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Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimat

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimat

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimat

The CH4 growth rate in the atmosphere showed large variations after the Pinatubo eruption in June 1991. A decrease of more than 10 ppb yr-1 in the growth rate over the course of 1992 was reported, and a partial recovery in the following year. Although several reasons have been proposed to explain the evolution of CH4 after the eruption, their contributions to the observed variations are not yet resolved. CH4 is removed from the atmosphere by the reaction with tropospheric OH, which in turn is produced by O3 photolysis under UV radiation. The CH4 removal after the Pinatubo eruption might have been affected by changes in tropospheric UV levels due to the presence of stratospheric SO2 and sulfate aerosols, and due to enhanced ozone depletion on Pinatubo aerosols. The perturbed climate after the eruption also altered both sources and sinks of atmospheric CH4. Furthermore, CH4 concentrations were influenced by other factors of natural variability in that period, such as El Niño-Southern Oscillation (ENSO) and biomass burning events. Emissions of CO, NOX and non-methane volatile organic compounds (NMVOCs) also affected CH4 concentrations indirectly by influencing tropospheric OH levels. Potential drivers of CH4 variability are investigated using the TM5 global chemistry model. The contribution that each driver had to the global CH4 variability during the period 1990 to 1995 is quantified. We find that a decrease of 8-10 ppb yr-1 CH4 is explained by a combination of the above processes. However, the timing of the minimum growth rate is found 6-9 months later than observed. The long-term decrease in CH4 growth rate over the period 1990 to 1995 is well captured and can be attributed to an increase in OH concentrations over this time period. Potential uncertainties in our modelled CH4 grow

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bott

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bott

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (g1/4 biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003-2012 decade, global methane emissions are estimated by top-down inversions at 558g Tgg CH4g yrg'1, range 540-568. About 60g % of global emissions are anthropogenic (range 50-65g %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenar

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bott

The UV index (UVI) and dose (UVD) are quantities of UV irradiance weighted for its effect on organisms. Both quantities are widely used as informative tools or as proxies for UV irradiance, commonly used in e.g. skin cancer research. The UVI and UVD can be measured using groundbased spectrometers, or modelled using satellite observations of ozone. The Royal Netherlands Meteorological Institute has developed a UV model with a unique spatial and temporal coverage. This study describes the update of this model. Updates include changing the computation and data sets used, regarding: ground elevation, surface albedo, cloud cover and error estimation. The updated model is used to compute UVI and UVD from the long-term Multi-Sensor Reanalysis of ozone, and compared with ozone fields that would have been present if the 1987 Montreal Protocol had not been adopted. We find that the northern hemisphere ozone depletion event of 2011, which is greatly exaggerated in absence of the Montreal Protocol, has only little effect on UV irradiance. Comparing scenarios with and without Montreal Protocol, we find that by the year 2012 the implementation of the Montreal Protocol has prevented UV levels from shifting nearly 10 degrees poleward in summer, an increased global sunburn rate by 9.9%, while also preventing a 14.5% increase in (sun related) vitamin D production. For UVD thresholds relevant for vitamin D sufficiency, we found an order of magnitude estimation of the effect of the Montreal Protocol: Removing part of the ozone layer, which the Montreal Protocol prevented, has a similar effect on surface UV irradiance as removing all cloud cover throughout the year.

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bott

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (g1/4 biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003-2012 decade, global methane emissions are estimated by top-down inversions at 558g Tgg CH4g yrg'1, range 540-568. About 60g % of global emissions are anthropogenic (range 50-65g %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenar

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (~biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (T-D, exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories, and data-driven approaches (B-U, including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by T-D inversions at 558 Tg CH4 yr−1 (range [540–568]). About 60 % of global emissions are anthropogenic (range [50–65 %]). B-U approaches suggest larger global emissions (736 Tg CH4 yr−1 [596–884]) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources

The UV index (UVI) and dose (UVD) are quantities of UV irradiance weighted for its effect on organisms. Both quantities are widely used as informative tools or as proxies for UV irradiance, commonly used in e.g. skin cancer research. The UVI and UVD can be measured using groundbased spectrometers, or modelled using satellite observations of ozone. The Royal Netherlands Meteorological Institute has developed a UV model with a unique spatial and temporal coverage. This study describes the update of this model. Updates include changing the computation and data sets used, regarding: ground elevation, surface albedo, cloud cover and error estimation. The updated model is used to compute UVI and UVD from the long-term Multi-Sensor Reanalysis of ozone, and compared with ozone fields that would have been present if the 1987 Montreal Protocol had not been adopted. We find that the northern hemisphere ozone depletion event of 2011, which is greatly exaggerated in absence of the Montreal Protocol, has only little effect on UV irradiance. Comparing scenarios with and without Montreal Protocol, we find that by the year 2012 the implementation of the Montreal Protocol has prevented UV levels from shifting nearly 10 degrees poleward in summer, an increased global sunburn rate by 9.9%, while also preventing a 14.5% increase in (sun related) vitamin D production. For UVD thresholds relevant for vitamin D sufficiency, we found an order of magnitude estimation of the effect of the Montreal Protocol: Removing part of the ozone layer, which the Montreal Protocol prevented, has a similar effect on surface UV irradiance as removing all cloud cover throughout the year.

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bott

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bott

The CH4 growth rate in the atmosphere showed large variations after the Pinatubo eruption in June 1991. A decrease of more than 10 ppb yr-1 in the growth rate over the course of 1992 was reported, and a partial recovery in the following year. Although several reasons have been proposed to explain the evolution of CH4 after the eruption, their contributions to the observed variations are not yet resolved. CH4 is removed from the atmosphere by the reaction with tropospheric OH, which in turn is produced by O3 photolysis under UV radiation. The CH4 removal after the Pinatubo eruption might have been affected by changes in tropospheric UV levels due to the presence of stratospheric SO2 and sulfate aerosols, and due to enhanced ozone depletion on Pinatubo aerosols. The perturbed climate after the eruption also altered both sources and sinks of atmospheric CH4. Furthermore, CH4 concentrations were influenced by other factors of natural variability in that period, such as El Niño-Southern Oscillation (ENSO) and biomass burning events. Emissions of CO, NOX and non-methane volatile organic compounds (NMVOCs) also affected CH4 concentrations indirectly by influencing tropospheric OH levels. Potential drivers of CH4 variability are investigated using the TM5 global chemistry model. The contribution that each driver had to the global CH4 variability during the period 1990 to 1995 is quantified. We find that a decrease of 8-10 ppb yr-1 CH4 is explained by a combination of the above processes. However, the timing of the minimum growth rate is found 6-9 months later than observed. The long-term decrease in CH4 growth rate over the period 1990 to 1995 is well captured and can be attributed to an increase in OH concentrations over this time period. Potential uncertainties in our modelled CH4 growth rate include emissions of CH4 from wetlands, biomass burning emissions of CH4 and other compounds, biogenic NMVOC and the sensitivity of OH to NMVOC emission changes. Two inventories are

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (~biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (T-D, exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories, and data-driven approaches (B-U, including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by T-D inversions at 558 Tg CH4 yr−1 (range [540–568]). About 60 % of global emissions are anthropogenic (range [50–65 %]). B-U approaches suggest larger global emissions (736 Tg CH4 yr−1 [596–884]) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (~biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (T-D, exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories, and data-driven approaches (B-U, including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by T-D inversions at 558 Tg CH4 yr−1 (range [540–568]). About 60 % of global emissions are anthropogenic (range [50–65 %]). B-U approaches suggest larger global emissions (736 Tg CH4 yr−1 [596–884]) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (~biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (T-D, exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories, and data-driven approaches (B-U, including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by T-D inversions at 558 Tg CH4 yr−1 (range [540–568]). About 60 % of global emissions are anthropogenic (range [50–65 %]). B-U approaches suggest larger global emissions (736 Tg CH4 yr−1 [596–884]) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (~biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (T-D, exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories, and data-driven approaches (B-U, including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by T-D inversions at 558 Tg CH4 yr−1 (range [540–568]). About 60 % of global emissions are anthropogenic (range [50–65 %]). B-U approaches suggest larger global emissions (736 Tg CH4 yr−1 [596–884]) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources

Methane is an important greenhouse gas, responsible for about 20% of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios-which differ in fossil fuel and microbial emissions-to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain. © 2013 Macmillan Publishers Limited.

Methane is an important greenhouse gas, responsible for about 20% of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios-which differ in fossil fuel and microbial emissions-to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain. © 2013 Macmillan Publishers Limited.

The global methane (CH4) growth rate showed large variations after the eruption of Mount Pinatubo in June 1991. Both sources and sinks of tropospheric CH4 were altered following the eruption, by feedback processes between climate and tropospheric photochemistry. Such processes include Ultra Violet (UV) radiative changes due to the presence of volcanic sulfur dioxide (SO2) and sulphate aerosols in the stratosphere, and due to stratospheric ozone depletion. Changes in temperature and water vapour in the following years caused changes in tropospheric chemistry, as well as in natural emissions. We present a sensitivity study that investigates the relative effects that these processes had on tropospheric CH4 concentrations, using a simple one-dimensional chemistry model representative for the global tropospheric column. To infer the changes in UV radiative fluxes, the chemistry model is coupled to a radiative transfer model. We find that the overall effect of natural processes after the eruption on the CH4 growth rate is dominated by the reduction in CH4 lifetime due to stratospheric ozone depletion. However, all the other processes are found to have non-negligible effects, and should therefore be taken into account in order to obtain a good estimate of CH4 concentrations after Pinatubo. We find that the overall effect was a small initial increase in the CH4 growth rate after the eruption, followed by a decrease of about 7 ppb yr(-1) by mid-1993. When changes in anthropogenic emissions are employed according to emission inventories, an additional decrease of about 5 ppb yr(-1) in the CH4 growth rate is obtained between the years 1991 and 1993. The results using the simplified single column model are in good qualitative agreement with observed changes in the CH4 growth rate. Further analysis, taking into account changes in the dynamics of the atmosphere, variations in emissions from biomass burning, and in biogenic emissions of non-methane volatile organic compounds (NMVO

The global methane growth rate showed large variations after the eruption of Mount Pinatubo in June 1991. Both sources and sinks of tropospheric methane were altered following the eruption, by feedback processes between climate and photo-chemistry. 5 Such processes include Ultra Violet (UV) radiative changes due to the presence of volcanic sulfur dioxide (SO2) and sulphate aerosols in the stratosphere, and due to stratospheric ozone depletion. Changes in temperature and water vapour in the following years caused changes in the tropospheric chemistry, as well as in natural emissions. We quantify the effects that these processes had on methane concentrations using a 10 one-dimensional chemistry model representative for the global tropospheric column. To infer the changes in UV radiative fluxes, we couple the chemistry model to a radiative transfer model. We find that the overall effect of the eruption on the methane growth rate is dominated by the effect of stratospheric ozone depletion. However, all the other processes are found to have non-negligible effects, and should therefore be 15 taken into account in order to obtain a good estimate of methane concentrations after the eruption. We find that the overall effect was a small initial increase in the methane growth rate after the eruption, then a decrease by about 8 ppbyr−1 by mid-1993. When changes in anthropogenic emissions are employed according to emission inventories, an additional decrease of about 5 ppbyr−1 in the methane growth rate is obtained be20 tween the years 1991 and 1993.

We present a comprehensive description and benchmark evaluation of the tropospheric chemistry version of the global chemistry transport model TM5 (Tracer Model 5, version TM5-chem-v3.0). A full description is given concerning the photochemical mechanism, the interaction with aerosol, the treatment of the stratosphere, the wet and dry deposition parameterizations, and the applied emissions. We evaluate the model against a suite of ground-based, satellite, and aircraft measurements of components critical for understanding global photochemistry for the year 2006. The model exhibits a realistic oxidative capacity at a global scale. The methane lifetime is ~8.9 years with an associated lifetime of methyl chloroform of 5.86 years, which is similar to that derived using an optimized hydroxyl radical field. The seasonal cycle in observed carbon monoxide (CO) is well simulated at different regions across the globe. In the Northern Hemisphere CO concentrations are underestimated by about 20 ppbv in spring and 10 ppbv in summer, which is related to missing chemistry and underestimated emissions from higher hydrocarbons, as well as to uncertainties in the seasonal variation of CO emissions. The model also captures the spatial and seasonal variation in formaldehyde tropospheric columns as observed by SCIAMACHY. Positive model biases over the Amazon and eastern United States point to uncertainties in the isoprene emissions as well as its chemical breakdown. Simulated tropospheric nitrogen dioxide columns correspond well to observations from the Ozone Monitoring Instrument in terms of its seasonal and spatial variability (with a global spatial correlation coefficient of 0.89), but TM5 fields are lower by 25–40%. This is consistent with earlier studies pointing to a high bias of 0–30% in the OMI retrievals, but uncertainties in the emission inventories have probably also contributed to the discrepancy. TM5 tropospheric nitrogen dioxide profiles are in good agreement (within ~0.1 pp

We present a comprehensive description and benchmark evaluation of the tropospheric chemistry version of the global chemistry transport model TM5 (Tracer Model 5, version TM5-chem-v3.0). A full description is given concerning the photochemical mechanism, the interaction with aerosol, the treatment of the stratosphere, the wet and dry deposition parameterizations, and the applied emissions. We evaluate the model against a suite of ground-based, satellite, and aircraft measurements of components critical for understanding global photochemistry for the year 2006. The model exhibits a realistic oxidative capacity at a global scale. The methane lifetime is ~8.9 years with an associated lifetime of methyl chloroform of 5.86 years, which is similar to that derived using an optimized hydroxyl radical field. The seasonal cycle in observed carbon monoxide (CO) is well simulated at different regions across the globe. In the Northern Hemisphere CO concentrations are underestimated by about 20 ppbv in spring and 10 ppbv in summer, which is related to missing chemistry and underestimated emissions from higher hydrocarbons, as well as to uncertainties in the seasonal variation of CO emissions. The model also captures the spatial and seasonal variation in formaldehyde tropospheric columns as observed by SCIAMACHY. Positive model biases over the Amazon and eastern United States point to uncertainties in the isoprene emissions as well as its chemical breakdown. Simulated tropospheric nitrogen dioxide columns correspond well to observations from the Ozone Monitoring Instrument in terms of its seasonal and spatial variability (with a global spatial correlation coefficient of 0.89), but TM5 fields are lower by 25–40%. This is consistent with earlier studies pointing to a high bias of 0–30% in the OMI retrievals, but uncertainties in the emission inventories have probably also contributed to the discrepancy. TM5 tropospheric nitrogen dioxide profiles are in good agreement (within ~0.1 pp

Chemically active climate compounds are either primary compounds like methane (CH4), removed by oxidation in the atmosphere, or secondary compounds like ozone (O3), sulfate and organic aerosols, both formed and removed in the atmosphere. Man-induced climate–chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate–chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds like O3 and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds like O3, and of particles inducing both direct and indirect effects. Through EU projects like ACCENT, QUANTIFY, and the AeroCom project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric–tropospheric exchange of ozone, more frequent periods with stable conditions favoring pollution build up over industrial areas, enhanced temperature induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentrati

Chemically active climate compounds are either primary compounds like methane (CH4), removed by oxidation in the atmosphere, or secondary compounds like ozone (O3), sulfate and organic aerosols, both formed and removed in the atmosphere. Man-induced climate–chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate–chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds like O3 and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds like O3, and of particles inducing both direct and indirect effects. Through EU projects like ACCENT, QUANTIFY, and the AeroCom project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric–tropospheric exchange of ozone, more frequent periods with stable conditions favoring pollution build up over industrial areas, enhanced temperature induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentrati

The UV/Vis/near infrared spectrometer SCIAMACHY on board the European ENVISAT satellite enables total column retrieval of atmospheric methane with high sensitivity to the lower troposphere. The vertical column density of methane is converted to column averaged mixing ratio by using carbon dioxide retrievals as proxy for the probed atmospheric column. For this purpose, we apply concurrent total column measurements of CO2 in combination with modeled column-averaged CO2 mixing ratios. Possible systematic errors are discussed in detail while the precision error is 1.8% on average. This paper focuses on methane retrievals from January 2003 through December 2004. The measurements with global coverage over continents are compared with model results from the chemistry–transport model TM4. In the retrievals, the north-south gradient as well as regions with enhanced methane levels can be clearly identified. The highest abundances are found in the Red Basin of China, followed by northern South America, the Gangetic plains of India and central parts of Africa. Especially the abundances in northern South America and the Red Basin are generally higher than modeled. Further, we present the seasonal variations within the investigated time period. Peak values in Asia due to rice emissions are observed from August through October. We expand earlier investigations that suggest underestimated emissions in the tropics. It is shown that these underestimations show a seasonal behavior that peaks from August through December. The global measurements may be used for inverse modeling and are thus an important step towards better quantification of the methane budget.

Two sets of sea surface temperature/sea ice changes are used to test the sensitivity of tracer transport to the pattern of warming in the doubled CO2 climate. One set (2CO2WT) has greater tropical and high latitude sea surface temperature changes than the other (2CO2), although both fall within the range of plausible response. Simulations were done both with and without interactive ozone. Results show that the SST pattern affects the circulation change throughout the troposphere and middle atmosphere; the ozone interaction affects primarily the upper stratosphere, but through wave-mean flow interaction has effects that extend down into the upper troposphere. Both experiments feature increased tropospheric/stratospheric exchange at low latitudes and greater vertical mixing within the troposphere; only the WT experiments result in increased interhemispheric transport and a more direct circulation in the high latitude stratosphere. Ozone increases in the upper stratosphere and decreases in the lower stratosphere in all the simulations, with greater transport of high latitude ozone into the troposphere in the WT runs. At sea level there is a more positive phase of the Arctic Oscillation (AO)-type oscillation, and this is also true at 100 mbar, but there is no significance in the middle troposphere and the sign is different in the middle stratosphere. Many of these results differ from those generated in older versions of the GISS GCMAM despite the same SST forcing due to differences in control run characteristics, which has implications for model intercomparison experiments.

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.

[1] The photolysis frequency of NO2, j(NO2), was determined by various instrumental techniques and calculated using a number of radiative transfer models for 4 days in June 1998 at the International Photolysis Frequency Measurement and Modeling Intercomparison (IPMMI) in Boulder, Colorado. Experimental techniques included filter radiometry, spectroradiometry, and chemical actinometry. Eight research groups participated using 14 different instruments to determine j( NO2). The blind intercomparison experimental results were submitted to the independent experimental referee and have been compared. Also submitted to the modeling referee were the results of NO2 photolysis frequency calculations for the same time period made by 13 groups who used 15 different radiative transfer models. These model results have been compared with each other and also with the experimental results. The model calculation of clear-sky j(NO2) values can yield accurate results, but the accuracy depends heavily on the accuracy of the molecular parameters used in these calculations. The instrumental measurements of j(NO2) agree to within the uncertainty of the individual instruments and indicate the stated uncertainties in the instruments or the uncertainties of the molecular parameters may be overestimated. This agreement improves somewhat with the use of more recent NO2 cross-section data reported in the literature.

[1] The International Photolysis Frequency Measurement and Model Intercomparison (IPMMI) took place in Boulder, Colorado, from 15 to 19 June 1998, aiming to investigate the level of accuracy of photolysis frequency and spectral downwelling actinic flux measurements and to explore the ability of radiative transfer models to reproduce the measurements. During this period, 2 days were selected to compare model calculations with measurements, one cloud-free and one cloudy. A series of ancillary measurements were also performed and provided parameters required as input to the models. Both measurements and modeling were blind, in the sense that no exchanges of data or calculations were allowed among the participants, and the results were objectively analyzed and compared by two independent referees. The objective of this paper is, first, to present the results of comparisons made between measured and modeled downwelling actinic flux and irradiance spectra and, second, to investigate the reasons for which some of the models or measurements deviate from the others. For clear skies the relative agreement between the 16 models depends strongly on solar zenith angle (SZA) and wavelength as well as on the input parameters used, like the extraterrestrial (ET) solar flux and the absorption cross sections. The majority of the models (11) agreed to within about +/-6% for solar zenith angles smaller than similar to60degrees. The agreement among the measured spectra depends on the optical characteristics of the instruments (e.g., slit function, stray light rejection, and sensitivity). After transforming the measurements to a common spectral resolution, two of the three participating spectroradiometers agree to within similar to10% for wavelengths longer than 310 nm and at all solar zenith angles, while their differences increase when moving to shorter wavelengths. Most models agree well with the measurements (both downwelling actinic flux and global irradiance), especially at local n

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.

Two sets of sea surface temperature/sea ice changes are used to test the sensitivity of tracer transport to the pattern of warming in the doubled CO2 climate. One set (2CO2WT) has greater tropical and high latitude sea surface temperature changes than the other (2CO2), although both fall within the range of plausible response. Simulations were done both with and without interactive ozone. Results show that the SST pattern affects the circulation change throughout the troposphere and middle atmosphere; the ozone interaction affects primarily the upper stratosphere, but through wave-mean flow interaction has effects that extend down into the upper troposphere. Both experiments feature increased tropospheric/stratospheric exchange at low latitudes and greater vertical mixing within the troposphere; only the WT experiments result in increased interhemispheric transport and a more direct circulation in the high latitude stratosphere. Ozone increases in the upper stratosphere and decreases in the lower stratosphere in all the simulations, with greater transport of high latitude ozone into the troposphere in the WT runs. At sea level there is a more positive phase of the Arctic Oscillation (AO)-type oscillation, and this is also true at 100 mbar, but there is no significance in the middle troposphere and the sign is different in the middle stratosphere. Many of these results differ from those generated in older versions of the GISS GCMAM despite the same SST forcing due to differences in control run characteristics, which has implications for model intercomparison experiments.

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.

Ozone is an air quality problem today for much of the world's population. Regions can exceed the ozone air quality standards (AQS) through a combination of local emissions, meteorology favoring pollution episodes, and the clean-air baseline levels of ozone upon which pollution builds. The IPCC 2001 assessment studied a range of global emission scenarios and found that all but one projects increases in global tropospheric ozone during the 21st century. By 2030, near-surface increases over much of the northern hemisphere are estimated to be about 5 ppb (+2 to +7 ppb over the range of scenarios). By 2100 the two more extreme scenarios project baseline ozone increases of >20 ppb, while the other four scenarios give changes of -4 to +10 ppb. Even modest increases in the background abundance of tropospheric ozone might defeat current AQS strategies. The larger increases, however, would gravely threaten both urban and rural air quality over most of the northern hemisphere.