J. E. Williams

Three decades of global methane sources and sinks

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.

The influence of biomass burning and transport on tropospheric composition over the tropical Atlantic Ocean and Equatorial Africa during the West African monsoon in 2006

Biomass burning (BB) in southern Africa is the largest emission source of CO and O 3 precursors within Africa during the West African Monsoon (WAM) between June and August. The long range transport and chemical processing of such emissions thus has the potential to exert a dominant influence on the composition of the tropical troposphere over Equatorial Africa (EA) and the Tropical Atlantic Ocean (TAO). We have performed simulations using a three-dimensional global chemistry-transport model (CTM) to quantify the effect that continental transport of such BB plumes has on the EA region. BB emissions from southern Africa were found to exert a significant influence over the TAO and EA between 10 ◦ S–20 N. The maximum concentrations in CO and O3 occur between 0–5 ◦ S near the position of the African Easterly Jet – South as placed by the European Centre for Medium range Weather Forecasts (ECMWF) meteorological analysis data. By comparing co-located model output with in-situ measurements we show that the CTM fails to capture the tropospheric profile of CO in southern Africa near the main source region of the BB emissions, as well as the “extreme” concentrations of both CO and O 3 seen between 600–700 hPa over EA around 6 ◦ N. For more northerly locations the model exhibits high background concentrations in both CO and O3 related to BB emissions from southern Africa. By altering both the temporal resolution and the vertical distribution of BB emissions in the model we show that Correspondence to: J. E. Williams (williams@knmi.nl) changes in temporal resolution have the largest influence on the transport of trace gases near the source regions, EA, and in the outflow towards the west of Central Africa. Using a set of trajectory calculations we show that the performance of the CTM is heavily constrained by the ECMWF meteorological fields used to drive the CTM, which transport biomass burning plumes from southern Africa into the lower troposphere of the TAO rather than up towards the middle troposphere at 650 hPa. Similar trajectory simulations repeated using an updated meteorological dataset, which assimilates additional measurement data taken around EA, show markedly different origins for pollution events and highlight the current limitations in modelling this tropical region.

Global Chemistry Simulations in the AMMA Multimodel Intercomparison Project

The authors present results obtained during the chemistry-transport modeling (CTM) component of the African Monsoon Multi-disciplinary Analysis Multimodel Intercomparison Project (AMMA-MIP) using the recently developed L3JRCv2 emission dataset for Af-rica, where emphasis is placed on the summer of 2006. With the use of passive tracers, the authors show that the application of different parameterizations to describe advection, vertical diffusion, and convective mixing in a suite of state-of-the-art global CTMs results in significantly different transport mechanisms westward of the African continent. Moreover, the authors identify that the atmospheric composition over the southern Atlantic is governed by air masses originating from southern Africa for this period, resulting in maximal concentrations around 5°S. Comparisons with ozonesonde measurements at Cotonou (6.2°N, 2.2°E) indicate that the models generally overpredict surface ozone and underpredict ozone in the upper troposphere. Moreover, using recent aircraft measurements, the authors show that the high ozone concentrations that occur around 700 hPa around 5°N are not captured by any of the models, indicating shortcomings in the description of transport, the magnitude and/or location of emissions, or the in situ chemical ozone production by the various chemical mechanisms employed.

The effect of stratospheric sulfur from Mount Pinatubo on tropospheric oxidizing capacity and methane

The eruption of Mount Pinatubo in 1991 injected a large amount of SO2 into the stratosphere, which formed sulfate aerosols. Increased scattering and absorption of UV radiation by the enhanced stratospheric SO2 and aerosols decreased the amount of UV radiation reaching the troposphere, causing changes in tropospheric photochemistry. These changes affected the oxidizing capacity of the atmosphere and the removal rate of CH4 in the years following the eruption. We use the three-dimensional chemistry transport model TM5 coupled to the aerosol microphysics module M7 to simulate the evolution of SO2 and sulfate aerosols from the Pinatubo eruption. Their effect on tropospheric photolysis frequencies and concentrations of OH and CH4 is quantified for the first time. We find that UV attenuation by stratospheric sulfur decreased the photolysis frequencies of both ozone and NO2 by about 2% globally, decreasing global OH concentrations by a similar amount in the first 2 years after the eruption. SO2 absorption mainly affects OH primary production by ozone photolysis, while aerosol scattering also alters OH recycling. The effect of stratospheric sulfur on global OH and CH4 is dominated by the effect of aerosol extinction, while SO2 absorption contributes by 12.5% to the overall effect in the first year after the eruption. The reduction in OH concentrations causes an increase in the CH4 growth rate of 4 and 2 ppb/yr in the first and second years after the eruption, respectively, contributing 11 Tg to the 27 Tg observed CH4 burden change in late 1991 and early 1992.

Uncertainty in the Future Distribution of Tropospheric Ozone over West Africa due to Variability in Anthropogenic Emissions Estimates between 2025 and 2050

Particle and trace gas emissions due to anthropogenic activity are expected to increase significantly in West Africa over the next few decades due to rising population and more energy intensive lifestyles. Here we perform 3D global chemistry-transport model calculations for 2025 and 2050 using both a “business-as-usual” (A1B) and “clean economy” (B1) future anthropogenic emission scenario to focus on the changes in the distribution and uncertainties associated with tropospheric O3 due to the various projected emission scenarios. When compared to the present-day troposphere we find that there are significant increases in tropospheric O3 for the A1B emission scenario, with the largest increases being located in the lower troposphere near the source regions and into the Sahel around 15–20°N. In part this increase is due to more efficient NOx re-cycling related to increases in the background methane concentrations. Examining the uncertainty across different emission inventories reveals that there is an associated uncertainty of up to ~20% in the predicted increases at 2025 and 2050. For the upper troposphere, where increases in O3 have a more pronounced impact on radiative forcing, the uncertainty is influenced by transport of O3 rich air from Asia on the Tropical Easterly Jet.

Top-down NO x emissions of european cities based on the downwind plume of modelled and space-borne tropospheric NO 2 columns

Top-down estimates of surface NOX emissions were derived for 23 European cities based on the downwind plume decay of tropospheric nitrogen dioxide (NO2) columns from the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) chemistry transport model (CTM) and from Ozone Monitoring Instrument (OMI) satellite retrievals, averaged for the summertime period (April–September) during 2013. Here we show that the top-down NOX emissions derived from LOTOS-EUROS for European urban areas agree well with the bottom-up NOX emissions from the MACC-III inventory data (R2 = 0.88) driving the CTM demonstrating the potential of this method. OMI top-down NOX emissions over the 23 European cities are generally lower compared with the MACC-III emissions and their correlation is slightly lower (R2 = 0.79). The uncertainty on the derived NO2 lifetimes and NOX emissions are on average ~55% for OMI and ~63% for LOTOS-EUROS data. The downwind NO2 plume method applied on both LOTOS-EUROS and OMI tropospheric NO2 columns allows to estimate NOX emissions from urban areas, demonstrating that this is a useful method for real-time updates of urban NOX emissions with reasonable accuracy.