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The NCAR Community Earth System Model (CESM) now includes an atmospheric component that extends in altitude to the lower thermosphere. This atmospheric model, known as the Whole Atmosphere Community Climate Model (WACCM), includes fully interactive chemistry, allowing, for example, a self-consistent representation of the development and recovery of the stratospheric ozone hole and its effect on the troposphere. This paper focuses on analysis of an ensemble of transient simulations using CESM1(WACCM), covering the period from the preindustrial era to present day, conducted as part of phase 5 of the Coupled Model Intercomparison Project. Variability in the stratosphere, such as that associated with stratospheric sudden warmings and the development of the ozone hole, is in good agreement with observations. The signals of these phenomena propagate into the troposphere, influencing near-surface winds, precipitation rates, and the extent of sea ice. In comparison of tropospheric climate change predictions with those from a version of CESM that does not fully resolve the stratosphere, the global-mean temperature trends are indistinguishable. However, systematic differences do exist in other climate variables, particularly in the extratropics. The magnitude of the difference can be as large as the climate change response itself. This indicates that the representation of stratosphere–troposphere coupling could be a major source of uncertainty in climate change projections in CESM.

The current standard version of the Whole Atmosphere Community Climate Model (WACCM) simulates Southern Hemisphere winter and spring temperatures that are too cold compared with observations. This “cold-pole bias” leads to unrealistically low ozone column amounts in Antarctic spring. Here, the cold-pole problem is addressed by introducing additional mechanical forcing of the circulation via parameterized gravity waves. Insofar as observational guidance is ambiguous regarding the gravity waves that might be important in the Southern Hemisphere stratosphere, the impact of increasing the forcing by orographic gravity waves was investigated. This reduces the strength of the Antarctic polar vortex in WACCM, bringing it into closer agreement with observations, and accelerates the Brewer–Dobson circulation in the polar stratosphere, which warms the polar cap and improves substantially the simulation of Antarctic temperature. These improvements are achieved without degrading the performance of the model in the Northern Hemisphere stratosphere or in the mesosphere and lower thermosphere of either hemisphere. It is shown, finally, that other approaches that enhance gravity wave forcing can also reduce the cold-pole bias such that careful examination of observational evidence and model performance will be required to establish which gravity wave sources are dominant in the real atmosphere. This is especially important because a “downward control” analysis of these results suggests that the improvement of the cold-pole bias itself is not very sensitive to the details of how gravity wave drag is altered.

The distribution of gases such as ozone and water vapour in the stratosphere—which affect surface climate—is influenced by the meridional overturning of mass in the stratosphere, the Brewer–Dobson circulation. However, observation-based estimates of the global strength of this circulation are difficult to obtain. Here we present two calculations of the mean strength of the meridional overturning of the stratosphere. We analyse satellite data that document the global diabatic circulation between 2007–2011, and compare these to three reanalysis data sets and to simulations with a state-of-the-art chemistry–climate model. Using measurements of sulfur hexafluoride (SF 6 ) and nitrous oxide, we calculate the global mean diabatic overturning mass flux throughout the stratosphere. In the lower stratosphere, these two estimates agree, and at a potential temperature level of 460 K (about 20 km or 60 hPa in tropics) the global circulation strength is 6.3–7.6 × 10 9  kg s −1 . Higher in the atmosphere, only the SF 6 -based estimate is available, and it diverges from the reanalysis data and simulations. Interpretation of the SF 6 -data-based estimate is limited because of a mesospheric sink of SF 6 ; however, the reanalyses also differ substantially from each other. We conclude that the uncertainty in the mean meridional overturning circulation strength at upper levels of the stratosphere amounts to at least 100%. The strength of the global meridional overturning circulation in the stratosphere is uncertain. An analysis of satellite data, reanalyses and model simulations reveals a strength of 6.3–7.6 × 10 9  kg s −1 , but no convergence at higher altitudes.

Observational evidence shows the ubiquitous presence of ocean-emitted short-lived halogens in the global atmosphere1,2,3. Natural emissions of these chemical compounds have been anthropogenically amplified since pre-industrial times4,5,6, while, in addition, anthropogenic short-lived halocarbons are currently being emitted to the atmosphere7,8. Despite their widespread distribution in the atmosphere, the combined impact of these species on Earth’s radiative balance remains unknown. Here we show that short-lived halogens exert a substantial indirect cooling effect at present (−0.13 ± 0.03 watts per square metre) that arises from halogen-mediated radiative perturbations of ozone (−0.24 ± 0.02 watts per square metre), compensated by those from methane (+0.09 ± 0.01 watts per square metre), aerosols (+0.03 ± 0.01 watts per square metre) and stratospheric water vapour (+0.011 ± 0.001 watts per square metre). Importantly, this substantial cooling effect has increased since 1750 by −0.05 ± 0.03 watts per square metre (61 per cent), driven by the anthropogenic amplification of natural halogen emissions, and is projected to change further (18–31 per cent by 2100) depending on climate warming projections and socioeconomic development. We conclude that the indirect radiative effect due to short-lived halogens should now be incorporated into climate models to provide a more realistic natural baseline of Earth’s climate system.

CH 4 is the most abundant reactive greenhouse gas and a complete understanding of its atmospheric fate is needed to formulate mitigation policies. Current chemistry-climate models tend to underestimate the lifetime of CH 4 , suggesting uncertainties in its sources and sinks. Reactive halogens substantially perturb the budget of tropospheric OH, the main CH 4 loss. However, such an effect of atmospheric halogens is not considered in existing climate projections of CH 4 burden and radiative forcing. Here, we demonstrate that reactive halogen chemistry increases the global CH 4 lifetime by 6–9% during the 21st century. This effect arises from significant halogen-mediated decrease, mainly by iodine and bromine, in OH-driven CH 4 loss that surpasses the direct Cl-induced CH 4 sink. This increase in CH 4 lifetime helps to reduce the gap between models and observations and results in a greater burden and radiative forcing during this century. The increase in CH 4 burden due to halogens (up to 700 Tg or 8% by 2100) is equivalent to the observed atmospheric CH 4 growth during the last three to four decades. Notably, the halogen-driven enhancement in CH 4 radiative forcing is 0.05 W/m 2 at present and is projected to increase in the future (0.06 W/m 2 by 2100); such enhancement equals ~10% of present-day CH 4 radiative forcing and one-third of N 2 O radiative forcing, the third-largest well-mixed greenhouse gas. Both direct (Cl-driven) and indirect (via OH) impacts of halogens should be included in future CH 4 projections. Methane is a powerful greenhouse gas and previous studies focus on its sources with less attention on the loss. Here the authors show that reactive halogen species, not considered in climate projections, significantly reduces the methane loss, increasing its lifetime, burden, and radiative forcing.

Anthropogenic mercury (Hg(0)) emissions oxidize to gaseous Hg(II) compounds, before deposition to Earth surface ecosystems. Atmospheric reduction of Hg(II) competes with deposition, thereby modifying the magnitude and pattern of Hg deposition. Global Hg models have postulated that Hg(II) reduction in the atmosphere occurs through aqueous-phase photoreduction that may take place in clouds. Here we report that experimental rainfall Hg(II) photoreduction rates are much slower than modelled rates. We compute absorption cross sections of Hg(II) compounds and show that fast gas-phase Hg(II) photolysis can dominate atmospheric mercury reduction and lead to a substantial increase in the modelled, global atmospheric Hg lifetime by a factor two. Models with Hg(II) photolysis show enhanced Hg(0) deposition to land, which may prolong recovery of aquatic ecosystems long after Hg emissions are lowered, due to the longer residence time of Hg in soils compared with the ocean. Fast Hg(II) photolysis substantially changes atmospheric Hg dynamics and requires further assessment at regional and local scales. Reduction of gaseous Hg(II) compounds drives atmospheric mercury wet and dry deposition to Earth surface ecosystems. Global Hg models assume this reduction takes place in clouds. Here the authors report a new gas-phase Hg photochemical mechanism that changes atmospheric mercury lifetime and its deposition to the surface.

Atmospheric methane is both a potent greenhouse gas and photochemically active, with approximately equal anthropogenic and natural sources. The addition of chlorine to the atmosphere has been proposed to mitigate global warming through methane reduction by increasing its chemical loss. However, the potential environmental impacts of such climate mitigation remain unexplored. Here, sensitivity studies are conducted to evaluate the possible effects of increasing reactive chlorine emissions on the methane budget, atmospheric composition and radiative forcing. Because of non-linear chemistry, in order to achieve a reduction in methane burden (instead of an increase), the chlorine atom burden needs to be a minimum of three times the estimated present-day burden. If the methane removal target is set to 20%, 45%, or 70% less global methane by 2050 compared to the levels in the Representative Concentration Pathway 8.5 scenario (RCP8.5), our modeling results suggest that additional chlorine fluxes of 630, 1250, and 1880 Tg Cl/year, respectively, are needed. The results show that increasing chlorine emissions also induces significant changes in other important climate forcers. Remarkably, the tropospheric ozone decrease is large enough that the magnitude of radiative forcing decrease is similar to that of methane. Adding 630, 1250, and 1880 Tg Cl/year to the RCP8.5 scenario, chosen to have the most consistent current-day trends of methane, will decrease the surface temperature by 0.2, 0.4, and 0.6 °C by 2050, respectively. The quantity and method in which the chlorine is added, its interactions with climate pathways, and the potential environmental impacts on air quality and ocean acidity, must be carefully considered before any action is taken. Methane, a powerful greenhouse gas, has comparable anthropogenic and natural sources, complicating emission control. Increasing reactive chlorine has been proposed for mitigation. This study assesses the global environmental impacts of such proposal.

We have analyzed near-global stratospheric data (and mesospheric data as well for H2O) in terms of absolute abundances, variability, and trends for O3, H2O, HCl, N2O, and HNO3, based on Aura Microwave Limb Sounder (MLS) data, as well as longer-term series from the Global OZone Chemistry And Related trace gas Data records for the Stratosphere (GOZCARDS). While we emphasize the evaluation of stratospheric models via data comparisons through 2014 to free-running (FR-WACCM) and specified dynamics (SD-WACCM) versions of the Community Earth System Model version 1 (CESM1) Whole Atmosphere Community Climate Model (WACCM), we also highlight observed stratospheric changes, using the most recent data from MLS. Regarding highlights from the satellite data, we have used multiple linear regression to derive trends based on zonal mean time series from Aura MLS data alone, between 60∘ S and 60∘ N. In the upper stratosphere, MLS O3 shows increases over 2005–2018 at ∼0.1–0.3 % yr−1 (depending on altitude and latitude) with 2σ errors of ∼0.2 % yr−1. For the lower stratosphere (LS), GOZCARDS O3 data for 1998–2014 point to small decreases between 60∘ S and 60∘ N, but the trends are more positive if the starting year is 2005. Southern midlatitudes (30–60∘ S) exhibit near-zero or slightly positive LS trends for 1998–2018. The LS O3 trends based on 2005–2018 MLS data are most positive (0.1–0.2 % yr−1) at these southern midlatitudes, although marginally statistically significant, in contrast to slightly negative or near-zero trends for 2005–2014. Given the high variability in LS O3, and the high sensitivity of trends to the choice of years used, especially for short periods, further studies are required for a robust longer-term LS trend result. For H2O, upper-stratospheric and mesospheric trends from GOZCARDS 1992–2010 data are near zero (within ∼0.2 % yr−1) and significantly smaller than trends (within ∼0.4–0.7 % yr−1) from MLS for 2005–2014 or 2005–2018. The latter short-term positive H2O trends are larger than expected from changes resulting from long-term increases in methane. We note that the very shallow solar flux maximum of solar cycle 24 has contributed to fairly large short-term mesospheric and upper-stratospheric H2O trends since 2005. However, given known drifts in the MLS H2O time series, MLS H2O trend results, especially after 2010, should be viewed as upper limits. The MLS data also show regions and periods of small HCl increases in the lower stratosphere, within the context of the longer-term stratospheric decrease in HCl, as well as interhemispheric–latitudinal differences in short-term HCl tendencies. We observe similarities in such short-term tendencies, and interhemispheric asymmetries therein, for lower-stratospheric HCl and HNO3, while N2O trend profiles exhibit anti-correlated patterns. In terms of the model evaluation, climatological averages for 2005–2014 from both FR-WACCM and SD-WACCM for O3, H2O, HCl, N2O, and HNO3 compare favorably with Aura MLS data averages over this period. However, the models at mid- to high latitudes overestimate mean MLS LS O3 values and seasonal amplitudes by as much as 50 %–60 %; such differences appear to implicate, in part, a transport-related model issue. At lower-stratospheric high southern latitudes, variations in polar winter and spring composition observed by MLS are well matched by SD-WACCM, with the main exception being for the early winter rate of decrease in HCl, which is too slow in the model. In general, we find that the latitude–pressure distributions of annual and semiannual oscillation amplitudes derived from MLS data are properly captured by the model amplitudes. In terms of closeness of fit diagnostics for model–data anomaly series, not surprisingly, SD-WACCM (driven by realistic dynamics) generally matches the observations better than FR-WACCM does. We also use root mean square variability as a more valuable metric to evaluate model–data differences. We find, most notably, that FR-WACCM underestimates observed interannual variability for H2O; this has implications for the time period needed to detect small trends, based on model predictions. The WACCM O3 trends generally agree (within 2σ uncertainties) with the MLS data trends, although LS trends are typically not statistically different from zero. The MLS O3 trend dependence on latitude and pressure is matched quite well by the SD-WACCM results. For H2O, MLS and SD-WACCM positive trends agree fairly well, but FR-WACCM shows significantly smaller increases; this discrepancy for FR-WACCM is even more pronounced for longer-term GOZCARDS H2O records. The larger discrepancies for FR-WACCM likely arise from its poorer correlations with cold point temperatures and with quasi-biennial oscillation (QBO) variability. For HCl, while some expected decreases in the global LS are seen in the observations, there are interhemispheric differences in the trends, and increasing tendencies are suggested in tropical MLS data at 68 hPa, where there is only a slight positive trend in SD-WACCM. Although the vertical gradients in MLS HCl trends are well duplicated by SD-WACCM, the model trends are always somewhat more negative; this deserves further investigation. The original MLS N2O product time series yield small positive LS tropical trends (2005–2012), consistent with models and with rates of increase in tropospheric N2O. However, longer-term series from the more current MLS N2O standard product are affected by instrument-related drifts that have also impacted MLS H2O. The LS short-term trend profiles from MLS N2O and HNO3 at midlatitudes in the two hemispheres have different signs; these patterns are well matched by SD-WACCM trends for these species. These model–data comparisons provide a reminder that the QBO and other dynamical factors affect decadal variability in a major way, notably in the lower stratosphere, and can thus significantly hinder the goals of robustly extracting (and explaining) small underlying long-term trends. The data sets and tools discussed here for model evaluation could be expanded to comparisons of species or regions not included here, as well as to comparisons between a variety of chemistry–climate models.

Reactive atmospheric halogens destroy tropospheric ozone (O3), an air pollutant and greenhouse gas. The primary source of natural halogens is emissions from marine phytoplankton and algae, as well as abiotic sources from ocean and tropospheric chemistry, but how their fluxes will change under climate warming, and the resulting impacts on O3, are not well known. Here, we use an Earth system model to estimate that natural halogens deplete approximately 13% of tropospheric O3 in the present-day climate. Despite increased levels of natural halogens through the twenty-first century, this fraction remains stable due to compensation from hemispheric, regional and vertical heterogeneity in tropospheric O3 loss. Notably, this halogen-driven O3 buffering is projected to be greatest over polluted and populated regions, due mainly to iodine chemistry, with important implications for air quality.An Earth system model estimates that natural halogens, of marine biotic and abiotic origin, remove about 13% of present-day global tropospheric O3. Projections suggest this ratio is stable through 2100, with high spatial heterogeneity, despite increasing natural halogens.

One of the key questions in the air quality and climate sciences is how tropospheric ozone concentrations will change in the future. This will depend on two factors: changes in stratosphere-to-troposphere transport (STT) and changes in tropospheric chemistry. Here we aim to identify robust changes in STT using simulations from the Chemistry Climate Model Initiative (CCMI) under a common climate change scenario (RCP6.0). We use two idealized stratospheric tracers to isolate changes in transport: stratospheric ozone (O3S), which is exactly like ozone but has no chemical sources in the troposphere, and st80, a passive tracer with fixed volume mixing ratio in the stratosphere. We find a robust increase in the tropospheric columns of these two tracers across the models. In particular, stratospheric ozone in the troposphere is projected to increase 10 %–16 % by the end of the 21st century in the RCP6.0 scenario. Future STT is enhanced in the subtropics due to the strengthening of the shallow branch of the Brewer–Dobson circulation (BDC) in the lower stratosphere and of the upper part of the Hadley cell in the upper troposphere. The acceleration of the deep branch of the BDC in the Northern Hemisphere (NH) and changes in eddy transport contribute to increased STT at high latitudes. These STT trends are caused by greenhouse gas (GHG) increases, while phasing out of ozone-depleting substances (ODS) does not lead to robust transport changes. Nevertheless, the decline of ODS increases the reservoir of ozone in the lower stratosphere, which results in enhanced STT of O3S at middle and high latitudes. A higher emission scenario (RCP8.5) produces stronger STT trends, with increases in tropospheric column O3S more than 3 times larger than those in the RCP6.0 scenario by the end of the 21st century.