Abstract: Gobal methane emissions were estimated for 2000–2012 using the CarbonTracker Europe-CH4 (CTE-CH4) data assimilation system. In CTE-CH4, the anthropogenic and biosphere emissions of CH4 are simultaneously constrained by global atmospheric in-situ methane mole fraction observations. We use three configurations developed in Tsuruta et al. (2016) to assess the sensitivity of the CH4 flux estimates to (a) the number of unknown flux scaling factors to be optimized which in turn depends on the choice of underlying land-ecosystem map, and (b) on the parametrization of vertical mixing in the 30 atmospheric transport model TM5. The posterior emission estimates were evaluated by comparing simulations to surface in-situ observation sites, to profile observations made by aircraft, to dry air total column-averaged mole fractions (XCH4) observations from the Total Carbon Column Observing Network (TCCON), and to XCH4 retrievals from the Greenhouse gases Observing SATellite (GOSAT). Our estimated posterior mean global total emissions during 2000–2012 are 516 $\pm$ 51 Tg CH4 yr\textminus1, and emission estimates during 2007–2012 are 18 Tg CH4 yr\textminus1 greater than those from 2001–2006, mainly driven by an 35 increase in emissions from the south America temperate region, the Asia temperate region and Asia tropics. The sensitivity of the flux estimates to the underlying ecosystem map was large for the Asia temperate region and Australia, but not significant in the northern latitude regions, i.e. the north American boreal region, the north American temperate region and Europe. Instead, the posterior estimates for the northern latitude regions show larger sensitivity to the choice of convection scheme in TM5. The Gregory et al. (2000) mixing scheme with faster interhemispheric exchange leads to higher estimated CH4 emissions at northern latitudes, and lower emissions in southern latitudes, compared to the estimates using Tiedtke (1989) convection scheme. Our evaluation with non-assimilated observations showed that posterior mole fractions were better matched with the 5 observations when Gregory et al. (2000) convection scheme was used.

Abstract: In this paper, we present a description of the tropospheric chemistry component of the UK Chemistry and Aerosols (UKCA) model which has been coupled to the Met Office Hadley Centre's HadGEM family of climate models. We assess the model's transport and scavenging processes, in particular focussing on convective transport, boundary layer mixing, wet scavenging and inter-hemispheric exchange. Simulations with UKCA of the short-lived radon tracer suggest that modelled distributions are comparable to those of other models and the comparison with observations indicate that apart from a few locations, boundary layer mixing and convective transport are effective in the model as a means of vertically redistributing surface emissions of radon. Comparisons of modelled lead tracer concentrations with observations suggest that UKCA captures surface concentrations in both hemispheres very well, although there is a tendency to underestimate the observed geographical and interannual variability in the Northern Hemisphere. In particular, UKCA replicates the shape and absolute concentrations of observed lead profiles, a key test in the evaluation of a model's wet scavenging scheme. The timescale for inter-hemispheric transport, calculated in the model using a simple krypton tracer experiment, does appear to be long relative to other models and could indicate deficiencies in tropical deep convection and/or insufficient boundary layer mixing. We also describe the main components of the tropospheric chemistry and evaluate it against observations and other tropospheric chemistry models. In particular, from a climate forcing perspective, present-day observed surface methane concentrations and tropospheric ozone concentrations are reproduced very well by the model, thereby making it suitable for long centennial integrations as well as studies of biogeochemical feedbacks. Results from both historical and future simulations with UKCA tropospheric chemistry are presented. Future projections of tropospheric ozone vary with the Representative Concentration Pathway (RCP). In RCP2.6, for example, tropospheric ozone increases up to 2010 and then declines by 13% of its year-2000 global mean by the end of the century. In RCP8.5, tropospheric ozone continues to rise steadily throughout the 21st century, with methane being the main driving factor. Finally, we highlight aspects of the UKCA model which are undergoing and/or have undergone recent developments and are suitable for inclusion in a next-generation Earth System Model.