ALBERT

Description: The precise contribution of the two major sinks for anthropogenic CO2 emissions, terrestrial vegetation and the ocean, and their location and year-to-year variability are not well understood. Top-down estimates of the spatiotemporal variations in emissions and uptake of CO2 are expected to benefit from the increasing measurement density brought by recent in situ and remote CO2 observations. We uniquely apply a batch Bayesian synthesis inversion at relatively high resolution to in situ surface observations and bias-corrected GOSAT satellite column CO2 retrievals to deduce the global distributions of natural CO2 fluxes during 2009–2010. The GOSAT inversion is generally better constrained than the in situ inversion, with smaller posterior regional flux uncertainties and correlations, because of greater spatial coverage, except over North America and northern and southern high-latitude oceans. Complementarity of the in situ and GOSAT data enhances uncertainty reductions in a joint inversion; however, remaining coverage gaps, including those associated with spatial and temporal sampling biases in the passive satellite measurements, still limit the ability to accurately resolve fluxes down to the sub-continental or sub-ocean basin scale. The GOSAT inversion produces a shift in the global CO2 sink from the tropics to the north and south relative to the prior, and an increased source in the tropics of ∼ 2 Pg C yr−1 relative to the in situ inversion, similar to what is seen in studies using other inversion approaches. This result may be driven by sampling and residual retrieval biases in the GOSAT data, as suggested by significant discrepancies between posterior CO2 distributions and surface in situ and HIPPO mission aircraft data. While the shift in the global sink appears to be a robust feature of the inversions, the partitioning of the sink between land and ocean in the inversions using either in situ or GOSAT data is found to be sensitive to prior uncertainties because of negative correlations in the flux errors. The GOSAT inversion indicates significantly less CO2 uptake in the summer of 2010 than in 2009 across northern regions, consistent with the impact of observed severe heat waves and drought. However, observations from an in situ network in Siberia imply that the GOSAT inversion exaggerates the 2010–2009 difference in uptake in that region, while the prior CASA-GFED model of net ecosystem production and fire emissions reasonably estimates that quantity. The prior, in situ posterior, and GOSAT posterior all indicate greater uptake over North America in spring to early summer of 2010 than in 2009, consistent with wetter conditions. The GOSAT inversion does not show the expected impact on fluxes of a 2010 drought in the Amazon; evaluation of posterior mole fractions against local aircraft profiles suggests that time-varying GOSAT coverage can bias the estimation of interannual flux variability in this region.

Description: Ozone fields simulated for the first phase of the Chemistry-Climate Model Initiative (CCMI-1) will be used as forcing data in the 6th Coupled Model Intercomparison Project. Here we assess, using reference and sensitivity simulations produced for CCMI-1, the suitability of CCMI-1 model results for this process, investigating the degree of consistency amongst models regarding their responses to variations in individual forcings. We consider the influences of methane, nitrous oxide, a combination of chlorinated or brominated ozone-depleting substances, and a combination of carbon dioxide and other greenhouse gases. We find varying degrees of consistency in the models' responses in ozone to these individual forcings, including some considerable disagreement. In particular, the response of total-column ozone to these forcings is less consistent across the multi-model ensemble than profile comparisons. We analyse how stratospheric age of air, a commonly used diagnostic of stratospheric transport, responds to the forcings. For this diagnostic we find some salient differences in model behaviour, which may explain some of the findings for ozone. The findings imply that the ozone fields derived from CCMI-1 are subject to considerable uncertainties regarding the impacts of these anthropogenic forcings. We offer some thoughts on how to best approach the problem of generating a consensus ozone database from a multi-model ensemble such as CCMI-1.

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

Description: We present an overview of state-of-the-art chemistry–climate and chemistry transport models that are used within phase 1 of the Chemistry–Climate Model Initiative (CCMI-1). The CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, tropospheric composition, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI-1 recommendations for simulations have been followed is necessary to understand model responses to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI-1 simulations with the aim of informing CCMI data users.

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

Description: The precise contribution of the two major sinks for anthropogenic CO2 emissions, terrestrial vegetation and the ocean, and their location and year-to-year variability are not well understood. Top-down estimates of the spatiotemporal variations in emissions and uptake of CO2 are expected to benefit from the increasing measurement density brought by recent in situ and remote CO2 observations. We uniquely apply a batch Bayesian synthesis inversion at relatively high resolution to in situ surface observations and bias-corrected GOSAT satellite column CO2 retrievals to deduce the global distributions of natural CO2 fluxes during 2009–2010. Our objectives include evaluating bottom-up prior flux estimates, assessing the value added by the satellite data, and examining the impacts of inversion technique and assumptions on posterior fluxes and uncertainties. The GOSAT inversion is generally better constrained than the in situ inversion, with smaller posterior regional flux uncertainties and correlations, because of greater spatial coverage, except over North America and high-latitude ocean. Complementarity of the in situ and GOSAT data enhances uncertainty reductions in a joint inversion; however, spatial and temporal gaps in sampling still limit the ability to accurately resolve fluxes down to the sub-continental scale. The GOSAT inversion produces a shift in the global CO2 sink from the tropics to the north and south relative to the prior, and an increased source in the tropics of ~ 2 Pg C y−1 relative to the in situ inversion, similar to what is seen in studies using other inversion approaches. This result may be driven by sampling and residual retrieval biases in the GOSAT data, as suggested by significant discrepancies between posterior CO2 distributions and surface in situ and HIPPO mission aircraft data. While the shift in the global sink appears to be a robust feature of the inversions, the partitioning of the sink between land and ocean in the inversions using either in situ or GOSAT data is found to be sensitive to prior uncertainties because of negative correlations in the flux errors. The GOSAT inversion indicates significantly less CO2 uptake in summer of 2010 than in 2009 across northern regions, consistent with the impact of observed severe heat waves and drought. However, observations from an in situ network in Siberia imply that the GOSAT inversion exaggerates the 2010–2009 difference in uptake in that region, while the prior CASA-GFED model of net ecosystem production and fire emissions reasonably estimates that quantity. The prior, in situ posterior, and GOSAT posterior all indicate greater uptake over North America in spring to early summer of 2010 than in 2009, consistent with wetter conditions. The GOSAT inversion does not show the expected impact on fluxes of a 2010 drought in the Amazon; evaluation of posterior mole fractions against local aircraft profiles suggests that time-varying GOSAT coverage can bias estimation of flux interannual variability in this region.

Description: We present an overview of state-of-the-art chemistry-climate and chemistry transport models that are used within phase 1 of the Chemistry-Climate Model Initiative (CCMI-1). The CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, tropospheric composition, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI-1 recommendations for simulations have been followed is necessary to understand model responses to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI-1 simulations with the aim of informing CCMI data users.

Description: Ozone fields simulated for the first phase of the Chemistry-Climate Model Initiative (CCMI-1) will be used as forcing data in the 6th Coupled Model Intercomparison Project. Here we assess, using reference and sensitivity simulations produced for CCMI-1, the suitability of CCMI-1 model results for this process, investigating the degree of consistency amongst models regarding their responses to variations in individual forcings. We consider the influences of methane, nitrous oxide, a combination of chlorinated or brominated ozone-depleting substances, and a combination of carbon dioxide and other greenhouse gases. We find varying degrees of consistency in the models' responses in ozone to these individual forcings, including some considerable disagreement. In particular, the response of total-column ozone to these forcings is less consistent across the multi-model ensemble than profile comparisons. We analyse how stratospheric age of air, a commonly used diagnostic of stratospheric transport, responds to the forcings. For this diagnostic we find some salient differences in model behaviour, which may explain some of the findings for ozone. The findings imply that the ozone fields derived from CCMI-1 are subject to considerable uncertainties regarding the impacts of these anthropogenic forcings. We offer some thoughts on how to best approach the problem of generating a consensus ozone database from a multi-model ensemble such as CCMI-1.

Description: The precise contribution of the two major sinks for anthropogenic CO2 emissions, terrestrial vegetation and the ocean, and their location and year-to-year variability are not well understood. Top-down estimates of the spatiotemporal variations in emissions and uptake of CO2 are expected to benefit from the increasing measurement density brought by recent in situ and remote CO2 observations. We uniquely apply a batch Bayesian synthesis inversion at relatively high resolution to in situ surface observations and bias-corrected GOSAT satellite column CO2 retrievals to deduce the global distributions of natural CO2 fluxes during 2009-2010. Our objectives include evaluating bottom-up prior flux estimates, assessing the value added by the satellite data, and examining the impacts of inversion technique and assumptions on posterior fluxes and uncertainties. The GOSAT inversion is generally better constrained than the in situ inversion, with smaller posterior regional flux uncertainties and correlations, because of greater spatial coverage, except over North America and high-latitude ocean. Complementarity of the in situ and GOSAT data enhances uncertainty reductions in a joint inversion; however, spatial and temporal gaps in sampling still limit the ability to accurately resolve fluxes down to the subcontinental scale. The GOSAT inversion produces a shift in the global CO2 sink from the tropics to the north and south relative to the prior, and an increased source in the tropics of ~2 Pg C y(exp -1) relative to the in situ inversion, similar to what is seen in studies using other inversion approaches. This result may be driven by sampling and residual retrieval biases in the GOSAT data, as suggested by significant discrepancies between posterior CO2 distributions and surface in situ and HIPPO mission aircraft data. While the shift in the global sink appears to be a robust feature of the inversions, the partitioning of the sink between land and ocean in the inversions using either in situ or GOSAT data is found to be sensitive to prior uncertainties because of negative correlations in the flux errors. The GOSAT inversion indicates significantly less CO2 uptake in summer of 2010 than in 2009 across northern regions, consistent with the impact of observed severe heat waves and drought. However, observations from an in situ network in Siberia imply that the GOSAT inversion exaggerates the 2010-2009 difference in uptake in that region, while the prior CASA-GFED model of net ecosystem production and fire emissions reasonably estimates that quantity. The prior, in situ posterior, and GOSAT posterior all indicate greater uptake over North America in spring to early summer of 2010 than in 2009, consistent with wetter conditions. The GOSAT inversion does not show the expected impact on fluxes of a 2010 drought in the Amazon; evaluation of posterior mole fractions against local aircraft profiles suggests that time-varying GOSAT coverage can bias estimation of flux interannual variability in this region.