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Observations show that mesospheric clouds (MCs) have been increasing in recent decades, presumably due to increased mesospheric water vapor which is mainly caused by greater methane (CH4) oxidation in the middle atmosphere. Past warm climates such as those of the early Cretaceous and Paleogene periods are thought to have had higher CH4 concentrations than present day, and future CH4 concentrations will also likely continue to rise. Here, idealized atmosphere chemistry‐climate model experiments forced with strong polar‐amplified sea‐surface temperatures and elevated carbon dioxide (CO2) and CH4 concentrations predict a substantial spreading of MCs to middle and low latitudes, well beyond regions where they are currently found. Sensitivity tests show that increased water vapor from CH4 oxidation and cooling from increased CO2 and CH4 concentrations create favorable conditions for cloud formation, producing MC fractions of 0.02 in the low latitudes and 0.1 in the mid‐latitudes in the Northern Hemisphere when CH4 concentration is 16× higher than pre‐industrial. Further increases in CH4 result in a monotonic increase in low‐ and mid‐latitude MCs. A uniform surface ocean warming, changes in polar amplification, or the solar constant do not significantly affect our results. While the appearance of these clouds is interesting, their ice and liquid water content is not sufficient to cause a significant radiative effect. On the other hand, dehydration of the mesosphere due to these low‐ and mid‐latitude MCs could potentially lead to a reduction in atomic hydrogen, thereby affecting mesospheric ozone concentration, although further study is required to confirm this. [ABSTRACT FROM AUTHOR]

Abstract Observations show that mesospheric clouds (MCs) have been increasing in recent decades, presumably due to increased mesospheric water vapor which is mainly caused by greater methane (CH4) oxidation in the middle atmosphere. Past warm climates such as those of the early Cretaceous and Paleogene periods are thought to have had higher CH4 concentrations than present day, and future CH4 concentrations will also likely continue to rise. Here, idealized atmosphere chemistry‐climate model experiments forced with strong polar‐amplified sea‐surface temperatures and elevated carbon dioxide (CO2) and CH4 concentrations predict a substantial spreading of MCs to middle and low latitudes, well beyond regions where they are currently found. Sensitivity tests show that increased water vapor from CH4 oxidation and cooling from increased CO2 and CH4 concentrations create favorable conditions for cloud formation, producing MC fractions of 0.02 in the low latitudes and 0.1 in the mid‐latitudes in the Northern Hemisphere when CH4 concentration is 16× higher than pre‐industrial. Further increases in CH4 result in a monotonic increase in low‐ and mid‐latitude MCs. A uniform surface ocean warming, changes in polar amplification, or the solar constant do not significantly affect our results. While the appearance of these clouds is interesting, their ice and liquid water content is not sufficient to cause a significant radiative effect. On the other hand, dehydration of the mesosphere due to these low‐ and mid‐latitude MCs could potentially lead to a reduction in atomic hydrogen, thereby affecting mesospheric ozone concentration, although further study is required to confirm this.

Increasing the horizontal resolution of an ocean model is frequently seen as a way to reduce the model biases in the North Atlantic, but we are often limited by computational resources. Here, a two‐way nested ocean model configuration (VIKING10) that consists of a high‐resolution (1/10°) component and covers the northern North Atlantic, is embedded in a 1/2° ocean grid as part of the global chemistry‐climate model, FOCI (called FOCI‐VIKING10). This configuration yields a significantly improved path of the North Atlantic current (NAC), which here reduces the North Atlantic cold bias by ∼50%. Compared with the coarse‐resolution, non‐eddying model, the improved thermal state of upper ocean layers and surface heat fluxes in a historical simulation based on FOCI‐VIKING10 are beneficial for simulating the subdecadal North Atlantic Oscillation (NAO) variability (i.e., a period of 8 years). A northward drift of the NAO‐forced ocean thermal anomalies as seen in observations and the eddying FOCI‐VIKING10, provide a lagged ocean feedback to the NAO via changes in the net surface heat flux, leading to the NAO periodicity of 8 years. This lagged feedback and the 8 years variability of the NAO cannot be captured by the non‐eddying standard FOCI historical simulation. Furthermore, the argumentative responses of the North Atlantic to the 11‐year solar cycle are re‐examined in this study. The reported solar‐induced NAO‐like responses are confirmed in the 9‐member ensemble mean based on FOCI but with low robustness among individual members. A lagged NAO‐like response is only found in the nested eddying simulation but absent from the non‐eddying reference simulation, suggesting North Atlantic biases importantly limit climate model capability to realistically solar imprints in North Atlantic climate. Plain Language Summary: A long‐standing cold bias in the North Atlantic in climate models could be reduced by increasing the horizontal resolution, but we are often limited by computational resources. Here we embedded a nest with 1/10° resolution in the ocean in the North Atlantic in a global chemistry‐climate model (called FOCI‐VIKING10). It can largely reduce the North Atlantic cold bias (roughly 50%) and correct the path of the North Atlantic current (NAC). North Atlantic Oscillation (NAO) subdecadal variability (a period of 8 years) can be simulated by FOCI‐VIKING10 when the representations of the NAO‐forced anomalies and the ocean feedback are improved by alleviating the biases. The reported NAO‐like responses to the 11‐year solar cycle are confirmed in the 9‐member ensemble mean with FOCI (non‐eddying). Although the solar signals are also found in a single member with FOCI‐VIKING10, we cannot rule out the aliasing of the internal variability in this single short member. For detecting a weak or varying signal of external forcings like the 11‐year solar cycle in this study, a large ensemble with a "coarse" resolution model is favorable over a single realization with a "presumably" better model. Key Points: North Atlantic biases are alleviated by an eddying nested ocean configuration embedded in a global climate model, FOCI‐VIKING10It is indicated that reduction of the North Atlantic biases could improve the representation of NAO sub‐decadal (8 years) variabilityFor detecting weak external imprints with limited computational resources, an ensemble with a coarse‐resolution model is favorable [ABSTRACT FROM AUTHOR]

We describe a new chemistry-climate model, Global/Regional Integrated Model system Chemistry Climate Model (GRIMs-CCM), developed by coupling the chemistry modules of the GEOS-Chem chemical transport model to the GRIMs general circulation model. The GRIMs-CCM is driven by meteorological variables simulated by the GRIMs and uses simulated gas and aerosol concentrations to calculate the radiative transfer equations at each time step. The model is evaluated by comparing ozone and aerosol concentrations with respective observations from the surface networks and the satellite datasets. It is found that the GRIMs-CCM successfully reproduces the observed spatial distributions of annual-mean aerosol optical depth and captures the seasonal and latitudinal variations of total column ozone. The evaluation of simulated aerosols in surface air against the observations reveals that the model reproduces the observed temporal and spatial variations but shows biases in soil dust aerosols. We also estimate the climatic impact of aerosols by conducting two sets of 10-year simulations for the preindustrial and present conditions. The GRIMs-CCM shows the aerosol radiative forcing of − 0.30 W m−2 from the preindustrial to present-day climates, comparable to the values from other climate model intercomparison projects. These results suggest that the GRIMs-CCM is suitable for studying chemistry-climate interactions and their changes over time. [ABSTRACT FROM AUTHOR]

The effect of the seasonal cycle on the quasi-biennial oscillation (QBO) in the equatorial stratosphere was investigated using a chemistry-climate model (CCM) by fixing the seasonal cycle in CCM simulations. The CCM realistically reproduced the QBO in wind and ozone fields of a 30-month period in a climatological simulation (control run) under annually repeating sea surface temperature (SST) with a seasonal cycle. For the control run, four experimental simulations (perpetual runs) were made by fixing solar declination and SST on the 15th of January, April, July, and October, respectively, for about 20 years. In the three perpetual runs of January, July, and October, the QBO was maintained and persisted throughout the 20-year integration in spite of some small differences in period and amplitude among the three runs. On the other hand, the QBO in the perpetual April run began to weaken after about 15 years and the downward propagation of westerly wind stopped at about 20 hPa, resulting in the QBO's ceasing. The cause of this QBO disappearance is related to the evolution of the background mean flow in the lower stratosphere, which filtered out the parameterized gravity waves propagating upwards farther. [ABSTRACT FROM AUTHOR]

Surface ozone is an important pollutant causing damage to human health and ecosystems. Here, we find that the Arctic surface ozone during the 2020–2021 winter was evidently enhanced after the sudden stratospheric warming (SSW) onset based on reanalysis data and simulations of a state-of-the-art chemistry-climate model. Further analysis suggests that this enhancement of Arctic surface ozone is primarily a result of the strengthening of the stratosphere-to-troposphere transport associated with the SSW. It is found that the SSW leads to more ozone in the Arctic stratosphere and enhanced downward transport with SSW-related downdraft. The 2021 SSW may also lead to positive anomalies in surface ozone in the northern midlatitudes, which are associated with cold air outbreaks. Our results indicate that the SSW not only affects the weather and climate in the troposphere but may also affect the surface air quality.

Hydrofluorocarbons (HFCs) have been increasingly replacing chlorofluorocarbons and hydrochlorofluorocarbons. Although their direct chemical ozone‐depleting potential is negligible, as potent greenhouse gases they modify atmospheric temperature and circulation patterns, thereby indirectly influencing stratospheric ozone recovery. Measurements and model projections must continue to evaluate HFC limitation measures and assess the long‐term impact of HFCs on the atmospheric radiation budget and stratospheric ozone. In this study, we present multi‐member ensemble simulations designed to estimate the impact of HFCs on stratospheric temperature, ozone and circulation changes at the end of the century. We compared simulations with and without HFCs for two three‐dimensional chemistry‐climate models that use the same chemistry module but different physical schemes. At low and mid‐latitudes, temperature and ozone responses were comparable for both models and in general agreement with previous studies. HFCs induced a marked temperature increase up to about 10–20 hPa and vertically alternating positive and negative ozone anomalies. We explained this pattern by competing effects of vertical motion (low and middle stratosphere) and temperature (upper stratosphere) anomalies. At northern high latitudes, there were strong discrepancies with previous studies and between the models themselves, attributed to differences in ozone anomalies caused by wave activity during winter. Quantitatively, we found a net positive, but small, HFC impact on total ozone amounts. Largest anomalies were less than 1% in the winter polar stratosphere. Our results indicate that increasing HFC amounts will likely have a limited impact on stratospheric ozone recovery within this century, with large uncertainty in the polar regions. Key Points: Unregulated hydrofluorocarbons (HFCs) have a small, global impact on total column ozone by the end of the century, as simulated by two chemistry‐climate modelsHFCs cause positive and negative O3 changes in vertical profile at low and mid‐latitudes and high‐latitude O3 changes from wave activity anomaliesStatistical significance of the changes and model consistency are mostly high for profile O3 but low for total column O3 and wave activity [ABSTRACT FROM AUTHOR]

Stratospheric water vapor variations, which may play an important role in surface climate, have drawn extensive studies. Here, the variation in stratospheric water vapor is investigated by using data from observations of the Microwave Limb Sounder (MLS) on the Aura satellite, from the ECMWF Interim Reanalysis (ERAI), and simulations by the Whole Atmosphere Community Climate Model (WACCM). We find that the differences of annual mean stratospheric water vapor among these datasets may be partly caused by the differences in vertical transports. Using budget analysis, we find that the upward transport of water vapor at 100 hPa is mainly located over the Pacific warm pool region and South America in the equatorial tropics in boreal winter and over the southeast of the South Asian high and south of North America in boreal summer. It is found that temperature averaged over regions with upward transport is a better indicator of interannual variability of tropical mean stratospheric water vapor than the tropical mean temperature. It seems that the distributions of the seasonal cycle amplitude of lower stratospheric water vapor in the tropics can also be impacted by the vertical transport. The radiative effects of the interannual changes in water vapor in the lowermost stratosphere are underestimated by approximately 29% in both ERAI and WACCM compared to MLS, although the interannual variations of water vapor in the lowermost stratosphere are dramatically overestimated in ERAI and WACCM. The results here indicate that the radiative effect of long-term changes in water vapor in the lowermost stratosphere may be underestimated in both ERAI and WACCM simulations. [ABSTRACT FROM AUTHOR]

In the extratropical atmosphere, Rossby waves (RWs) and internal gravity waves (GWs) propagating from the troposphere mediate a coupling with the middle atmosphere by influencing the dynamics therein. In state‐of‐the‐art chemistry‐climate models (CCMs), RW effects are well resolved while the majority of GW effects have to be parameterized. Here, we analyze orographic GW (OGW) interaction with resolved dynamics in a comprehensive CCM on daily time scales. For this, we apply a recently developed method of strong OGW drag event composites for three pronounced northern hemisphere OGW hotspots. We show that strong OGW drag events are associated with anomalous resolved wave propagation in the stratosphere. Causal links are inferred from previously published work and are supported by the anomalies in zonal circulation and wave activity tendencies. The nature of these anomalies varies depending on the hotspot region, which underlines the parameterized OGW‐resolved dynamics interaction being a two‐way process. Plain Language Summary: The majority of atmospheric waves are generated near the surface and propagate subsequently upward in the atmosphere. This includes Rossby waves that are resolved in climate models and small‐scale gravity waves (GWs) that commonly have to be parameterized. In the middle atmosphere, the waves eventually break, thereby dissipating their momentum and energy, which influences atmospheric dynamics. The interaction of GWs with the large‐scale circulation is to date poorly understood. In this study, we associate regionally enhanced GW drag with anomalies in resolved wave propagation in the stratosphere in a comprehensive chemistry‐climate model on the time scale of days. For this, we identify strong orographic GW (OGW) events for the three most pronounced northern hemisphere OGW hotspots and construct composites of anomalies of selected variables with respect to the climatological mean. We find that the response of the resolved wavefield strongly depends on the hotspot region, leading to diverse consequences on the large‐scale stratospheric circulation. Strong OGW events in the hotspots are in turn determined by the resolved fields from the surface to the level of OGW dissipation, which highlights the two‐way coupling between OGWs and resolved flow. Key Points: Intermittent parameterized orographic gravity wave drag affects stratospheric large‐scale dynamics in a chemistry‐climate modelDependence of the resolved dynamical response on the hotspot in question underlines the two‐way nature of the interactionUnsteady nature of the dynamical response sheds new light on how parameterized orographic gravity waves affect stratospheric transport [ABSTRACT FROM AUTHOR]

Abstract We describe the baseline model configuration and simulation characteristics of the Geophysical Fluid Dynamics Laboratory (GFDL)'s Atmosphere Model version 4.1 (AM4.1), which builds on developments at GFDL over 2013–2018 for coupled carbon‐chemistry‐climate simulation as part of the sixth phase of the Coupled Model Intercomparison Project. In contrast with GFDL's AM4.0 development effort, which focused on physical and aerosol interactions and which is used as the atmospheric component of CM4.0, AM4.1 focuses on comprehensiveness of Earth system interactions. Key features of this model include doubled horizontal resolution of the atmosphere (~200 to ~100 km) with revised dynamics and physics from GFDL's previous‐generation AM3 atmospheric chemistry‐climate model. AM4.1 features improved representation of atmospheric chemical composition, including aerosol and aerosol precursor emissions, key land‐atmosphere interactions, comprehensive land‐atmosphere‐ocean cycling of dust and iron, and interactive ocean‐atmosphere cycling of reactive nitrogen. AM4.1 provides vast improvements in fidelity over AM3, captures most of AM4.0's baseline simulations characteristics, and notably improves on AM4.0 in the representation of aerosols over the Southern Ocean, India, and China—even with its interactive chemistry representation—and in its manifestation of sudden stratospheric warmings in the coldest months. Distributions of reactive nitrogen and sulfur species, carbon monoxide, and ozone are all substantially improved over AM3. Fidelity concerns include degradation of upper atmosphere equatorial winds and of aerosols in some regions.

We describe the baseline model configuration and simulation characteristics of the Geophysical Fluid Dynamics Laboratory (GFDL)'s Atmosphere Model version 4.1 (AM4.1), which builds on developments at GFDL over 2013–2018 for coupled carbon‐chemistry‐climate simulation as part of the sixth phase of the Coupled Model Intercomparison Project. In contrast with GFDL's AM4.0 development effort, which focused on physical and aerosol interactions and which is used as the atmospheric component of CM4.0, AM4.1 focuses on comprehensiveness of Earth system interactions. Key features of this model include doubled horizontal resolution of the atmosphere (~200 to ~100 km) with revised dynamics and physics from GFDL's previous‐generation AM3 atmospheric chemistry‐climate model. AM4.1 features improved representation of atmospheric chemical composition, including aerosol and aerosol precursor emissions, key land‐atmosphere interactions, comprehensive land‐atmosphere‐ocean cycling of dust and iron, and interactive ocean‐atmosphere cycling of reactive nitrogen. AM4.1 provides vast improvements in fidelity over AM3, captures most of AM4.0's baseline simulations characteristics, and notably improves on AM4.0 in the representation of aerosols over the Southern Ocean, India, and China—even with its interactive chemistry representation—and in its manifestation of sudden stratospheric warmings in the coldest months. Distributions of reactive nitrogen and sulfur species, carbon monoxide, and ozone are all substantially improved over AM3. Fidelity concerns include degradation of upper atmosphere equatorial winds and of aerosols in some regions. Plain Language Summary: GFDL has developed a coupled chemistry‐climate Atmospheric Model (AM4.1) as part of its fourth‐generation coupled model development activities. AM4.1 includes comprehensive atmospheric chemistry for representing ozone and aerosols and has been developed for use in chemistry and air quality applications, including advanced land‐atmosphere‐ocean coupling. With fidelity near to that of AM4.0, AM4.1 features vastly improved representation of climate mean patterns and variability from previous GFDL atmospheric chemistry‐climate models. Key Points: A new atmospheric chemistry‐climate model (AM4.1) has been developed for the Geophysical Fluid Dynamics Laboratory (GFDL)'s fourth‐generation model suiteAM4.1 includes an advanced dynamical core and physical parameterizations, with enhanced vertical resolution and revised aerosol and chemistry interactionsThe AM4.1 model exhibits substantially enhanced fidelity compared to previous‐generation GFDL atmospheric models [ABSTRACT FROM AUTHOR]

Ozone loss pathways and their rates in the ozone quasi-biennial oscillation (QBO), which is simulated by a chemistry-climate model developed by the Meteorological Research Institute of Japan, are evaluated using an objective pathway analysis program (PAP). The analyzed chemical system contains catalytic cycles caused by NOx, HOx, ClOx, Ox, and BrOx. PAP quantified the rates of all significant catalytic ozone loss cycles, and evaluated the partitioning among these cycles. The QBO amplitude of the sum of all cycles amounts to about 4 and 14% of the annual mean of the total ozone loss rate at 10 and 20 hPa, respectively. The contribution of catalytic cycles to the QBO of the ozone loss rate is found to be as follows: NOx cycles contribute the largest fraction (50 - 85%) of the QBO amplitude of the total ozone loss rate; HOx cycles are the second-largest (20 - 30%) below 30 hPa and the third-largest (about 10%) above 20 hPa; Ox cycles rank third (5 - 20%) below 30 hPa and second (about 20%) above 20 hPa; ClOx cycles rank fourth (5 - 10%); and BrOx cycles are almost negligible. The relative contribution of the NOx and Ox cycles to the QBO amplitude of ozone loss differs by up to 10% and 20%, respectively, from their contribution to the annual mean ozone loss rate. The ozone QBO at 20 hPa is mainly driven by ozone transport, which then alters the ozone loss rate. In contrast, the ozone QBO at 10 hPa is driven chemically by NOx and the temperature dependence of [O]/[O3], which results from the temperature dependence of the reaction O + O2 + M O 3 + M. In addition, the ozone QBO at 10 hPa is influenced by the overhead ozone column, which affects [O]/[O3] (through ozone photolysis) and the ozone production rate (through oxygen photolysis). [ABSTRACT FROM AUTHOR]

Dry deposition (DD) is a major loss process for tropospheric ozone and some reactive nitrogen and carbon precursors. We investigate the response of summertime ozone and its production chemistry over the Southeast United States (USA) to variability in this sink. Turning off DD of oxidized nitrogen, ozone, or all species over the United States in the Geophysical Fluid Dynamics Laboratory AM3 model increases regional mean surface ozone by 5, 18, or 25 ppb, respectively. Additional sensitivity simulations demonstrate that, assuming linearity, surface ozone has a similar sensitivity to ozone DD as to NOx emissions. Trends in ozone production efficiency derived from observed relationships between ozone and precursor oxidation products may not solely reflect precursor emission changes if ozone DD varies (e.g., with meteorology). We conclude that DD variability merits consideration when interpreting observed ozone trends. Quantifying the impact of changes in sinks versus sources will require long‐term DD measurements across the region of interest. Plain Language Summary: Ozone is an air pollutant near Earth's surface and a greenhouse gas higher in the atmosphere. While many studies consider which ozone sources should be controlled to reduce air pollution, we focus here on a poorly understood removal pathway, "dry deposition" (DD), to the Earth's surface. We use a model to quantify how ozone responds to changes in the DD of ozone and related gases (oxidized nitrogen and carbon gases). We find that a 50% decrease in DD changes ozone concentrations in the Southeast United States by at least as much as recent changes in national emissions of nitrogen oxides (which form ozone in the presence of sunlight and reactive carbon gases). Our model suggests that DD variability, potentially driven by changes in meteorology or land use, could affect surface ozone trends. However, we lack the observations that would allow an assessment of how DD changes over space and time. Key Points: A 50% decrease in ozone dry deposition has twice the effect on surface ozone over the Southeast USA as a 25% increase in NOx emissionsTwo different metrics for ozone production efficiency show opposite‐signed responses to shutting off ozone dry depositionBounding the influence of ozone dry deposition on tropospheric composition requires long‐term, regional observations of its variability [ABSTRACT FROM AUTHOR]

The influence of sea-surface temperature (SST) on the lower troposphere and lower stratosphere temperature in the tropical, middle, and polar latitudes is studied for 1980–2019 based on the MERRA2, ERA5, and Met Office reanalysis data, and numerical modeling with a chemistry-climate model (CCM) of the lower and middle atmosphere. The variability of SST is analyzed according to Met Office and ERA5 data, while the variability of atmospheric temperature is investigated according to MERRA2 and ERA5 data. Analysis of sea surface temperature trends based on reanalysis data revealed that a significant positive SST trend of about 0.1 degrees per decade is observed over the globe. In the middle latitudes of the Northern Hemisphere, the trend (about 0.2 degrees per decade) is 2 times higher than the global average, and 5 times higher than in the Southern Hemisphere (about 0.04 degrees per decade). At polar latitudes, opposite SST trends are observed in the Arctic (positive) and Antarctic (negative). The impact of the El Niño Southern Oscillation phenomenon on the temperature of the lower and middle atmosphere in the middle and polar latitudes of the Northern and Southern Hemispheres is discussed. To assess the relative influence of SST, CO2, and other greenhouse gases’ variability on the temperature of the lower troposphere and lower stratosphere, numerical calculations with a CCM were performed for several scenarios of accounting for the SST and carbon dioxide variability. The results of numerical experiments with a CCM demonstrated that the influence of SST prevails in the troposphere, while for the stratosphere, an increase in the CO2 content plays the most important role.

Arctic ozone amount in winter to spring shows large year-to-year variation. This study investigates Arctic spring ozone in relation to the phase of quasi-biennial oscillation (QBO)/the 11-year solar cycle, using satellite observations, reanalysis data, and outputs of a chemistry climate model (CCM) during the period of 1979–2017. For this duration, we found that the composite mean of the Northern Hemisphere high-latitude total ozone in the QBO-westerly (QBO-W)/solar minimum (Smin) phase is slightly smaller than those averaged for the QBO-W/Smax and QBO-E/Smax years in March. An analysis of a passive ozone tracer in the CCM simulation indicates that this negative anomaly is primarily caused by transport. The negative anomaly is consistent with a weakening of the residual mean downward motion in the polar lower stratosphere. The contribution of chemical processes estimated using the column amount difference between ozone and the passive ozone tracer is between 10–20% of the total anomaly in March. The lower ozone levels in the Arctic spring during the QBO-W/Smin years are associated with a stronger Arctic polar vortex from late winter to early spring, which is linked to the reduced occurrence of sudden stratospheric warming in the winter during the QBO-W/Smin years.

With the gradual yet unequivocal phasing out of ozone depleting substances (ODSs), the environmental crisis caused by the discovery of an ozone hole over the Antarctic has lessened in severity and a promising recovery of the ozone layer is predicted in this century. However, strong volcanic activity can also cause ozone depletion that might be severe enough to threaten the existence of life on Earth. In this study, a transport model and a coupled chemistry-climate model were used to simulate the impacts of super volcanoes on ozone depletion. The volcanic eruptions in the experiments were the 1991 Mount Pinatubo eruption and a 100 × Pinatubo size eruption. The results show that the percentage of global mean total column ozone depletion in the 2050 RCP8.5 100 × Pinatubo scenario is approximately 6% compared to two years before the eruption and 6.4% in tropics. An identical simulation, 100 × Pinatubo eruption only with natural source ODSs, produces an ozone depletion of 2.5% compared to two years before the eruption, and with 4.4% loss in the tropics. Based on the model results, the reduced ODSs and stratospheric cooling lighten the ozone depletion after super volcanic eruption. [ABSTRACT FROM AUTHOR]

The Whole Atmosphere Community Climate Model (WACCM) is used to investigate the relative importance of CO emissions, chemical and dynamical processes on temporal variations of CO in the tropical upper troposphere (UT) and the lower stratosphere (LS). The semi-annual oscillation (SAO) in the tropical UT and the annual oscillation (AO) in the tropical LS detected in the MLS CO observations can be well captured by the model. The model simulations reveal that the CO surface emissions explain most of the SAO signals in the tropical UT, with the remainder being attributed to dynamical and chemical processes. The CO AO in the LS primarily results from combined effects of dynamical and chemical processes while the dynamical and chemical processes make opposite contributions to the CO AO signals, consistent with the previous findings. Our analysis further reveals that CO surface emissions tend to weaken the amplitude of the CO annual cycle in the tropical LS, while the annual variations in the meridional component of the Brewer–Dobson (BD) circulation can amplify the annual variations of CO above 30 hPa. The model simulations also indicate that the CO annual cycle in the LS has a mixed behaviour with the annual variations of tropical upwelling reflected in CO between ~70 and ~50 hPa and a standard tape-recorder signal above 50 hPa. Moreover, the AO signals of CO exist up to 10 hPa when the chemical processes are switched off. The temporal and spatial variations of CO in the UT and near the tropopause are mainly driven by the upward transport of CO by tropical deep convection and the Asian summer monsoon circulation. In the early stage of the South Asian summer monsoon over the Bay of Bengal and the South China in the late spring and early summer, the transport of the CO surface emissions over Southeast Asia by the South Asian summer monsoon leads to an increase in the tropical CO, but the horizontal transport from the extratropics into the tropics (termed in-mixing) driven by the Asian summer monsoon anticyclone in the boreal summer decreases the tropical CO.

Simulated stratospheric temperatures over the period 1979–2016 in models from the Chemistry‐Climate Model Initiative are compared with recently updated and extended satellite data sets. The multimodel mean global temperature trends over 1979–2005 are −0.88 ± 0.23, −0.70 ± 0.16, and −0.50 ± 0.12 K/decade for the Stratospheric Sounding Unit (SSU) channels 3 (~40–50 km), 2 (~35–45 km), and 1 (~25–35 km), respectively (with 95% confidence intervals). These are within the uncertainty bounds of the observed temperature trends from two reprocessed SSU data sets. In the lower stratosphere, the multimodel mean trend in global temperature for the Microwave Sounding Unit channel 4 (~13–22 km) is −0.25 ± 0.12 K/decade over 1979–2005, consistent with observed estimates from three versions of this satellite record. The models and an extended satellite data set comprised of SSU with the Advanced Microwave Sounding Unit‐A show weaker global stratospheric cooling over 1998–2016 compared to the period of intensive ozone depletion (1979–1997). This is due to the reduction in ozone‐induced cooling from the slowdown of ozone trends and the onset of ozone recovery since the late 1990s. In summary, the results show much better consistency between simulated and satellite‐observed stratospheric temperature trends than was reported by Thompson et al. (2012, https://doi.org/10.1038/nature11579) for the previous versions of the SSU record and chemistry‐climate models. The improved agreement mainly comes from updates to the satellite records; the range of stratospheric temperature trends over 1979–2005 simulated in Chemistry‐Climate Model Initiative models is comparable to the previous generation of chemistry‐climate models. Plain Language Summary: A previous analysis by Thompson et al. (2012, https://doi.org/10.1038/nature11579) showed substantial differences between satellite‐observed and model‐simulated stratospheric cooling trends since the late 1970s. Here we compare recently revised and extended satellite temperature records with new simulations from 14 chemistry‐climate models. The results show much better agreement in the magnitude of stratospheric cooling over 1979–2005 between models and observations. This cooling was predominantly driven by increasing greenhouse gases and declining stratospheric ozone levels. An extended satellite temperature record and the chemistry‐climate models show weaker global stratospheric cooling over 1998–2016 compared to 1979–1997. This is due to the reduction in ozone‐induced cooling from the slowdown of ozone trends and the onset of ozone recovery since the late 1990s. There are larger differences in the latitudinal structure of past stratospheric temperature trends due to the effects of unforced atmospheric variability. In summary, the results show much better consistency between simulated and satellite‐observed stratospheric temperature trends than was reported by Thompson et al. (2012, https://doi.org/10.1038/nature11579) for the previous versions of the satellite record and last generation of chemistry‐climate models. The improved agreement mainly comes from updates to the satellite records, while the range of simulated trends is comparable to the previous generation of models. Key Points: There is substantial improvement in the comparison between modeled and observed stratospheric temperature trends over the satellite eraObservations and models show weaker stratospheric cooling since ~1998 when ozone‐depleting substances have been declining in the atmosphereLarger differences exist between modeled and observed stratospheric temperature trends at high latitudes partly due to internal variability [ABSTRACT FROM AUTHOR]

The atmospheric methane growth rate has fluctuated over the past three decades, signifying variations in methane sources and sinks. Methane isotopic ratios ( δ 13 CH 4 ) differ between emission categories, and can therefore be used to distinguish which methane sources have changed. However, isotopic modelling studies have mainly focused on uncertainties in methane emissions rather than uncertainties in isotopic source signatures. We simulated atmospheric δ 13 CH 4 for the period 1990–2010 using the global chemistry-climate model SOCOL. Empirically-derived regional variability in the isotopic signatures was introduced in a suite of sensitivity simulations. These simulations were compared to a baseline simulation with commonly used global mean isotopic signatures. We investigated coal, natural gas/oil, wetland, livestock, and biomass burning source signatures to determine whether regional variations impact the observed isotopic trend and spatial distribution. Based on recently published source signature datasets, our calculated global mean isotopic signatures are in general lighter than the commonly used values. Trends in several isotopic signatures were also apparent during the period 1990–2010. Tropical livestock emissions grew during the 2000s, introducing isotopically heavier livestock emissions since tropical livestock consume more C 4 vegetation than midlatitude livestock. Chinese coal emissions, which are isotopically heavy compared to other coals, increase during the 2000s leading to higher global values of δ 13 CH 4 for coal emissions. EDGAR v4.2 emissions disagree with the observed atmospheric isotopic trend for almost all simulations, confirming past doubts about this emissions inventory. The agreement between the modelled and observed δ 13 CH 4 interhemispheric differences improves when regional source signatures are used. Even though the simulated results are highly dependent on the choice of methane emission inventories, they emphasize that the commonly used global mean signatures are inadequate. Regional isotopic signatures should be employed in modelling studies that try to constrain methane emission inventories. [ABSTRACT FROM AUTHOR]

As countries take action to mitigate global warming, both by ratifying the UNFCCC Paris Agreement and enacting the Kigali Amendment to the Montreal Protocol to manage hydrofluorocarbons (HFCs), it is important to consider the relative importance of the pertinent greenhouse gases and the distinct structure of their atmospheric impacts, and how the timing of potential greenhouse gas regulations would affect future changes in atmospheric temperature and ozone. HFCs should be explicitly considered in upcoming climate and ozone assessments, since chemistry-climate model simulations demonstrate that HFCs could contribute substantially to anthropogenic climate change by the mid-21st century, particularly in the upper troposphere and lower stratosphere i.e., global average warming up to 0.19 K at 80 hPa. The HFC mitigation scenarios described in this study demonstrate the benefits of taking early action in avoiding future atmospheric change: more than 90% of the climate change impacts of HFCs can be avoided if emissions stop by 2030.

Using a detailed, fully coupled chemistry climate model (CCM), the effect of increasing stratospheric H2O on ozone and temperature is investigated. Different CCM time-slice runs have been performed to investigate the chemical and radiative impacts of an assumed 2 ppmv increase in H2O. The chemical effects of this H2O increase lead to an overall decrease of the total column ozone (TCO) by ∼1% in the tropics and by a maximum of 12% at southern high latitudes. At northern high latitudes, the TCO is increased by only up to 5% due to stronger transport in the Arctic. A 2-ppmv H2O increase in the model’s radiation scheme causes a cooling of the tropical stratosphere of no more than 2 K, but a cooling of more than 4 K at high latitudes. Consequently, the TCO is increased by about 2%–6%. Increasing stratospheric H2O, therefore, cools the stratosphere both directly and indirectly, except in the polar regions where the temperature responds differently due to feedbacks between ozone and H2O changes. The combined chemical and radiative effects of increasing H2O may give rise to more cooling in the tropics and middle latitudes but less cooling in the polar stratosphere. The combined effects of H2O increases on ozone tend to offset each other, except in the Arctic stratosphere where both the radiative and chemical impacts give rise to increased ozone. The chemical and radiative effects of increasing H2O cause dynamical responses in the stratosphere with an evident hemispheric asymmetry. In terms of ozone recovery, increasing the stratospheric H2O is likely to accelerate the recovery in the northern high latitudes and delay it in the southern high latitudes. The modeled ozone recovery is more significant between 2000–2050 than between 2050–2100, driven mainly by the larger relative change in chlorine in the earlier period. [ABSTRACT FROM AUTHOR]

Abstract: The simulated micrometerology by a single-column chemistry-climate model (SCM) has been evaluated by comparison with BEWA2000 field campaign measurements over a coniferous forest, July–August 2001. This comparison indicates the limitations in the representation of the SCM''s micrometeorological parameters that control atmosphere–biosphere peroxide exchanges. The evaluation of the micrometeorology also indicates that the validity of the so-called nudging technique to force climate models such as the SCM to the observed meteorology is sensitive to the applied timestep. For the typical timestep used in global scale climate models, numerical instabilities in the calculation of surface exchanges occur due to a misrepresentation of the surface–atmosphere temperature gradient. However, using a 1-min timestep shows good agreement between the simulated and observed meteorology of a wet and cold period during the campaign whereas the model underestimates daytime and nocturnal turbulent exchanges during a following warm and dry period. [Copyright &y& Elsevier]

The El Niño-Southern Oscillation (ENSO), a dominant driver of interannual climate variations around the world, is characterized in the central-to-eastern tropical Pacific by anomalous sea-surface warming during the El Niño phase and cooling during the La Niña phase. Although ENSO strongly affects atmospheric circulation in East Asia, its effects on tropospheric ozone there have not been fully explored. Here we use satellite measurements of tropospheric column ozone and chemistry-climate model simulations to assess the effects of atmospheric circulations driven by ENSO on tropospheric column ozone levels in East Asia. We find that the observed ozone tends to increase in the East Asian troposphere 4 months after the La Niña peak, corresponding to anomalous northerly downward motions and suppressed convection. The circulation changes can be attributed to anomalous cyclonic flows in the western North Pacific, which links the La Niña and East Asian climate by modulating meridional transport of water vapor. These post-La Niña changes are also evident in the chemistry-climate model results, albeit with a slightly longer (5-month) lag. The model also reveals that La Niña-related ozone enhancement in East Asia is largely due to the intensified southward transport of ozone-rich air from higher latitudes. This suggests that ENSO should be considered to estimate the ozone concentration in East Asia, requiring much attention of ENSO properties in a changing climate. • A new link between ENSO and tropospheric ozone in East Asia is presented using satellite data and a chemistry-climate model. • Tropospheric column ozone tends to increase over East Asia 4–5 months after the La Niña peak. • This post-La Niña enhancement of tropospheric ozone can be attributed to anomalous ozone transport from higher latitudes. [ABSTRACT FROM AUTHOR]

Ozone feedback effects on the quasi-biennial oscillation (QBO) were investigated with a chemistry–climate model (CCM) by modifying ozone abundance in the radiative process. Under a standard run for 50 years, the CCM could realistically reproduce the QBO of about a 28-month period for wind and ozone. Five experiment runs were made for 20 years through varying ozone abundance only in the equatorial stratosphere from 100 to 10 hPa by −40, −20, −10, +10, and +20%, respectively, after the chemistry module and transferring the resultant ozone to the radiation calculation. It was found that the modification of ozone abundance in the radiation substantially changed the period of the QBO but slightly influenced the amplitude of the QBO. The 10% and 20% increase runs led to longer QBO periods (31 and 34 months) than that of the standard run, i.e., lengthening by 3 and 6 months, while the 10%, 20%, and 40% decrease runs resulted in shorter periods (24, 22, and 17 months), i.e., shortening by 4, 6, and 11 months. These substantial changes in the QBO period in the experiment runs indicate that the ozone feedback significantly affects the QBO dynamics through the modulation in solar heating. [ABSTRACT FROM AUTHOR]

Arctic ozone amount in winter to spring shows large year-to-year variation. This study investigates Arctic spring ozone in relation to the phase of quasi-biennial oscillation (QBO)/the 11-year solar cycle, using satellite observations, reanalysis data, and outputs of a chemistry climate model (CCM) during the period of 1979–2017. For this duration, we found that the composite mean of the Northern Hemisphere high-latitude total ozone in the QBO-westerly (QBO-W)/solar minimum (Smin) phase is slightly smaller than those averaged for the QBO-W/Smax and QBO-E/Smax years in March. An analysis of a passive ozone tracer in the CCM simulation indicates that this negative anomaly is primarily caused by transport. The negative anomaly is consistent with a weakening of the residual mean downward motion in the polar lower stratosphere. The contribution of chemical processes estimated using the column amount difference between ozone and the passive ozone tracer is between 10–20% of the total anomaly in March. The lower ozone levels in the Arctic spring during the QBO-W/Smin years are associated with a stronger Arctic polar vortex from late winter to early spring, which is linked to the reduced occurrence of sudden stratospheric warming in the winter during the QBO-W/Smin years. [ABSTRACT FROM AUTHOR]

The influence of sea-surface temperature (SST) on the lower troposphere and lower stratosphere temperature in the tropical, middle, and polar latitudes is studied for 1980–2019 based on the MERRA2, ERA5, and Met Office reanalysis data, and numerical modeling with a chemistry-climate model (CCM) of the lower and middle atmosphere. The variability of SST is analyzed according to Met Office and ERA5 data, while the variability of atmospheric temperature is investigated according to MERRA2 and ERA5 data. Analysis of sea surface temperature trends based on reanalysis data revealed that a significant positive SST trend of about 0.1 degrees per decade is observed over the globe. In the middle latitudes of the Northern Hemisphere, the trend (about 0.2 degrees per decade) is 2 times higher than the global average, and 5 times higher than in the Southern Hemisphere (about 0.04 degrees per decade). At polar latitudes, opposite SST trends are observed in the Arctic (positive) and Antarctic (negative). The impact of the El Niño Southern Oscillation phenomenon on the temperature of the lower and middle atmosphere in the middle and polar latitudes of the Northern and Southern Hemispheres is discussed. To assess the relative influence of SST, CO2, and other greenhouse gases' variability on the temperature of the lower troposphere and lower stratosphere, numerical calculations with a CCM were performed for several scenarios of accounting for the SST and carbon dioxide variability. The results of numerical experiments with a CCM demonstrated that the influence of SST prevails in the troposphere, while for the stratosphere, an increase in the CO2 content plays the most important role. [ABSTRACT FROM AUTHOR]