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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

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 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 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) 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.

[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.

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.

The validity of a radiative transfer model can be checked either by comparing its results with measurements or with solutions for artificial cases. Unfortunately, neither type of comparison can guarantee that the spectral UV surface irradiance is accurately calculated for real atmospheric cases. There is a need therefore for benchmarks, i.e., standard results that can be used as a validation tool for UV radiation models. In this paper we give such benchmarks for six cloud-free situations. The chosen cases are characterized by different values of solar zenith angle, ozone column, aerosol loading, and surface albedo. Observations are also available for these cases to allow a further comparison between model results and measurements. An intercomparison of 12 numerical models is used to construct the benchmarks. Each model is supplied with identical input data, and a distinction is made between models that assume a planeparallel geometry and those that use a pseudospherical approximation. Differences remain between the model results, because of different treatments of the input data set. Calculations of direct and global transmission and direct and global irradiance are within 3% for wavelengths longer than 320 nm. For the low-Sun cases the calculations are within 10% for wavelengths longer than 300 nm. On the basis of these calculations, six benchmark UV spectra (295–400 nm) are established with a standard deviation of 2%. Relative standard deviations are higher for the lowest absolute intensities at low Sun (5% at 300 nm). The variation between models is typically less than the variation seen between model and measurement. Differences between the benchmarks and the observed spectra are mainly due to the uncertainty in the input parameters. In four of the six cases the benchmarks agree with the observed spectra within 13% over the whole UV spectral region.

RIVM rapport:Het mondiale vliegverkeer is de laatste decennia sterk gestegen en groeit naar verwachting in de komende 20 jaar met 5-6% per jaar. De emissies van sporengassen door het vliegverkeer, zoals kooldioxide, stikstofoxiden, koolwaterstoffen, zwaveldioxide, waterdamp en roet kunnen effecten hebben op het milieu en direct en indirect bijdragen aan klimaatveranderingen. Het AIRFORCE project (Aircraft Influences and Radiative Forcing from Emissions) is een project van de drie onderzoeksinstituten (IMAU, KNMI en RIVM) die samen het Nederlands Centrum voor Klimaatonderzoek (CKO) vormen. De doelstellingen van AIRFORCE zijn: onderzoek naar het effect van vliegtuigemissies op de samenstelling van de atmosfeer en naar de directe en indirecte effecten van vliegtuigemissies via de stralings-forcering op het klimaat. De modelresultaten laten zien dat NOx emissies van het huidige vliegverkeer een toename veroorzaken van de NOx- en ozonconcentraties in de hoge troposfeer en lage stratosfeer, hetgeen leidt tot een positieve stralingsforcering. In het project is de dynamica en het chemisch mechanisme van enkele drie dimensionale chemie-transportmodellen (CTMK/TM3 en MOGUNTIA) sterk verbeterd. De resultaten van modelberekeningen zijn vergeleken met beschikbare metingen van de STREAM/AIRFORCE en POLINAT campagnes. In het kader van AIRFORCE is een pluimmodel ontwikkeld dat de chemische omzettingen in de pluim direct achter verkeersvliegtuigen beschrijft., Global air traffic has increased extensively during the last few decades and is expected to increase further over the next 20 years by about 5-6% per year. Emissions of trace gases such as carbon dioxide, nitrogen oxides, hydrocarbons, sulphur oxides, water vapour and soot from aircraft can have environmental effects and contribute directly or indirectly to global warming. The three institutes (IMAU, KNMI en RIVM) that form the Netherlands Centre for Climate Research (CKO) participated in the AIRFORCE project (Aircraft Influences and Radiative Forcing from Emissions). The goals of AIRFORCE are: Research on the effect of aircraft emissions on the composition of the atmosphere and on the direct and indirect effects of aircraft emissions on radiative forcing and climate. The model results indicate that NOx emissions from aircraft cause an increase in the NOx and ozone concentrations in the upper troposphere and lower stratosphere, and a positive radiative forcing. The dynamical and chemical mechanisms of several 3-dimensional chemical-transport models (CTMK/TM3 and MOGUNTIA) have been improved considerable in the project. The results have been compared with available measurements from the STREAM/AIRFORCE and POLINAT campaigns. To account for the chemical conversion and dispersion directly behind an aircraft, an aircraft plume model has been developed in the AIRFORCE project, to translate the aircraft NOx emissions into effective emissions that are used as input in the chemical transport models.