David A. Plummer

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.

Assessment of temperature, trace species, and ozone in chemistry-climate model simulations of the recent past

Simulations of the stratosphere from thirteen coupled chemistry-climate models (CCMs) are evaluated to provide guidance for the interpretation of ozone predictions made by the same CCMs. The focus of the evaluation is on how well the fields and processes that are important for determining the ozone distribution are represented in the simulations of the recent past. The core period of the evaluation is from 1980 to 1999 but long-term trends are compared for an extended period (1960–2004). Comparisons of polar high-latitude temperatures show that most CCMs have only small biases in the Northern Hemisphere in winter and spring, but still have cold biases in the Southern Hemisphere spring below 10 hPa. Most CCMs display the correct stratospheric response of polar temperatures to wave forcing in the Northern, but not in the Southern Hemisphere. Global long-term stratospheric temperature trends are in reasonable agreement with satellite and radiosonde observations. Comparisons of simulations of methane, mean age of air, and propagation of the annual cycle in water vapor show a wide spread in the results, indicating differences in transport. However, for around half the models there is reasonable agreement with observations. In these models the mean age of air and the water vapor tape recorder signal are generally better than reported in previous model intercomparisons. Comparisons of the water vapor and inorganic chlorine (Cly) fields also show a large intermodel spread. Differences in tropical water vapor mixing ratios in the lower stratosphere are primarily related to biases in the simulated tropical tropopause temperatures and not transport. The spread in Cly, which is largest in the polar lower stratosphere, appears to be primarily related to transport differences. In general the amplitude and phase of the annual cycle in total ozone is well simulated apart from the southern high latitudes. Most CCMs show reasonable agreement with observed total ozone trends and variability on a global scale, but a greater spread in the ozone trends in polar regions in spring, especially in the Arctic. In conclusion, despite the wide range of skills in representing different processes assessed here, there is sufficient agreement between the majority of the CCMs and the observations that some confidence can be placed in their predictions.

Multimodel projections of stratospheric ozone in the 21st century

[1] Simulations from eleven coupled chemistry-climate models (CCMs) employing nearly identical forcings have been used to project the evolution of stratospheric ozone throughout the 21st century. The model-to-model agreement in projected temperature trends is good, and all CCMs predict continued, global mean cooling of the stratosphere over the next 5 decades, increasing from around 0.25 K/decade at 50 hPa to around 1 K/ decade at 1 hPa under the Intergovernmental Panel on Climate Change (IPCC) Special Report on Emissions Scenarios (SRES) A1B scenario. In general, the simulated ozone evolution is mainly determined by decreases in halogen concentrations and continued cooling of the global stratosphere due to increases in greenhouse gases (GHGs). Column ozone is projected to increase as stratospheric halogen concentrations return to 1980s levels. Because of ozone increases in the middle and upper stratosphere due to GHGinduced cooling, total ozone averaged over midlatitudes, outside the polar regions, and globally, is projected to increase to 1980 values between 2035 and 2050 and before lowerstratospheric halogen amounts decrease to 1980 values. In the polar regions the CCMs simulate small temperature trends in the first and second half of the 21st century in midwinter. Differences in stratospheric inorganic chlorine (Cly) among the CCMs are key to diagnosing the intermodel differences in simulated ozone recovery, in particular in the Antarctic. It is found that there are substantial quantitative differences in the simulated Cly, with the October mean Antarctic Cly peak value varying from less than 2 ppb to over 3.5 ppb in the CCMs, and the date at which the Cly returns to 1980 values varying from before 2030 to after 2050. There is a similar variation in the timing of recovery of Antarctic springtime column ozone back to 1980 values. As most models underestimate peak Clynear 2000, ozone recovery in the Antarctic could occur even later, between 2060 and 2070. In the Arctic the column ozone increase in spring does not follow halogen decreases as closely as in the Antarctic, reaching 1980 values before Arctic halogen amounts decrease

Impact of stratospheric ozone on Southern Hemisphere circulation change: A multimodel assessment

The impact of stratospheric ozone on the tropospheric general circulation of the Southern Hemisphere (SH) is examined with a set of chemistry-climate models participating in the Stratospheric Processes and their Role in Climate (SPARC)/Chemistry-Climate Model Validation project phase 2 (CCMVal-2). Model integrations of both the past and future climates reveal the crucial role of stratospheric ozone in driving SH circulation change: stronger ozone depletion in late spring generally leads to greater poleward displacement and intensification of the tropospheric midlatitude jet, and greater expansion of the SH Hadley cell in the summer. These circulation changes are systematic as poleward displacement of the jet is typically accompanied by intensification of the jet and expansion of the Hadley cell. Overall results are compared with coupled models participating in the Intergovernmental Panel on Climate Change Fourth Assessment Report (IPCC AR4), and possible mechanisms are discussed. While the tropospheric circulation response appears quasi-linearly related to stratospheric ozone changes, the quantitative response to a given forcing varies considerably from one model to another. This scatter partly results from differences in model climatology. It is shown that poleward intensification of the westerly jet is generally stronger in models whose climatological jet is biased toward lower latitudes. This result is discussed in the context of quasi-geostrophic zonal mean dynamics.

Chemistry-climate model simulations of twenty-first century stratospheric climate and circulation changes

The response of stratospheric climate and circulation to increasing amounts of greenhouse gases (GHGs) and ozone recovery in the twenty-first century is analyzed in simulations of 11 chemistry–climate models using near-identical forcings and experimental setup. In addition to an overall global cooling of the stratosphere in the simulations (0.59 6 0.07 K decade 21 at 10 hPa), ozone recovery causes a warming of the Southern Hemisphere polar lower stratosphere in summer with enhanced cooling above. The rate of warming correlates with the rate of ozone recovery projected by the models and, on average, changes from 0.8 to 0.48 K decade 21 at 100 hPa as the rate of recovery declines from the first to the second half of the century. In the winter northern polar lower stratosphere the increased radiative cooling from the growing abundance of GHGs is, in most models, balanced by adiabatic warming from stronger polar downwelling. In the Antarctic lower stratosphere the models simulate an increase in low temperature extremes required for polar stratospheric cloud (PSC) formation, but the positive trend is decreasing over the twenty-first century in all models. In the Arctic, none of the models simulates a statistically significant increase in Arctic PSCs throughout the twentyfirst century. The subtropical jets accelerate in response to climate change and the ozone recovery produces a westward acceleration of the lower-stratospheric wind over the Antarctic during summer, though this response is sensitive to the rate of recovery projected by the models. There is a strengthening of the Brewer–Dobson

Global premature mortality due to anthropogenic outdoor air pollution and the contribution of past climate change

Increased concentrations of ozone and fine particulate matter (PM2.5) since preindustrial times reflect increased emissions, but also contributions of past climate change. Here we use modeled concentrations from an ensemble of chemistry?climate models to estimate the global burden of anthropogenic outdoor air pollution on present-day premature human mortality, and the component of that burden attributable to past climate change. Using simulated concentrations for 2000 and 1850 and concentration?response functions (CRFs), we estimate that, at present, 470?000 (95% confidence interval, 140?000 to 900?000) premature respiratory deaths are associated globally and annually with anthropogenic ozone, and 2.1 (1.3 to 3.0) million deaths with anthropogenic PM2.5-related cardiopulmonary diseases (93%) and lung cancer (7%). These estimates are smaller than ones from previous studies because we use modeled 1850 air pollution rather than a counterfactual low concentration, and because of different emissions. Uncertainty in CRFs contributes more to overall uncertainty than the spread of model results. Mortality attributed to the effects of past climate change on air quality is considerably smaller than the global burden: 1500 (?20?000 to 27?000) deaths yr?1 due to ozone and 2200 (?350?000 to 140?000) due to PM2.5. The small multi-model means are coincidental, as there are larger ranges of results for individual models, reflected in the large uncertainties, with some models suggesting that past climate change has reduced air pollution mortality.

Separating the Dynamical Effects of Climate Change and Ozone Depletion. Part II: Southern Hemisphere Troposphere

Abstract The separate effects of ozone depleting substances (ODSs) and greenhouse gases (GHGs) on forcing circulation changes in the Southern Hemisphere extratropical troposphere are investigated using a version of the Canadian Middle Atmosphere Model (CMAM) that is coupled to an ocean. Circulation-related diagnostics include zonal wind, tropopause pressure, Hadley cell width, jet location, annular mode index, precipitation, wave drag, and eddy fluxes of momentum and heat. As expected, the tropospheric response to the ODS forcing occurs primarily in austral summer, with past (1960–99) and future (2000–99) trends of opposite sign, while the GHG forcing produces more seasonally uniform trends with the same sign in the past and future. In summer the ODS forcing dominates past trends in all diagnostics, while the two forcings contribute nearly equally but oppositely to future trends. The ODS forcing produces a past surface temperature response consisting of cooling over eastern Antarctica, and is the dominant...

Multimodel assessment of the upper troposphere and lower stratosphere: Tropics and global trends

The performance of 18 coupled Chemistry Climate Models (CCMs) in the Tropical Tropopause Layer (TTL) is evaluated using qualitative and quantitative diagnostics. Trends in tropopause quantities in the tropics and the extratropical Upper Troposphere and Lower Stratosphere (UTLS) are analyzed. A quantitative grading methodology for evaluating CCMs is extended to include variability and used to develop four different grades for tropical tropopause temperature and pressure, water vapor and ozone. Four of the 18 models and the multi‐model mean meet quantitative and qualitative standards for reproducing key processes in the TTL. Several diagnostics are performed on a subset of the models analyzing the Tropopause Inversion Layer (TIL), Lagrangian cold point and TTL transit time. Historical decreases in tropical tropopause pressure and decreases in water vapor are simulated, lending confidence to future projections. The models simulate continued decreases in tropopause pressure in the 21st century, along with ∼1K increases per century in cold point tropopause temperature and 0.5–1 ppmv per century increases in water vapor above the tropical tropopause. TTL water vapor increases below the cold point. In two models, these trends are associated with 35% increases in TTL cloud fraction. These changes indicate significant perturbations to TTL processes, specifically to deep convective heating and humidity transport. Ozone in the extratropical lowermost stratosphere has significant and hemispheric asymmetric trends. O3 is projected to increase by nearly 30% due to ozone recovery in the Southern Hemisphere (SH) and due to enhancements in the stratospheric circulation. These UTLS ozone trends may have significant effects in the TTL and the troposphere.

Review of the formulation of present‐generation stratospheric chemistry‐climate models and associated external forcings

The goal of the Chemistry-Climate Model Validation (CCMVal) activity is to improve understanding of chemistry-climate models (CCMs) through process-oriented evaluation and to provide reliable projections of stratospheric ozone and its impact on climate. An appreciation of the details of model formulations is essential for understanding how models respond to the changing external forcings of greenhouse gases and ozone-depleting substances, and hence for understanding the ozone and climate forecasts produced by the models participating in this activity. Here we introduce and review the models used for the second round (CCMVal-2) of this intercomparison, regarding the implementation of chemical, transport, radiative, and dynamical processes in these models. In particular, we review the advantages and problems associated with approaches used to model processes of relevance to stratospheric dynamics and chemistry. Furthermore, we state the definitions of the reference simulations performed, and describe the forcing data used in these simulations. We identify some developments in chemistry-climate modeling that make models more physically based or more comprehensive, including the introduction of an interactive ocean, online photolysis, troposphere-stratosphere chemistry, and non-orographic gravity-wave deposition as linked to tropospheric convection. The relatively new developments indicate that stratospheric CCM modeling is becoming more consistent with our physically based understanding of the atmosphere.

Stratosphere-troposphere coupling and annular mode variability in chemistry-climate models

The internal variability and coupling between the stratosphere and troposphere in CCMValA¢Â�Â�2 chemistryA¢Â�Â�climate models are evaluated through analysis of the annular mode patterns of variability. Computation of the annular modes in long data sets with secular trends requires refinement of the standard definition of the annular mode, and a more robust procedure that allows for slowly varying trends is established and verified. The spatial and temporal structure of the modelsA¢Â�Â� annular modes is then compared with that of reanalyses. As a whole, the models capture the key features of observed intraseasonal variability, including the sharp vertical gradients in structure between stratosphere and troposphere, the asymmetries in the seasonal cycle between the Northern and Southern hemispheres, and the coupling between the polar stratospheric vortices and tropospheric midlatitude jets. It is also found that the annular mode variability changes little in time throughout simulations of the 21st century. There are, however, both common biases and significant differences in performance in the models. In the troposphere, the annular mode in models is generally too persistent, particularly in the Southern Hemisphere summer, a bias similar to that found in CMIP3 coupled climate models. In the stratosphere, the periods of peak variance and coupling with the troposphere are delayed by about a month in both hemispheres. The relationship between increased variability of the stratosphere and increased persistence in the troposphere suggests that some tropospheric biases may be related to stratospheric biases and that a wellA¢Â�Â�simulated stratosphere can improve simulation of tropospheric intraseasonal variability.