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This study provides a new look at the observed and calculated long-term temperature changes from the lower troposphere to the lower stratosphere since 1958 over the Northern Hemisphere. The data sets include the NCEP/NCAR reanalysis, the Free University of Berlin (FU-Berlin) and the RICH radiosonde data sets as well as historical simulations with the CESM1-WACCM global model participating in CMIP5. The analysis is mainly based on monthly layer mean temperatures derived from geopotential height thicknesses in order to take advantage of the use of the independent FU-Berlin stratospheric data set of geopotential height data since 1957. This approach was followed to extend the records for the investigation of the stratospheric temperature trends to the earliest possible time. After removing the natural variability with an autoregressive multiple regression model our analysis shows that the period 1958-2011 can be divided into two distinct sub-periods of long-term temperature variability and trends: before and after 1980. By calculating trends for the summer time to reduce interannual variability, the two periods are as follows. From 1958 until 1979, a non-significant trend (0.06 ± 0.06 °C decade-1 for NCEP) and slightly cooling trends (-0.12 ± 0.06 °C decade-1 for RICH) are found in the lower troposphere. The second period from 1980 to the end of the records shows significant warming (0.25 ± 0.05 °C decade-1 for both NCEP and RICH). Above the tropopause a significant cooling trend is clearly seen in the lower stratosphere both in the pre-1980 period (-0.58 ± 0.17 °C decade-1 for NCEP, -0.30 ± 0.16 °C decade-1 for RICH and -0.48 ± 0.20 °C decade-1 for FU-Berlin) and the post-1980 period (-0.79 ± 0.18 °C decade-1 for NCEP, -0.66 ± 0.16 °C decade-1 for RICH and -0.82 ± 0.19 °C decade-1 for FU-Berlin). The cooling in the lower stratosphere persists throughout the year from the tropics up to 60° N. At polar latitudes competing dynamical and radiative processes reduce the statistical significance of these trends. Model results are in line with reanalysis and the observations, indicating a persistent cooling (-0.33 °C decade-1) in the lower stratosphere during summer before and after 1980; a feature that is also seen throughout the year. However, the lower stratosphere CESM1-WACCM modelled trends are generally lower than reanalysis and the observations. The contrasting effects of ozone depletion at polar latitudes in winter/spring and the anticipated strengthening of the Brewer-Dobson circulation from man-made global warming at polar latitudes are discussed. Our results provide additional evidence for an early greenhouse cooling signal in the lower stratosphere before 1980, which appears well in advance relative to the tropospheric greenhouse warming signal. The suitability of early warning signals in the stratosphere relative to the troposphere is supported by the fact that the stratosphere is less sensitive to changes due to cloudiness, humidity and man-made aerosols. Our analysis also indicates that the relative contribution of the lower stratosphere versus the upper troposphere low-frequency variability is important for understanding the added value of the long-term tropopause variability related to human-induced global warming. [ABSTRACT FROM AUTHOR]

This study provides a new look at the observed and calculated long-term temperature changes since 1958 for the region extending from the lower troposphere up to the lower stratosphere of the Northern Hemisphere. The analysis is mainly based on monthly layer mean temperatures derived from geopotential height thicknesses between specific pressure levels. Layer mean temperatures from thickness improve homogeneity in both space and time and reduce uncertainties in the trend analysis. Datasets used include the NCEP/NCAR I reanalysis, the Free University of Berlin (FU-Berlin) and the RICH radiosonde datasets as well as historical simulations with the CESM1-WACCM global model participating in CMIP5. After removing the natural variability with an autoregressive multiple regression model our analysis shows that the time interval of our study 1958-2011 can be divided in two distinct sub-periods of long term temperature variability and trends; before and after 1980s. By calculating trends for the summer time to reduce interannual variability, the two periods are as follows. From 1958 until 1979, non-significant trends or slight cooling trends prevail in the lower troposphere (0.06±0.06°C decade-1 for NCEP and -0.12±0.06°C decade-1 for RICH). The second period from 1980 to the end of the records shows significant warming trends (0.25±0.05°C decade-1 for both NCEP and RICH). Above the tropopause a persistent cooling trend is clearly seen in the lower stratosphere both in the pre-1980s period (-0.58±0.17°C decade for NCEP, -0.30±0.16°C decade-1 for RICH and -0.48±0.20°C decade for FU-Berlin) and the post-1980s period (-0.79±0.18°C decade for NCEP, -0.66±0.16°C decade for RICH and -0.82±0.19°C decade for FU-Berlin). The cooling in the lower stratosphere is a persistent feature from the tropics up to 60 north for all months. At polar latitudes competing dynamical and radiative processes are reducing the statistical significance of these trends. Model results are in line with re-analysis and the observations, indicating a persistent cooling in the lower stratosphere during summer before and after the 1980s by -0.33°C decade ; a feature that is also seen throughout the year. However, the lower stratosphere modelled trends are generally lower than re-analysis and the observations. The contrasting effects of ozone depletion at polar latitudes in winter/spring and the anticipated strengthening of the Brewer Dobson circulation from man-made global warming at polar latitudes are discussed. Our results provide additional evidence for an early greenhouse cooling signal in the lower stratosphere before the 1980s, which it appears well in advance relative to the tropospheric greenhouse warming signal. Hence it may be postulated that the stratosphere could have provided an early warning of man-made climate change. The suitability for early warning signals in the stratosphere relative to the troposphere is supported by the fact that the stratosphere is less sensitive to changes due to cloudiness, humidity and manmade aerosols. Our analysis also indicates that the relative contribution of the lower stratosphere vs. the upper troposphere low frequency variability is important for understanding the added value of the long term tropopause variability related to human induced global warming. [ABSTRACT FROM AUTHOR]

The results of a comparison between monthly mean ozone column variations calculated from the chemical transport model Oslo CTM2 and those derived from solar backscatter ultraviolet (SBUV) satellite observations are presented for the period 1998-2009. Monthly mean total ozone derived from improved model simulations were used to compute monthly zonal means over 10° latitude zones over the northern and southern hemispheres. Ozone column variations from Oslo CTM2 are highly correlated with SBUV retrievals at all latitude zones. Equatorial zonal winds at 30 hPa were used as index to study the impact of quasi-biennial oscillation (QBO) on ozone. Correlations between modeled ozone and the QBO were found to be the order of +0.8 in the tropics. The impact of QBO was most pronounced at equatorial latitudes with amplitudes of +4 to −4 %. Seasonal variations in surface ozone and tropospheric ozone column calculated by the model are also presented. [ABSTRACT FROM AUTHOR]

The future impact of traffic emissions on atmospheric ozone and OH has been investigated separately for the three sectors AIRcraft, maritime SHIPping and ROAD traffic. To reduce uncertainties we present results from an ensemble of six different atmospheric chemistry models, each simulating the atmospheric chemical composition in a possible high emission scenario (A1B), and with emissions from each transport sector reduced by 5% to estimate sensitivities. Our results are compared with optimistic future emission scenarios (B1 and B1 ACARE), presented in a companion paper, and with the recent past (year 2000). Present-day activity indicates that anthropogenic emissions so far evolve closer to A1B than the B1 scenario. As a response to expected changes in emissions, AIR and SHIP will have increased impacts on atmospheric O3 and OH in the future while the impact of ROAD traffic will decrease substantially as a result of technological improvements. In 2050, maximum aircraft-induced O3 occurs near 80° N in the UTLS region and could reach 9 ppbv in the zonal mean during summer. Emissions from ship traffic have their largest O3 impact in the maritime boundary layer with a maximum of 6 ppbv over the North Atlantic Ocean during summer in 2050. The O3 impact of road traffic emissions in the lower troposphere peaks at 3 ppbv over the Arabian Peninsula, much lower than the impact in 2000. Radiative forcing (RF) calculations show that the net effect of AIR, SHIP and ROAD combined will change from a marginal cooling of -0.44 ± 13 mW m-2 in 2000 to a relatively strong cooling of -32 ± 9.3 (B1) or -32 ± 18 mW m-2 (A1B) in 2050, when taking into account RF due to changes in O3, CH4 and CH4-induced O3. This is caused both by the enhanced negative net RF from SHIP, which will change from -19 ± 5.3 mW m-2 in 2000 to -31 ± 4.8 (B1) or -40 ± 9 mW m-2 (A1B) in 2050, and from reduced O3 warming from ROAD, which is likely to turn from a positive net RF of 12 ± 8.5 mW m-2 in 2000 to a slightly negative net RF of -3.1 ± 2.2 (B1) or -3.1 ± 3.4 (A1B) mW m-2 in the middle of this century. The negative net RF from ROAD is temporary and induced by the strong decline in ROAD emissions prior to 2050, which only affects the methane cooling term due to the longer lifetime of CH4 compared to O3. The O3 RF from AIR in 2050 is strongly dependent on scenario and ranges from 19 ± 6.8 (B1 ACARE) to 61 ± 14 mW m-2 (A1B). There is also a considerable span in the net RF from AIR in 2050, ranging from -0.54 ± 4.6 (B1 ACARE) to 12 ± 11 (A1B) mW m-2 compared to 6.6 ± 2.2 mW m-2 in 2000. [ABSTRACT FROM AUTHOR]

Several graphs regarding the chemical transport model Oslo (CTM)3 are presented.

The impact of future emissions from aviation and shipping on the atmospheric chemical composition has been estimated using an ensemble of six different atmospheric chemistry models. This study considers an optimistic emission scenario (B1) taking into account e.g. rapid introduction of clean and resource-efficient technologies, and a mitigation option for the aircraft sector (B1 ACARE), assuming further technological improvements. Results from sensitivity simulations, where emissions from each of the transport sectors were reduced by 5 %, show that emissions from both aircraft and shipping will have a larger impact on atmospheric ozone and OH in near future (2025; B1) and for longer time horizons (2050; B1) compared to recent time (2000). However, the ozone and OH impact from aircraft can be reduced substantially in 2050 if the technological improvements considered in the B1 ACARE will be achieved. Shipping emissions have the largest impact in the marine boundary layer and their ozone contribution may exceed 4 ppbv (when scaling the response of the 5% emission perturbation to 100% by applying a factor 20) over the North Atlantic Ocean in the future (2050; B1) during northern summer (July). In the zonal mean, ship-induced ozone relative to the background levels may exceed 12% near the surface. Corresponding numbers for OH are 6.0x105 molecules cm-3 and 30 %, respectively. This large impact on OH from shipping leads to a relative methane lifetime reduction of 3.92 (±0.48)% on the global average in 2050 B1 (ensemble mean CH4 lifetime is 8.0 (±1.0) yr), compared to 3.68 (±0.47)% in 2000. Aircraft emissions have about 4 times higher ozone enhancement efficiency (ozone molecules enhanced relative to NOx molecules emitted) than shipping emissions, and the maximum impact is found in the UTLS region. Zonal mean aircraft-induced ozone could reach up to 5 ppbv at northern mid- and high latitudes during future summer (July 2050; B1), while the relative impact peaks during northern winter (January) with a contribution of 4.2 %. Although the aviation-induced impact on OH is lower than for shipping, it still causes a reduction in the relative methane lifetime of 1.68 (±0.38)% in 2050 B1. However, for B1 ACARE the perturbation is reduced to 1.17 (±0.28) %, which is lower than the year 2000 estimate of 1.30 (±0.30) %. Based on the fully scaled perturbations we calculate net radiative forcings from the six models taking into account ozone, methane (including stratospheric water vapour), and methane-induced ozone changes. For the B1 scenario, shipping leads to a net cooling with radiative forcings of -28.0 (±5.1) and -30.8 (±4.8)mWm-2 in 2025 and 2050, respectively, due to the large impact on OH and, thereby, methane lifetime reductions. Corresponding values for the aviation sector shows a net warming effect with 3.8 (±6.1) and 1.9 (±6.3)mWm-2, respectively, but with a small net cooling of -0.6 (±4.6)mW m-2 for B1 ACARE in 2050. [ABSTRACT FROM AUTHOR]

The article presents a study on the Atmospheric Composition Change: the European Network (ACCENT) model evaluation protocol which is a framework for model evaluation and benchmarking. It mentions its basis on input data from observational and modelling communities. It also notes various steps from global model applications which involve purpose, guidelines and processes.

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The sulfur cycle and radiative effects of sulfate aerosol on climate are studied with a Global tropospheric Climate-Chemistry Model in which chemistry, radiation and dynamics are fully coupled. Production and removal mechanisms of sulfate are analyzed for the conditions of natural and anthropogenic sulfur emissions. Results show that the 1985 anthropogenic emission doubled the global SO2 and sulfate loadings from its natural value of 0.15 and 0.27 Tg S, respectively. Under natural conditions, the fraction of sulfate produced in-cloud is 87%, and the lifetime of SO2 and sulfate are 1.8 and 4.0 days, respectively; whereas with anthropogenic emissions, changes in in-cloud sulfate production are small, while SO2 and sulfate lifetimes are significant reduced (1.0 and 2.4 days, respectively). The doubling of sulfate results in a direct radiative forcing of -0.32 and -0.14 W m-2 under clear-sky and all-sky conditions, respectively, and a significant first indirect forcing of -1.69 W m-2. The first indirect forcing is sensitive to the relationship between aerosol concentration and cloud droplet number concentration. Two aspects of chemistry-climate interaction are addressed. Firstly, the coupling effects lead to 10% and 2% decreases in sulfate loading, respectively, for the cases of natural and anthropogenic added sulfur emissions. Secondly, only the indirect effect of sulfate aerosols yields significantly stronger signals in changes of near surface temperature and sulfate loading than changes due to intrinsic climate variability, while other responses to the indirect effect and all responses to the direct effect are weak. [ABSTRACT FROM AUTHOR]

The effect of anthropogenic emissions from China on global burdens of ozone, sulphate, organic carbon (OC) and black carbon (BC) aerosols is examined, using the three-dimensional chemistry transport model Oslo CTM2. Two model simulations were performed, the first with global present-day emissions and the second with the anthropogenic emissions from China set to their pre-industrial levels. The global radiative forcing for these species is then calculated. Industrial emissions from China are found to account for a 4–5% increase in the global burden of OC aerosol, the change in secondary organic aerosol being slightly less than that of primary organic aerosol. A 10% increase in the global sulphate aerosol burden is calculated, and the increase in BC is 23%. The global radiative forcing of aerosols from China was calculated to be −62, −3.7, −13 and 89 mW m−2, for sulphate, secondary organic, primary organic and BC aerosols, respectively. The increase in ozone causes a forcing of 77 mW m−2. [ABSTRACT FROM AUTHOR]

To estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH in the present-day atmosphere six different atmospheric chemistry models have been used. Based on newly developed global emission inventories for road, ship and aircraft emission data sets each model performed sensitivity simulations reducing the emissions of each transport sector by 5%. The model results indicate that on global annual average lower tropospheric ozone responds most sensitive to ship emissions (50.6%±10.9% of the total traffic induced perturbation), followed by road (36.7%±9.3%) and aircraft exhausts (12.7%±2.9%), respectively. In the northern upper troposphere between 200-300 hPa at 30-60° N the maximum impact from road and ship are 93% and 73% of the maximum effect of aircraft, respectively. The latter is 0.185 ppbv for ozone (for the 5% case) or 3.69 ppbv when scaling to 100%. On the global average the impact of road even dominates in the UTLS-region. The sensitivity of ozone formation per NOx molecule emitted is highest for aircraft exhausts. The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 0.2 DU and occurs over the northern subtropical Atlantic extending to central Europe. Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine lower troposphere over the Atlantic. Based on the 5% perturbation the effect on ozone can exceed 0.6% close to the marine surface (global zonal mean) which is 80% of the total traffic induced ozone perturbation. In the southern hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%-80% throughout the year. Methane lifetime changes against OH are affected strongest by ship emissions up to 0.21 (± 0.05)%, followed by road (0.08 (±0.01)%) and air traffic (0.05 (± 0.02)%). Based on the full scale ozone and methane perturbations positive radiative forcings were calculated for road emissions (7.3±6.2 mWm-2) and for aviation (2.9±2.3 mWm-2). Ship induced methane lifetime changes dominate over the ozone forcing and therefore lead to a net negative forcing (-25.5±13.2 mWm-2). [ABSTRACT FROM AUTHOR]

European emission trends of nitrogen oxides since 1880 and up to present are presented here and are linked to the evolution of road transport emissions. Road transport has been the dominating source of NOx emissions since 1970, and contributes with 40% to the total emissions in 2005. Five trend regimes have been identified between 1880 and 2005. The first regime (1880-1950) is determined by a slow increase in fuel consumption all over Europe. The second regime (1950-1980) is characterized by a continued steep upward trend in liquid fuel use and by the introduction of the first regulations on road traffic emissions. Reduction in fuel consumption determines the emission trends in the third regime (1980-1990) that is also characterized by important differences between Eastern and Western Europe. Emissions from road traffic continue to grow in Western Europe in this period, and it is argued here that the reason for this continued NOx emission increase is related to early inefficient regulations for NOx in the transport sector. The fourth regime (1990-2000) involves a turning point for road traffic emissions, with a general decrease of emissions in Europe during that decade. It is in this period that we can identify the first emission reductions due to technological abatement in Western Europe. In the fifth regime (2000-2005), the economic recovery in Eastern Europe imposes increased emission from road traffic in this area. Western European emissions are on the other hand decoupled from the fuel consumption, and continue to decrease. The implementation of strict measures to control NOx emissions is demonstrated here to be a main reason for the continued Western European emission reductions. The results indicate that even though the effectiveness of European standards is hampered by a slow vehicle turnover, loopholes in the type-approval testing, and an increase in diesel consumption, the effect of such technical abatement measures is traceable in the evolution of European road traffic emissions over the last 15 years. [ABSTRACT FROM AUTHOR]

The pre-industrial and present day distributions and burdens of Secondary Organic Aerosol (SOA) have been calculated using the off-line aerosol chemistry transport model Oslo CTM2. The production of SOA was found to have increased from about 43 Tg yr-1 to 69 Tg yr-1 since pre-industrial times, leading to an increase in the global annual mean SOA burden from 0.44 Tg to 0.70 Tg, or about 59%. The increases are greatest over industrialised areas, as well as over regions with high biogenic precursor emissions. The contribution of emissions from different sources to the larger SOA burdens has been calculated. The results suggest that the majority of the increase is caused by emissions of primary organic aerosols (POA), from fossil fuel and bio fuel combustion. When SOA partitioning to ammonium sulphate aerosol was not accounted for, the increase in SOA burden between pre-industrial times and the present was found to be lower (51%), with a production increase of 55%. As yet, very few radiative forcing estimates of SOA exist, and no such estimates were provided in the latest IPCC report. In this study, we find that the change in SOA burden caused a radiative forcing of -0.09Wm-2, when SOA was allowed to partition to both organic and sulphate aerosols, and -0.06Wm-2 when only partitioning to organic aerosols was assumed. Therefore, the radiative forcing of SOA is found to be substantially stronger than the best estimate for POA in the latest IPCC assessment. [ABSTRACT FROM AUTHOR]

A high-resolution global aerosol model (Oslo CTM2) driven by meteorological data and allowing a comparison with a variety of aerosol observations is used to simulate radiative forcing (RF) of the direct aerosol effect. The model simulates all main aerosol components, including several secondary components such as nitrate and secondary organic carbon. The model reproduces the main chemical composition and size features observed during large aerosol campaigns. Although the chemical composition compares best with ground-based measurement over land for modelled sulphate, no systematic differences are found for other compounds. The modelled aerosol optical depth (AOD) is compared to remote sensed data from AERONET ground and MODIS and MISR satellite retrievals. To gain confidence in the aerosol modelling, we have tested its ability to reproduce daily variability in the aerosol content, and this is performing well in many regions; however, we also identified some locations where model improvements are needed. The annual mean regional pattern of AOD from the aerosol model is broadly similar to the AERONET and the satellite retrievals (mostly within 10-20%). We notice a significant improvement from MODIS Collection 4 to Collection 5 compared to AERONET data. Satellite derived estimates of aerosol radiative effect over ocean for clear sky conditions differs significantly on regional scales (almost up to a factor two), but also in the global mean. The Oslo CTM2 has an aerosol radiative effect close to the mean of the satellite derived estimates. We derive a radiative forcing (RF) of the direct aerosol effect of -0.35Wm-2 in our base case. Implementation of a simple approach to consider internal black carbon (BC) mixture results in a total RF of -0.28Wm-2. Our results highlight the importance of carbonaceous particles, producing stronger individual RF than considered in the recent IPCC estimate; how ever, net RF is less different. A significant RF from secondary organic aerosols (SOA) is estimated (close to -0.1Wm-2). The SOA also contributes to a strong domination of secondary aerosol species for the aerosol composition over land. A combination of sensitivity simulations and model evaluation show that the RF is rather robust and unlikely to be much stronger than in our best estimate. [ABSTRACT FROM AUTHOR]