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Chemistry Climate Models (CCMs) are essential tools for characterizing and predicting the role of atmospheric composition and chemistry in Earth's climate system. This study demonstrates the use of airborne in situ observations to diagnose the representation of chemical composition and transport by CCMs. Process-based diagnostics using dynamical and chemical coordinates are presented which minimize the spatial and temporal sampling differences between airborne in situ measurements and CCM grid points. The chosen process is the chemical impact of the Asian summer monsoon (ASM), where deep convection serves as a rapid transport pathway for surface emissions to reach the upper troposphere and lower stratosphere (UTLS). We examine two CCM configurations for their representation of the ASM UTLS using a set of airborne observations from south Asia. The diagnostics reveal good model performance at representing tropospheric tracer distribution throughout the troposphere and lower stratosphere, and excellent representation of chemical aging in the lower stratosphere when chemical loss is dominated by photolysis. Identified model limitations include the use of zonally averaged mole fraction boundary conditions for species with sufficiently short tropospheric lifetimes, which may obscure enhanced regional emissions sources. Overall, the diagnostics underscore the skill of current-generation models at representing pollution transport from the boundary layer to the stratosphere via the ASM mechanism, and demonstrate the strength of airborne in situ observations toward characterizing this representation.

Chlorinated very short-lived substances (Cl-VSLS) are ubiquitous in the troposphere and can contribute to the stratospheric chlorine budget. In this study, we present measurements of atmospheric dichloromethane (CH2Cl2), tetrachloroethene (C2Cl4), chloroform (CHCl3), and 1,2-dichloroethane (1,2-DCA) obtained during the National Aeronautics and Space Administration (NASA) Atmospheric Tomography (ATom) global-scale aircraft mission (2016?2018), and use the Community Earth System Model (CESM) updated with recent chlorine chemistry to further investigate their global tropospheric distribution. The measured global average Cl-VSLS mixing ratios, from 0.2 to 13 km altitude, were 46.6 ppt (CH2Cl2), 9.6 ppt (CHCl3), 7.8 ppt (1,2-DCA), and 0.84 ppt (C2Cl4) measured by the NSF NCAR Trace Organic Analyzer (TOGA) during ATom. Both measurements and model show distinct hemispheric gradients with the mean measured Northern to Southern Hemisphere (NH/SH) ratio of 2 or greater for all four Cl-VSLS. In addition, the TOGA profiles over the NH mid-latitudes showed general enhancements in the Pacific basin compared to the Atlantic basin, with up to ?18 ppt difference for CH2Cl2 in the mid troposphere. We tagged regional source emissions of CH2Cl2 and C2Cl4 in the model and found that Asian emissions dominate the global distributions of these species both at the surface (950 hPa) and at high altitudes (150 hPa). Overall, our results confirm relatively high mixing ratios of Cl-VSLS in the UTLS region and show that the CESM model does a reasonable job of simulating their global abundance but we also note the uncertainties with Cl-VSLS emissions and active chlorine sources in the model. These findings will be used to validate future emission inventories and to investigate the fast convective transport of Cl-VSLS to the UTLS region and their impact on stratospheric ozone.

Keeping global surface temperatures below international climate targets will require substantial measures to control atmospheric CO2 and CH4 concentrations. Recent studies have focused on interventions to decrease CH4 through enhanced atmospheric oxidation. Here for the first time using a set of models, we evaluate the effect of adding iron aerosols to the atmosphere to enhance molecular chlorine production, and thus enhance the atmospheric oxidation of methane and reduce its concentration. Using different iron emission sensitivity scenarios, we examine the potential role and impact of enhanced iron emissions on direct interactions with solar radiation, and on the chemical and radiative response of methane. Our results show that the impact of iron emissions on CH4 depends sensitively on the location of the iron emissions. In all emission regions there is a threshold in the amount of iron that must be added to remove methane. Below this threshold CH4 increases. Even once that threshold is reached, the iron-aerosol driven chlorine-enhanced impacts on climate are complex. The radiative forcing of both methane and ozone are decreased in the most efficient regions but the direct effect due to the addition of absorbing iron aerosols tends to warm the planet. Adding any anthropogenic aerosol may also cool the planet due to aerosol cloud interactions, although these are very uncertain, and here we focus on the unique properties of adding iron aerosols. If the added emissions have a similar distribution as current shipping emissions, our study shows that the amount of iron aerosols that must be added before methane decreases is 2.5 times the current shipping emissions of iron aerosols, or 6 Tg Fe yr−1 in the most ideal case examined here. Our study suggests that the photoactive fraction of iron aerosols is a key variable controlling the impact of iron additions and poorly understood. More studies of the sen

In contrast to the general stratospheric ozone recovery following international agreements, recent observations show an ongoing net ozone depletion in the tropical lower stratosphere (LS). This depletion is thought to be driven by dynamical transport accelerated by global warming, while chemical processes have been considered to be unimportant. Here we use a chemistry–climate model to demonstrate that halogenated ozone-depleting very short-lived substances (VSLS) chemistry may account for around a quarter of the observed tropical LS negative ozone trend in 1998–2018. VSLS sources include both natural and anthropogenic emissions. Future projections show the persistence of the currently unaccounted for contribution of VSLS to ozone loss throughout the twenty-first century in the tropical LS, the only region of the global stratosphere not projecting an ozone recovery by 2100. Our results show the need for mitigation strategies of anthropogenic VSLS emissions to preserve the present and future ozone layer in low latitudes.

© 2013 American Meteorological Society. We thank Rolando Garcia, Marianna Vertenstein, Christopher Fischer, Francis Vitt, and Fabrizio Sassi for assistance in developing CESM1 (WACCM) and interpreting its output. We also thank Edwin Gerber for discussions on deriving a simplified NAM index and Rich Neale and David Barriopedro for advice on the calculation of blocking frequency. The CESM project is supported by the National Science Foundation and the Office of Science (BER) of the U.S. Department of Energy. Computing resources were provided by the Climate Simulation Laboratory at NCAR's Computational and Information Systems Laboratory (CISL), sponsored by the National Science Foundation and other agencies. This research was enabled by CISL compute and storage resources. Bluefire, a 4064-processor IBM Power6 resource with a peak of 77 TeraFLOPS, provided more than 7.5 million computing hours, the GLADE high-speed disk resources provided 0.4 PetaBytes of dedicated disk, and CISL's 12-PB HPSS archive provided over 1 PetaByte of storage in support of this research project. LMP is supported in part by a grant from the U.S. National Science Foundation to Columbia University. The National Center for Atmospheric Research is sponsored by the National Science Foundation., 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., U.S. National Science Foundation to Columbia University, National Science Foundation, Office of Science (BER) of the U.S. Department of Energy, Depto. de Física de la Tierra y Astrofísica, Fac. de Ciencias Físicas, TRUE, pub

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., 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.

In contrast to the general stratospheric ozone recovery following international agreements, recent observations show an ongoing net ozone depletion in the tropical lower stratosphere (LS). This depletion is thought to be driven by dynamical transport accelerated by global warming, while chemical processes have been considered to be unimportant. Here we use a chemistry–climate model to demonstrate that halogenated ozone-depleting very short-lived substances (VSLS) chemistry may account for around a quarter of the observed tropical LS negative ozone trend in 1998–2018. VSLS sources include both natural and anthropogenic emissions. Future projections show the persistence of the currently unaccounted for contribution of VSLS to ozone loss throughout the twenty-first century in the tropical LS, the only region of the global stratosphere not projecting an ozone recovery by 2100. Our results show the need for mitigation strategies of anthropogenic VSLS emissions to preserve the present and future ozone layer in low latitudes.

Significance The role of chlorine and bromine in Antarctic stratospheric ozone depletion is well known. However, the contribution of iodine to the ozone hole chemistry has not been assessed, mainly due to the negligible amounts of iodine previously reported to enter the stratosphere. New measurements demonstrate that the injection of iodine to the lower stratosphere is higher than previously assumed. Based on these observations, our modeling work shows that iodine chemistry can enhance spring ozone loss at the lower part of the Antarctic ozone hole, and even dominate the halogen-mediated ozone loss during summer. Iodine can also alter, by several days, the timing of the seasonal formation and closure of the ozone hole.

Abstract As the leading mode of Pacific variability, El Niño–Southern Oscillation (ENSO) causes vast and widespread climatic impacts, including in the stratosphere. Following discovery of a stratospheric pathway of ENSO to the Northern Hemisphere surface, here we aim to investigate if there is a substantial Southern Hemisphere (SH) stratospheric pathway in relation to austral winter ENSO events. Large stratospheric anomalies connected to ENSO occur on average at high SH latitudes as early as August, peaking at around 10 hPa. An overall colder austral spring Antarctic stratosphere is generally associated with the warm phase of the ENSO cycle, and vice versa. This behavior is robust among reanalysis and six separate model ensembles encompassing two different model frameworks. A stratospheric pathway is identified by separating ENSO events that exhibit a stratospheric anomaly from those that do not and comparing to stratospheric extremes that occur during neutral ENSO years. The tropospheric eddy-driven jet response to the stratospheric ENSO pathway is the most robust in the spring following a La Niña, but extends into summer, and is more zonally symmetric compared to the tropospheric ENSO teleconnection. The magnitude of the stratospheric pathway is weaker compared to the tropospheric pathway and therefore, when it is present, has a secondary role. For context, the magnitude is approximately half that of the eddy-driven jet modulation due to austral spring ozone depletion in the model simulations. This work establishes that the stratospheric circulation acts as an intermediary in coupling ENSO variability to variations in the austral spring and summer tropospheric circulation.

Open questions about the modulation of near-surface trace gas variability by stratosphere-troposphere tracer transport complicate efforts to identify anthropogenic sources of gases such as CFC-11 and N2O and disentangle them from dynamical influences. In this study, we explore one model's modulation of lower stratospheric tracer advection by the quasi-biennial oscillation (QBO) of stratospheric equatorial zonal-mean zonal winds at 50 hPa. We assess instances of coherent modulation versus disruption through phase unlocking with the seasonal cycle in the model and in observations. We quantify modeled advective contributions to the temporal rate of change of stratospheric CFC-11 and N2O at extratropical and high-latitudes by calculating a transformed Eulerian mean (TEM) budget across isentropic surfaces from a 10-member WACCM4 ensemble simulation. We find that positive interannual variability in seasonal tracer advection generally occurs in the easterly QBO phase, as in previous work, and briefly discuss physical mechanisms. Individual simulations of the 10-member ensemble display phase-unlocking disruptions from this general pattern due to seasonally varying synchronizations between the model's repeating 28-month QBO cycle and the 12-month seasonal cycle. We find that phase locking and unlocking patterns of tracer advection calculations inferred from observations fall within the envelope of the ensemble member results. Our study bolsters evidence for variability in the interannual stratospheric dynamical influence of CFC-11 near-surface concentrations by assessing the QBO modulation of lower stratospheric advection via synchronization with the annual cycle. It identifies a likely cause of variations in the QBO influence on tropospheric abundances.