and 210.8 mW m−2 Tg−1 for BC, between −2.4 and −17.9 mW m−2 Tg−1 for OA and between −3.6 and −10.3 W m−2 Tg−1 for SO4. In most cases, the local influence dominates, but results show that mitigations in south and east Asia have substantial impacts on the radiative budget in all investigated receptor regions, especially for BC. In Russia and the Middle East, more than 80 % of the forcing for BC and OA is due to extra-regional emission reductions. Similarly, for North America, BC emissions control in east Asia is found to be more important than domestic mitigations, which is consistent with previous findings. Comparing fully resolved RF calculations to RF estimates based on vertically averaged AFE profiles allows us to quantify the importance of vertical resolution to RF estimates. We find that locally in the source regions, a 20 % emission reduction strengthens the radiative forcing associated with SO4 by 25 % when including the vertical dimension, as the AFE for SO4 is strongest near the surface. Conversely, the local RF from BC weakens by 37 % since BC AFE is low close to the ground. The fraction of BC direct effect forcing attributable to intercontinental transport, on the other hand, is enhanced by one-third when accounting for the vertical aspect, because long-range transport primarily leads to aerosol changes at high altitudes, where the BC AFE is strong. While the surface temperature response may vary with the altitude of aerosol change, the analysis in the present study is not extended to estimates of temperature or precipitation changes

The hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting methane lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among 10 models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D), the mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapour, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, methane, the photolysis frequency of NO2 by visible light (JNO2), overhead ozone column, and temperature account for little to no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapour on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, ozone column, and temperature are also in reasonably good agreement between the two studies.

In this paper, we compare model calculations of ozone profiles and their variability for the period 1998 to 2016 with satellite and lidar profiles at five ground-based stations. Under the investigation is the temporal impact of the stratospheric halogen reduction (chemical processes) and increase in greenhouse gases (i.e., global warming) on stratospheric ozone changes. Attention is given to the effect of greenhouse gases on ultraviolet-B radiation at ground level. Our chemistry transport and chemistry climate models (Oslo CTM3 and EMAC CCM) indicate that (a) the effect of halogen reduction is maximized in ozone recovery at 1–7 hPa and observed at all lidar stations; and (b) significant impact of greenhouse gases on stratospheric ozone recovery is predicted after the year 2050. Our study indicates that solar ultraviolet-B irradiance that produces DNA damage would increase after the year 2050 by +1.3% per decade. Such change in the model is driven by a significant decrease in cloud cover due to the evolution of greenhouse gases in the future and an insignificant trend in total ozone. If our estimates prove to be true, then it is likely that the process of climate change will overwhelm the effect of ozone recovery on UV-B irradiance in midlatitudes.

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.

In the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) exercise, a range of global atmospheric general circulation and chemical transport models performed coordinated perturbation experiments with 20 % reductions in emissions of anthropogenic aerosols, or aerosol precursors, in a number of source regions. Here, we compare the resulting changes in the atmospheric load and vertically resolved profiles of black carbon (BC), organic aerosols (OA) and sulfate (SO4) from 10 models that include treatment of aerosols. We use a set of temporally, horizontally and vertically resolved profiles of aerosol forcing efficiency (AFE) to estimate the impact of emission changes in six major source regions on global radiative forcing (RF) pertaining to the direct aerosol effect, finding values between. 51.9 and 210.8 mW m−2 Tg−1 for BC, between −2.4 and −17.9 mW m−2 Tg−1 for OA and between −3.6 and −10.3 W m−2 Tg−1 for SO4. In most cases, the local influence dominates, but results show that mitigations in south and east Asia have substantial impacts on the radiative budget in all investigated receptor regions, especially for BC. In Russia and the Middle East, more than 80 % of the forcing for BC and OA is due to extra-regional emission reductions. Similarly, for North America, BC emissions control in east Asia is found to be more important than domestic mitigations, which is consistent with previous findings. Comparing fully resolved RF calculations to RF estimates based on vertically averaged AFE profiles allows us to quantify the importance of vertical resolution to RF estimates. We find that locally in the source regions, a 20 % emission reduction strengthens the radiative forcing associated with SO4 by 25 % when including the vertical dimension, as the AFE for SO4 is strongest near the surface. Conversely, the local RF from BC weakens by 37 % since BC AFE is low close to the ground. The fraction of BC direct effect forcing attributable to intercontinental transport, on the other hand, is enhanced by one-third when accounting for the vertical aspect, because long-range transport primarily leads to aerosol changes at high altitudes, where the BC AFE is strong. While the surface temperature response may vary with the altitude of aerosol change, the analysis in the present study is not extended to estimates of temperature or precipitation changes.

Emissions of aviation include CO2, H2O, NOx, sulfur oxides, and soot. Many studies have investigated the annual mean climate impact of aviation emissions. While CO2 has a long atmospheric residence time and is almost uniformly distributed in the atmosphere, non-CO2 gases and particles and their products have short atmospheric residence times and are heterogeneously distributed. The climate impact of non-CO2 aviation emissions is known to vary with different meteorological background situations. The aim of this study is to systematically investigate the influence of characteristic weather situations on aviation climate effects over the North Atlantic region, to identify the most sensitive areas, and to potentially detect systematic weather-related similarities. If aircraft were re-routed to avoid climate-sensitive regions, the overall aviation climate impact might be reduced. Hence, the sensitivity of the atmosphere to local emissions provides a basis for the assessment of weather-related, climate-optimized flight trajectory planning. To determine the climate change contribution of an individual emission as a function of location, time, and weather situation, the radiative impact of local emissions of NOx and H2O to changes in O3, CH4, H2O and contrail cirrus was computed by means of the ECHAM5/MESSy Atmospheric Chemistry model. From this, 4-dimensional climate change functions (CCFs) were derived. Typical weather situations in the North Atlantic region were considered for winter and summer. Weather-related differences in O3, CH4, H2O, and contrail cirrus CCFs were investigated. The following characteristics were identified: enhanced climate impact of contrail cirrus was detected for emissions in areas with large-scale lifting, whereas low climate impact of contrail cirrus was found in the area of the jet stream. Northwards of 60∘ N, contrails usually cause climate warming in winter, independent of the weather situation. NOx emissions cause a high positive climate impact if released in the area of the jet stream or in high-pressure ridges, which induces a south- and downward transport of the emitted species, whereas NOx emissions at, or transported towards, high latitudes cause low or even negative climate impact. Independent of the weather situation, total NOx effects show a minimum at ∼250 hPa, increasing towards higher and lower altitudes, with generally higher positive impact in summer than in winter. H2O emissions induce a high climate impact when released in regions with lower tropopause height, whereas low climate impact occurs for emissions in areas with higher tropopause height. H2O CCFs generally increase with height and are larger in winter than in summer. The CCFs of all individual species can be combined, facilitating the assessment of total climate impact of aircraft trajectories considering CO2 and spatially and temporally varying non-CO2 effects. Furthermore, they allow for the optimization of aircraft trajectories with reduced overall climate impact. This also facilitates a fair evaluation of trade-offs between individual species. In most regions, NOx and contrail cirrus dominate the sensitivity to local aviation emissions. The findings of this study recommend considering weather-related differences for flight trajectory optimization in favour of reducing total climate impact.

Most socioeconomic pathways compatible with the aims of the Paris Agreement include large changes to land use and land cover. The associated vegetation changes can interact with the atmosphere and climate through numerous mechanisms. One of these is emissions of biogenic volatile organic compounds (BVOCs), which may lead to the formation of secondary organic aerosols (SOAs) and atmospheric chemistry changes. Here, we use a modeling framework to explore potential future global and regional changes in SOA and tropospheric ozone following idealized, large-scale vegetation perturbations, and their resulting radiative forcing (RF). Guided by projections in low-warming scenarios, we modify crop and forest cover, separately, and in concurrence with changes in anthropogenic emissions and CO2 level. We estimate that increasing global forest cover by 30% gives a 37% higher global SOA burden, with a resulting forcing of −0.13 W m−2. The effect on tropospheric ozone is relatively small. Large SOA burden changes of up to 48% are simulated for South America and Sub-Saharan Africa. Conversely, increasing crop cover at the expense of tropical forest, yields similar changes but of opposite sign. The magnitude of these changes is strongly affected by the concurrent evolution of anthropogenic emissions. Our land cover perturbations are representative of energy crop expansion and afforestation, two key mitigation measures in 1.5 °C compatible scenarios. Our results hence indicate that depending on the role of these two in the underlying mitigation strategies, scenarios with similar long-term global temperature levels could lead to opposite effects on SOA. Combined with the complexity of factors that control SOA, this highlights the importance of including BVOC effects in further studies and assessments of climate and air quality mitigation involving the land surface.

Aviation is seeking for ways to reduce its climate impact caused by CO2 emissions and non-CO2 effects. Operational measures which change overall flight altitude have the potential to reduce climate impact of individual effects, comprising CO2 but in particular non-CO2 effects. We study the impact of changes of flight altitude, specifically aircraft flying 2000 feet higher and lower, with a set of global models comprising chemistry-transport, chemistry-climate and general circulation models integrating distinct aviation emission inventories representing such alternative flight altitudes, estimating changes in climate impact of aviation by quantifying radiative forcing and induced temperature change. We find in our sensitivity study that flying lower leads to a reduction of radiative forcing of non-CO2 effects together with slightly increased CO2 emissions and impacts, when cruise speed is not modified. Flying higher increases radiative forcing of non-CO2 effects by about 10%, together with a slight decrease of CO2 emissions and impacts. Overall, flying lower decreases aviation-induced temperature change by about 20%, as a decrease of non-CO2 impacts by about 30% dominates over slightly increasing CO2 impacts assuming a sustained emissions scenario. Those estimates are connected with a large but unquantified uncertainty. To improve the understanding of mechanisms controlling the aviation climate impact, we study the geographical distributions of aviation-induced modifications in the atmosphere, together with changes in global radiative forcing and suggest further efforts in order to reduce long standing uncertainties.