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Evaluation of preindustrial to present-day black carbon and its albedo forcing from Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations, and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996-2000. We evaluate the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements. Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5-3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period.We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2-3 of the BC snowpack measurements except for Greenland and the Arctic Ocean. For the ice core evaluation, models tend to adequately capture both the observed temporal trends and the magnitudes at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice cores indicates a strong influence from Western Europe, but the modeled BC increases in that period are consistent with the emission changes in Eastern Europe, the Middle East, South and East Asia. At the Alps site, the simulated BC suggests a strong influence from Europe, which agrees with the Alps ice core observations. At Zuoqiupu on the Tibetan Plateau, models successfully simulate the higher BC concentrations observed during the non-monsoon season compared to the monsoon season but overpredict BC in both seasons. Despite a large divergence in BC deposition at two Antarctic ice core sites, some models with a BC lifetime of less than 7 days are able to capture the observed concentrations. In 2000 relative to 1850, globally and annually averaged BC surface albedo forcing from the offline simulations ranges from 0.014 to 0.019Wm−2 among the ACCMIP models. Comparing offline and online BC albedo forcings computed by some of the same models, we find that the global annual mean can vary by up to a factor of two because of different aerosol models or different BC-snow parameterizations and snow cover. The spatial distributions of the offline BC albedo forcing in 2000 show especially high BC forcing (i.e., over 0.1W/sq. m) over Manchuria, Karakoram, and most of the Former USSR. Models predict the highest global annual mean BC forcing in 1980 rather than 2000, mostly driven by the high fossil fuel and biofuel emissions in the Former USSR in 1980.

snow cover↗

SPARC's Stratospheric Sulfur and its Role in Climate Activity (SSiRC)

The stratospheric aerosol layer is a key component in the climate system. It affects the radiative balance of the atmosphere directly through interactions with solar and terrestrial radiation, and indirectly through its effect on stratospheric ozone. Because the stratospheric aerosol layer is prescribed in many climate models and Chemistry-Climate Models (CCMs), model simulations of future atmospheric conditions and climate generally do not account for the interaction between the aerosol-sulfur cycle and changes in the climate system. The present understanding of how the stratospheric aerosol layer may be affected by future climate change and how the stratospheric aerosol layer may drive climate change is, therefore, very limited. The purposes of SSiRC (Stratospheric Sulfur and its Role in Climate) include: (i) providing a coordinating structure for the various individual activities already underway in different research centers; (ii) encouraging and supporting new instrumentation and measurements of sulfur containing compounds, such as COS, DMS, and non-volcanic SO2 in the UT/LS globally; and (iii) initiating new model/data inter-comparisons. SSiRC is developing collaborations with a number of other SPARC activities including CCMI and ACAM. This presentation will highlight the scientific goals of this project and on-going activities and propose potential interactions between SSiRC and ACAM.

Thomason, Larry↗

Global Total Ozone Recovery Trends Attributed to Ozone-Depleting Substance (ODS) Changes Derived From Five Merged Ozone Datasets

We report on updated trends using different merged zonal mean total ozone datasets from satellite and ground-based observations for the period from 1979 to 2020. This work is an update of the trends reported in Weber et al. (2018) using the same datasets up to 2016. Merged datasets used in this study include NASA MOD v8.7 and NOAA Cohesive Data (COH) v8.6, both based on data from the series of Solar Backscatter Ultraviolet (SBUV), SBUV-2, and Ozone Mapping and Profiler Suite (OMPS) satellite instruments (1978–present), as well as the Global Ozone Monitoring Experiment (GOME)-type Total Ozone – Essential Climate Variable (GTO-ECV) and GOME-SCIAMACHY-GOME-2 (GSG) merged datasets (both 1995–present), mainly comprising satellite data from GOME, SCIAMACHY, OMI, GOME-2A, GOME-2B, and TROPOMI. The fifth dataset consists of the annual mean zonal mean data from ground-based measurements collected at the World Ozone and Ultraviolet Radiation Data Centre (WOUDC). Trends were determined by applying a multiple linear regression (MLR) to annual mean zonal mean data. The addition of 4 more years consolidated the fact that total ozone is indeed slowly recovering in both hemispheres as a result of phasing out ozone-depleting substances (ODSs) as mandated by the Montreal Protocol. The near-global (60° S–60° N) ODS-related ozone trend of the median of all datasets after 1995 was 0.4 ± 0.2 (2σ) %/decade, which is roughly a third of the decreasing rate of 1.5 ± 0.6 %/decade from 1978 until 1995. The ratio of decline and increase is nearly identical to that of the EESC (equivalent effective stratospheric chlorine or stratospheric halogen) change rates before and after 1995, confirming the success of the Montreal Protocol. The observed total ozone time series are also in very good agreement with the median of 17 chemistry climate models from CCMI-1 (Chemistry-Climate Model Initiative Phase 1) with current ODS and GHG (greenhouse gas) scenarios (REF-C2 scenario). The positive ODS-related trends in the Northern Hemisphere (NH) after 1995 are only obtained with a sufficient number of terms in the MLR accounting properly for dynamical ozone changes (Brewer–Dobson circulation, Arctic Oscillation (AO), and Antarctic Oscillation (AAO)). A standard MLR (limited to solar, Quasi-Biennial Oscillation (QBO), volcanic, and El Niño–Southern Oscillation (ENSO)) leads to zero trends, showing that the small positive ODS-related trends have been balanced by negative trend contributions from atmospheric dynamics, resulting in nearly constant total ozone levels since 2000.

Total Column Ozone Trends↗

Quantifying the Effect of Mixing on the Mean Age of Air in CCMVal-2 and CCMI-1 Models

The stratospheric age of air (AoA) is a useful measure of the overall capabilities of a general circulation model (GCM) to simulate stratospheric transport. Previous studies have reported a large spread in the simulation of AoA by GCMs and coupled chemistry-climate models (CCMs). Compared to observational estimates, simulated AoA is mostly too low. Here we attempt to untangle the processes that lead to the AoA differences between the models and between models and observations. AoA is influenced by both mean transport by the residual circulation and two-way mixing; we quantify the effects of these processes using data from the CCM inter-comparison projects CCMVal-2 (Chemistry-Climate Model Validation Activity 2) and CCMI-1 (Chemistry-Climate Model Initiative, phase 1). Transport along the residual circulation is measured by the residual circulation transit time (RCTT). We interpret the difference between AoA and RCTT as additional aging by mixing. Aging by mixing thus includes mixing on both the resolved and subgrid scale. We find that the spread in AoA between the models is primarily caused by differences in the effects of mixing and only to some extent by differences in residual circulation strength. These effects are quantified by the mixing efficiency, a measure of the relative increase in AoA by mixing. The mixing efficiency varies strongly between the models from 0.24 to 1.02. We show that the mixing efficiency is not only controlled by horizontal mixing, but by vertical mixing and vertical diffusion as well. Possible causes for the differences in the models' mixing efficiencies are discussed. Differences in subgrid-scale mixing (including differences in advection schemes and model resolutions) likely contribute to the differences in mixing efficiency. However, differences in the relative contribution of resolved versus parameterized wave forcing do not appear to be related to differences in mixing efficiency or AoA.

CCMI↗

Pre-industrial to End 21st Century Projections of Tropospheric Ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337+/-23 Tg, the ensemble mean burden for 1850 time slice is approx. 30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: −4% (−16 %) for RCP2.6, 2% (−7%) for RCP4.5, 1% (−9%) for RCP6.0, and 7% (18 %) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40-150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly.

Troposphere↗

The Impact of ENSO on Trace Gas Composition in the Upper Troposphere to Lower Stratosphere

The El Nino-Southern Oscillation (ENSO) is the dominant mode of interannual variability in the tropical troposphere and its effects extend well into the stratosphere. Its impact on atmospheric dynamics and chemistry cause important changes to trace gas constituent distributions. A comprehensive suite of satellite observations, reanalyses, and chemistry climate model simulations are illuminating our understanding of processes like ENSO. Analyses of more than a decade of observations from NASAs Aura and Aqua satellites, combined with simulations from the Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM) and other Chemistry Climate Modeling Initiative (CCMI) models, and the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) reanalysis have provided key insights into the response of atmospheric composition to ENSO. While we will primarily focus on ozone and water vapor responses in the upper troposphere to lower stratosphere, the effects of ENSO ripple through many important trace gas species throughout the atmosphere. The very large 2015-2016 El Nino event provides an opportunity to closely examine these impacts with unprecedented observational breadth. An improved quantification of natural climate variations, like those from ENSO, is needed to detect and quantify anthropogenic climate changes.

ENSO↗

Why Does the Stratosphere Get Moister During the 21st Century?

All chemistry-climate models predict that 1) the TTL warms during the 21st century and 2) that the humidity of air entering the stratosphere increases over this same period. It seems reasonable to conclude that the former causes the latter, but to our knowledge no one has actually tested that. We do so here by analyzing one chemistry-climate model in detail (the Goddard Earth Observing System Chemistry Climate Model, GEOSCCM) and find that the warming of the TTL explains only a fraction of the increase in humidity of air entering the stratosphere. We do this by using meteorological fields from the model to drive a trajectory model, which estimates the water vapor variations in response to the large-scale temperature field. Water vapor simulated by the trajectory model increases by about one quarter of the amount it increases in the GEOSCCM. We conclude that, over the 21st century, an increase in the flux of ice through the TTL is responsible for most of the increase in the humidity of air entering the stratosphere in this model.

water vapor↗

Evaluation of ACCMIP Outgoing Longwave Radiation from Tropospheric Ozone Using TES Satellite Observations.

We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5-20 ppb) in the Southern Hemisphere (SH) and modest high bias (5-10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005-2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120mW/ sq. m OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39+/- 41mW/ sq. m relative to TES data. We show that there is a correlation (Sq. R = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750-2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100mW/ sq. m. Removing these models leads to a mean ozone radiative forcing of 394+/- 42mW/ sq. m. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 +/- 60mW/ sq. m derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

troposphere↗

Implications of CO Bias for Ozone and Methane Lifetime in a CCM

A low bias in carbon monoxide compared to observations at high latitudes is a common feature of chemistry climate models. CO bias can both indicate and contribute to a bias in modeled OH and methane lifetime. This study examines possible causes of CO bias in the ACCMIP simulation of the GEOSCCM, and considers how attributing the CO bias to uncertainty in CO emissions versus biases in other constituents impacts the relationship between CO bias and methane lifetime. We use a simplified model of CO tagged by source with specified OH to quantify the sensitivity of the CO bias to changes in CO emissions or OH concentration, comparing the modeled CO to surface and MOPITT observations. The simplified model shows that decreasing OH in the northern hemisphere removes most of the global mean and inter-hemispheric bias in surface CO. We then use results from this analysis to explore how adjusting CO sources in the CCM impacts the concentrations of ozone, OH and methane. The CCM simulation also exhibits biases in ozone and water vapor compared to observations. We use a parameterized CO-OH-CH4 model that takes ozone and water vapor as inputs to the parameterization to examine whether correcting water and ozone biases can alter OH enough to remove the CO bias. Through this analysis, we aim to better quantify the relationship between CO bias and model biases in ozone concentrations and methane lifetime.

carbon monoxide↗

Interactive Ozone and Methane Chemistry in GISS-E2 Historical and Future Climate Simulations

The new generation GISS climate model includes fully interactive chemistry related to ozone in historical and future simulations, and interactive methane in future simulations. Evaluation of ozone, its tropospheric precursors, and methane shows that the model captures much of the largescale spatial structure seen in recent observations. While the model is much improved compared with the previous chemistry-climate model, especially for ozone seasonality in the stratosphere, there is still slightly too rapid stratospheric circulation, too little stratosphere-to-troposphere ozone flux in the Southern Hemisphere and an Antarctic ozone hole that is too large and persists too long. Quantitative metrics of spatial and temporal correlations with satellite datasets as well as spatial autocorrelation to examine transport and mixing are presented to document improvements in model skill and provide a benchmark for future evaluations. The difference in radiative forcing (RF) calculated using modeled tropospheric ozone versus tropospheric ozone observed by TES is only 0.016W/sq. m. Historical 20th Century simulations show a steady increase in whole atmosphere ozone RF through 1970 after which there is a decrease through 2000 due to stratospheric ozone depletion. Ozone forcing increases throughout the 21st century under RCP8.5 owing to a projected recovery of stratospheric ozone depletion and increases in methane, but decreases under RCP4.5 and 2.6 due to reductions in emissions of other ozone precursors. RF from methane is 0.05 to 0.18W/ sq. m higher in our model calculations than in the RCP RF estimates. The surface temperature response to ozone through 1970 follows the increase in forcing due to tropospheric ozone. After that time, surface temperatures decrease as ozone RF declines due to stratospheric depletion. The stratospheric ozone depletion also induces substantial changes in surface winds and the Southern Ocean circulation, which may play a role in a slightly stronger response per unit forcing during later decades. Tropical precipitation shifts south during boreal summer from 1850 to 1970, but then shifts northward from 1970 to 2000, following upper tropospheric temperature gradients more strongly than those at the surface.

Ozone↗

Multi-Model Impacts of Climate Change on Pollution Transport from Global Emission Source Regions

The impacts of climate change on tropospheric transport, diagnosed from a carbon monoxide (CO)-like tracer species emitted from global CO sources, are evaluated from an ensemble of four chemistry-climate model (CCMs) contributing to the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Model time-slice simulations for present-day and end of the 21st century conditions were performed under the Representative Concentrations Pathways (RCP) climate scenario RCP 8.5. All simulations reveal a strong seasonality in transport, especially over the tropics. The highest CO-tracer mixing ratios aloft occur during boreal winter when strong vertical transport is co-located with biomass burning emission source regions. A consistent and robust decrease in future CO-tracer mixing ratios throughout most of the troposphere, especially in the tropics, and an increase around the tropopause is found across the four CCMs in both winter and summer. Decreases in CO-tracer mixing ratios in the tropical troposphere are associated with reduced convective mass fluxes in this region, which in turn may reflect a weaker Hadley Cell circulation in the future climate. Increases in CO-tracer mixing ratios near the tropopause are largely attributable to a rise in tropopause height, although a poleward shift in the midlatitude jets may also play an important role in the extra-tropical upper troposphere. An increase in CO-tracer mixing ratios also occurs near the Equator, centred over EquatorialCentral Africa, extending from the surface to the mid troposphere which is most likely related to localised decreases in convection in the vicinity of the Intertropical Convergence Zone, resulting in larger CO-tracer mixing ratios over biomass burning regions and smaller mixing ratios downwind.

Tropospheric Transport↗

Large-Scale Transport into the Arctic: The Roles of the Midlatitude Jet and the Hadley Cell

Transport from the Northern Hemisphere (NH) midlatitudes to the Arctic plays a crucial role in determining the abundance of trace gases and aerosols that are important to Arctic climate via impacts on radiation and chemistry. Here we examine this transport using an idealized tracer with a fixed lifetime and predominantly midlatitude land-based sources in models participating in the Chemistry Climate Model Initiative (CCMI). We show that there is a 25%-45% difference in the Arctic concentrations of this tracer among the models. This spread is correlated with the spread in the location of the Pacific jet, as well as the spread in the location of the Hadley Cell (HC) edge, which varies consistently with jet latitude. Our results suggest that it is likely that the HC-related zonal-mean meridional transport rather than the jet-related eddy mixing is the major contributor to the inter-model spread in the transport of land-based tracers into the Arctic. Specifically, in models with a more northern jet, the HC generally extends further north and the tracer source region is mostly covered by surface southward flow associated with the lower branch of the HC, resulting in less efficient transport poleward to the Arctic. During boreal summer, there are poleward biases in jet location in free-running models, and these models likely underestimate the rate of transport into the Arctic. Models using specified dynamics do not have biases in the jet location, but do have biases in the surface meridional flow, which may result in differences in transport into the Arctic. In addition to the land-based tracer, the midlatitude-to-Arctic transport is further examined by another idealized tracer with zonally uniform sources. With equal sources from both land and ocean, the inter-model spread of this zonally uniform tracer is more related to variations in parameterized convection over oceans rather than variations in HC extent, particularly during boreal winter. This suggests that transport of land-based and oceanic tracers or aerosols towards the Arctic differs in pathways and therefore their corresponding inter-model variabilities result from different physical processes.

chemistry climate models↗

Quantifying Uncertainty in Projections of Stratospheric Ozone Over the 21st Century

Future stratospheric ozone concentrations will be determined both by changes in the concentration of ozone depleting substances (ODSs) and by changes in stratospheric and tropospheric climate, including those caused by changes in anthropogenic greenhouse gases (GHGs). Since future economic development pathways and resultant emissions of GHGs are uncertain, anthropogenic climate change could be a significant source of uncertainty for future projections of stratospheric ozone. In this pilot study, using an ensemble of opportunity of chemistry-climate model (CCM) simulations, the contribution of scenario uncertainty from different plausible emissions pathways for 10 ODSs and GHGs to future ozone projections is quantified relative to the contribution from model uncertainty and internal variability of the chemistry-climate system. For both the global, annual mean ozone concentration and for ozone in specific geographical regions, differences between CCMs are the dominant source of uncertainty for the first two-thirds of the 21 st century, up-to and after the time when ozone concentrations 15 return to 1980 values. In the last third of the 21st century, dependent upon the set of greenhouse gas scenarios used, scenario uncertainty can be the dominant contributor. This result suggests that investment in chemistry-climate modelling is likely to continue to refine projections of stratospheric ozone and estimates of the return of stratospheric ozone concentrations to pre-1980 levels.

Charlton-Perez, A. J.↗

Connections Between the TTL and Sea Surface Temperatures: Interannual Variability and Trends

Comprehensive chemistry climate models and satellite data are used to investigate the forcing of variability in the tropical lower stratosphere and upper troposphere. As this region is the origination region for air parcels which enter the stratosphere, it is important to understand variability in this region on timescales ranging from the seasonal to decadal. The warming trend in the tropical upper troposphere over the past 30 years is strongest near the Indo Pacific warm pool, while the warming trend in the western and central Pacific is much weaker. In the lower stratosphere, these trends are reversed: the historical cooling trend is strongest over the Indo Pacific warm pool and is weakest in the western and central Pacific. These zonal variations are stronger than the zonal mean response in boreal winter. Targeted experiments with a chemistry climate model are used to demonstrate that sea surface temperature trends are driving the zonal asymmetry in upper tropospheric and lower stratospheric tropical temperature trends. The anomalous circulation set up by the changing SSTs has led to zonal structure in the ozone and water vapor trends near the tropopause, and subsequently to less water vapor entering the stratosphere. Projected future sea surface temperatures appear to drive a temperature and water vapor response whose zonal structure is similar to the historical response. In the lower stratosphere, the changes in water vapor and temperature due to projected future sea surface temperatures is of similar strength to, though slightly weaker than, that due directly to projected future CO2, ozone, and methane. Finally, targeted experiments with a chemistry climate model are used to demonstrate that seasonality and the location of the peak warming of sea surface temperatures dictate the response of stratospheric water vapor to El Nino. In spring, El Nino events in which sea surface temperature anomalies peak in the eastern Pacific lead to a warming at the tropopause above the warm pool region, and subsequently to more stratospheric water vapor (consistent with previous work). However, in fall and in early winter, and also during El Nino events in which the sea surface temperature anomaly is found mainly in the central Pacific, the response is qualitatively different: temperature changes in the warm pool region are nonuniform and less water vapor enters the stratosphere. The difference in water vapor in the lower stratosphere between the two variants of El Nino approaches 0.3 ppmv, while the difference between the winter and spring responses exceeds 0.5 ppmv.

Tropical Tropopause Layer↗

The Connection between Model Performance on the CCMVal Transport Diagnostics and Simulated Sensitivity of Ozone to Chlorine Change

The chemistry climate models that contributed simulations for past and future ozone evolution to the 2010 Scientific Assessment of Ozone Depletion were subject to extensive evaluation by the SPARC (Stratospheric Processes and their Role in Climate) CCMVal (Chemistry-Climate Model Validation) activity. The sensitivity of ozone to changes in composition and climate varies among the models, but the relationship between these variations and the model evaluations of CCMVal is not obvious. We have learned that the transport evaluation can be used to interpret the comparisons between observed and simulated columns of chlorine reservoirs, hydrochloric acid (HCl) and chlorine nitrate (ClONO2); these comparisons were part of the CCMVal evaluation of chemistry. The simulations with best performance on the transport diagnostics most faithfully reproduce the evolution and seasonal variation of the chlorine reservoirs as observed at NDACC (Network for Detection of Atmospheric Composition Change) stations (NyAlesund 78.9N, Kiruna 67.8N, Harestua 60.2N, Jungfraujoch 46.6N, Toronto 43.6N, Kitt Peak 31.9N, Izana 28.3N, Mauna Loa 19.5N, Lauder 45S and Arrival Heights 77.8S). In the simulations, the HCl in the lower stratosphere depends on total inorganic chlorine (Cly) and partitioning between HCl and ClON02. Total inorganic chlorine depends on the fractional release of chlorine from source gases, and ratio of ClON02 to HCl is inversely dependent on methane and varies quadratically with ozone. Simulated HCl from various models may agree with observations even though Cly is in error, partitioning is in error, or both. Simulated ozone sensitivity to chlorine is shown to be greater for models that produce larger values of chlorine nitrate for background chlorine levels, and vice versa. Comparisons with the NDACC data show why the models with 'best' transport have similar sensitivity to chlorine change. The realistic evolution of the simulated HCl and ClONO2 columns suggests realistic levels of Cly in the lower atmosphere. In addition, the wide range values for the sensitivity of ozone to chlorine obtained from the CCMVal simulations is explained by the wide range in lower atmospheric columns of ClONO2 and the concomitant wide range of levels for chlorine monoxide.

Douglass, Anne↗

Impact of Stratospheric Ozone Zonal Asymmetries on the Tropospheric Circulation

The depletion and recovery of Antarctic ozone plays a major role in changes of Southern Hemisphere (SH) tropospheric climate. Recent studies indicate that the lack of polar ozone asymmetries in chemistry climate models (CCM) leads to a weaker and warmer Antarctic vortex, and smaller trends in the tropospheric mid-latitude jet and the surface pressure. However, the tropospheric response to ozone asymmetries is not well understood. In this study we report on a series of integrations of the Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) to further examine the effect of zonal asymmetries on the state of the stratosphere and troposphere. Integrations with the full, interactive stratospheric chemistry are compared against identical simulations using the same CCM except that (1) the monthly mean zonal mean stratospheric ozone from first simulation is prescribed and (2) ozone is relaxed to the monthly mean zonal mean ozone on a three day time scale. To analyze the tropospheric response to ozone asymmetries, we examine trends and quantify the differences in temperatures, zonal wind and surface pressure among the integrations.

Chemistry-Climate Modeling↗

Effects of Greenhouse Gas Increase and Stratospheric Ozone Depletion on Stratospheric Mean Age of Air in 1960-2010

The relative impacts of greenhouse gas (GHG) increase and stratospheric ozone depletion on stratospheric mean age of air in the 1960-2010 period are quantified using the Goddard Earth Observing System Chemistry-Climate Model. The experiment compares controlled simulations using a coupled atmosphere-ocean version of the Goddard Earth Observing System Chemistry-Climate Model, in which either GHGs or ozone depleting substances, or both factors evolve over time. The model results show that GHGs and ozone-depleting substances have about equal contributions to the simulated mean age decrease, but GHG increases account for about two thirds of the enhanced strength of the lower stratospheric residual circulation. It is also found that both the acceleration of the diabatic circulation and the decrease of the mean age difference between downwelling and upwelling regions are mainly caused by GHG forcing. The results show that ozone depletion causes an increase in the mean age of air in the Antarctic summer lower stratosphere through two processes: (1) a seasonal delay in the Antarctic polar vortex breakup that inhibits young midlatitude air from mixing with the older air inside the vortex, and (2) enhanced Antarctic downwelling that brings older air from middle and upper stratosphere into the lower stratosphere.

stratospheric ozone depletion↗

Lower-Stratospheric Tracer Trends and Variability from Reanalyses

Previous studies have robustly identified a decrease since 1998 in lower stratospheric ozone in the Northern Hemisphere (NH). While this ozone decrease is qualitatively explained as resulting from changes in the large-scale circulation, there is not yet a quantitative mechanistic explanation of these changes. Here we explore the drivers of recent ozone changes using two different configurations of the Goddard Earth Observing System (GEOS) general circulation model. The first configuration of GEOS includes a full chemistry module and is constrained with meteorological fields from the MERRA-2 reanalysis. This configuration (M2GMI) is used to analyze an idealized tracer that covaries closely with ozone on interannual and decadal timescales, revealing that recent ozone decreases in the NH subtropics are associated with a poleward expansion of upwelling in the NH LS, with reduced (enhanced) downwelling over northern subtropics (midlatitudes). The second configuration of GEOS is a free-running version of the GEOS Chemistry-Climate Model (CCM) that is used to perform a ten-member ensemble of free-running simulations. Comparisons of the two configurations reveal that, while the free-running model can produce negative ozone changes in the NH LS, the magnitude of these changes is significantly weaker, relative to both M2GMI and MERRA-2; moreover, these weaker ozone decreases are consistent with weaker simulated changes in the residual circulation. Finally, we examine the GEOS model results in the broader context of the hindcast simulations performed as part of Phase 1 of the Chemistry Climate Modeling Initiative. We show that the majority of the free-running simulations considered here also exhibit weaker long-term residual circulation changes, compared to reanalyses.

Wargan, Kris↗