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NASA NTRS2023

The Emissions Model Intercomparison Project (Emissions-MIP): Quantifying Model Sensitivity to Emission Characteristics

Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO 2 injection, seasonality of SO 2 and black carbon (BC) particulate emissions, and the assumed fraction of SO 2 emissions that is injected into the atmosphere as particulate phase sulfate (SO 4 ) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO 2 , SO 4 , and BC, with a particularly large relative variation for SO 2 , which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO 2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of −0.35 W m −2 ), SO 2 lifetime over Northern Hemisphere land (maximum difference of 0.8 d), surface SO 2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO 2 at height consistently increased SO 2 and SO 4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO 4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO 4 emission fraction are accurately and consistently represented in global models.

Emissions Model Intercomparison Project↗
NASA NTRS2013

Sensitivity of the Atmospheric Response to Warm Pool El Nino Events to Modeled SSTs and Future Climate Forcings

Warm pool El Nino (WPEN) events are characterized by positive sea surface temperature (SST) anomalies in the central equatorial Pacific. Under present-day climate conditions, WPEN events generate poleward propagating wavetrains and enhance midlatitude planetary wave activity, weakening the stratospheric polar vortices. The late 21st century extratropical atmospheric response to WPEN events is investigated using the Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM), version 2. GEOSCCM simulations are forced by projected late 21st century concentrations of greenhouse gases (GHGs) and ozone-depleting substances (ODSs) and by SSTs and sea ice concentrations from an existing ocean-atmosphere simulation. Despite known ocean-atmosphere model biases, the prescribed SST fields represent a best estimate of the structure of late 21st century WPEN events. The future Arctic vortex response is qualitatively similar to that observed in recent decades but is weaker in late winter. This response reflects the weaker SST forcing in the Nino 3.4 region and subsequently weaker Northern Hemisphere tropospheric teleconnections. The Antarctic stratosphere does not respond to WPEN events in a future climate, reflecting a change in tropospheric teleconnections: The meridional wavetrain weakens while a more zonal wavetrain originates near Australia. Sensitivity simulations show that a strong poleward wavetrain response to WPEN requires a strengthening and southeastward extension of the South Pacific Convergence Zone; this feature is not captured by the late 21st century modeled SSTs. Expected future increases in GHGs and decreases in ODSs do not affect the polar stratospheric responses to WPEN.

stratosphere↗
NASA NTRS2011

A Model Study of the Impact of Source Gas Changes on the Stratosphere for 1850-2100

The long term stratospheric impacts due to emissions of CO2, CH4, N2O, and ozone depleting substances (ODSs) are investigated using an updated version of the Goddard two-dimensional (2D) model. Perturbation simulations with the ODSs, CO2, CH4, and N2O varied individually are performed to isolate the relative roles of these gases in driving stratospheric changes over the 1850-2100 time period. We also show comparisons with observations and the God- 40 dard Earth Observing System chemistry-climate model simulations for the time period 1970-2100 to illustrate that the 2D model captures the basic processes responsible for longterm stratospheric change. The 2D simulations indicate that prior to 1940, the 45 ozone increases due to CO2 and CH4 loading outpace the ozone losses due to increasing N2O and carbon tetrachloride (CCl4) emissions, so that ozone reaches a broad maximum during the 1920s-1930s. This preceeds the significant ozone depletion during approx. 1960-2050 driven by the ODS loading. During the latter half of the 21st century as ODS emissions diminish, CO2, N2O, and CH4 loading will all have significant impacts on global total ozone based on the IPCC AIB (medium) scenario, with CO2 having the largest individual effect. Sensitivity tests illustrate that due to the strong chemical interaction between methane and chlorine, the CH4 impact on total ozone becomes significantly more positive with larger ODS loading. The model simulations also show that changes in stratospheric temperature, Brewer-Dobson circulation (BDC), and age of air during 1850-2100 are controlled mainly by the CO2 and ODS loading. The simulated acceleration of the BDC causes the age of air to decrease by approx. 1 year from 1860-2100. The corresponding photochemical lifetimes of N2O, CFCl3, CF2Cl2, and CCl4 decrease by 11-13% during 1960-2100 due to the acceleration of the BDC, with much smaller lifetime changes 4%) caused by changes in the photochemical loss rates.

Fleming, E. L.↗
NASA NTRS2011

Global Multi-Year O3-CO Correlation Patterns from Models and TES Satellite Observations

The correlation between measured tropospheric ozone (O3) and carbon monoxide (CO) has been used extensively in tropospheric chemistry studies to explore the photochemical characteristics of different regions and to evaluate the ability of models to capture these characteristics. Here, we present the first study that uses multi-year, global, vertically resolved, simultaneous and collocated O3 and CO satellite (Tropospheric Emission Spectrometer) measurements, to determine this correlation in the middle/lower free troposphere for two different seasons, and to evaluate two chemistry-climate models. We find results that are fairly robust across different years, altitudes and timescales considered, which indicates that the correlation maps presented here could be used in future model evaluations. The highest positive correlations (around 0.8) are found in the northern Pacific during summer, which is a common feature in the observations and the G-PUCCINI model. We make quantitative comparisons between the models using a single-figure metric (C), which we define as the correlation coefficient between the modeled and the observed O3-CO correlations for different regions of the globe. On a global scale, the G-PUCCINI model shows a good performance in the summer (C =0.71) and a satisfactory performance in the winter (C = 0.52). It captures midlatitude features very well, especially in the summer, whereas the performance in regions like South America or Central Africa is weaker. The UKCA model (C = 0.46/0.15 for July-August/December-January on a global scale) performs better in certain regions, such as the tropics in winter, and it captures some of the broad characteristics of summer extratropical correlations, but it systematically underestimates the O3-CO correlations over much of the globe. It is noteworthy that the correlations look very different in the two models, even though the ozone distributions are similar. This demonstrates that this technique provides a powerful global constraint for understanding modeled tropospheric chemical processes. We investigated the sources of the correlations by performing a series of sensitivity experiments. In these, the sign of the correlation is, in most cases, insensitive to removing different individual emissions, but its magnitude changes downwind of emission regions when applying such perturbations. Interestingly, we find that the O3-CO correlation does not solely reflect the strength of O3 photochemical production, as often assumed by earlier studies, but is more complicated and may reflect a mixture of different processes such as transport.

Voulgarakis, A.↗
NASA NTRS2012

Global Air Quality and Climate

Emissions of air pollutants and their precursors determine regional air quality and can alter climate. Climate change can perturb the long-range transport, chemical processing, and local meteorology that influence air pollution. We review the implications of projected changes in methane (CH4), ozone precursors (O3), and aerosols for climate (expressed in terms of the radiative forcing metric or changes in global surface temperature) and hemispheric-to-continental scale air quality. Reducing the O3 precursor CH4 would slow near-term warming by decreasing both CH4 and tropospheric O3. Uncertainty remains as to the net climate forcing from anthropogenic nitrogen oxide (NOx) emissions, which increase tropospheric O3 (warming) but also increase aerosols and decrease CH4 (both cooling). Anthropogenic emissions of carbon monoxide (CO) and non-CH4 volatile organic compounds (NMVOC) warm by increasing both O3 and CH4. Radiative impacts from secondary organic aerosols (SOA) are poorly understood. Black carbon emission controls, by reducing the absorption of sunlight in the atmosphere and on snow and ice, have the potential to slow near-term warming, but uncertainties in coincident emissions of reflective (cooling) aerosols and poorly constrained cloud indirect effects confound robust estimates of net climate impacts. Reducing sulfate and nitrate aerosols would improve air quality and lessen interference with the hydrologic cycle, but lead to warming. A holistic and balanced view is thus needed to assess how air pollution controls influence climate; a first step towards this goal involves estimating net climate impacts from individual emission sectors. Modeling and observational analyses suggest a warming climate degrades air quality (increasing surface O3 and particulate matter) in many populated regions, including during pollution episodes. Prior Intergovernmental Panel on Climate Change (IPCC) scenarios (SRES) allowed unconstrained growth, whereas the Representative Concentration Pathway (RCP) scenarios assume uniformly an aggressive reduction, of air pollutant emissions. New estimates from the current generation of chemistry-climate models with RCP emissions thus project improved air quality over the next century relative to those using the IPCC SRES scenarios. These two sets of projections likely bracket possible futures. We find that uncertainty in emission-driven changes in air quality is generally greater than uncertainty in climate-driven changes. Confidence in air quality projections is limited by the reliability of anthropogenic emission trajectories and the uncertainties in regional climate responses, feedbacks with the terrestrial biosphere, and oxidation pathways affecting O3 and SOA.

ozone↗
NASA NTRSDate not supplied

Improved Characterization of PSC Processes Derived from a Third-Generation CALIOP and MLS Detection and Composition Classification Algorithm

The new 3-year CloudSat and CALIPSO Science Team project described in this poster will use a unique combination of data from the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) instrument on CALIPSO and the Microwave Limb Sounder (MLS) on Aura, in conjunction with supporting meteorological information and detailed modeling studies, to advance our understanding of polar stratospheric cloud (PSC) processes and their role in ozone depletion. We will develop a third-generation (Gen3) PSC detection and composition algorithm that incorporates a new, more robust two-dimensional, multi-channel CALIOP feature detection scheme (2D-McDA). We will also devise and implement an improved two-dimensional PSC composition classification scheme that utilizes multiple parameters (e.g., CALIOP 532-nm parallel and perpendicular scattering ratios, CALIOP 1064-nm total scattering ratio, MLS HNO3 and H2O, ambient temperature, and temperature histories) in a Bayesian approach to determine the most likely PSC composition and help constrain solid PSC particle number density and size/shape. The combined CALIOP/MLS analyses will allow us to study in detail the full life cycle of PSCs and their resulting impact on gas-phase HNO3 and H2O, which should lead to improved parameterizations of PSC microphysics in global chemistry-climate models (CCMs) where detailed particle information is not available. The Gen3 CALIOP PSC algorithm will be a natural stepping-stone toward the analysis of data collected during future spaceborne lidar missions, such as NASA’s Atmosphere Observation System (AOS) mission currently scheduled for launch late in this decade. We will also investigate possible trends in PSC occurrence and composition over the entire CALIOP data record and through further comparisons with the Stratospheric Aerosol Measurement (SAM) II solar occultation PSC record from 1979-1989. Finally, we will validate the mountain-wave parameterization and PSC schemes used in the UM-UKCA (Unified Model coupled to the United Kingdom Chemistry and Aerosol module) CCM through detailed comparisons with earlier CALIOP PSC data products and those developed under this proposal.

CALIPSO↗
NASA NTRSDate not supplied

A14H-04 Analysis of Simulated and Observed Trends in Global Surface PM2.5 and Aerosol Optical Properties from 1958 to 2018 Using the NASA GEOSCCM

Modeling of long-term trends of aerosols and their properties is important for constraining aerosol-climate forcing, and for characterizing changes in particulate matter pollution speciation and exposure. Here we study global and regional long-term trends in surface fine particulate matter (PM ) and aerosol optical properties for 60 years from 1958 to 2018, using simulations performed with the NASA Goddard Earth Observing System Chemistry Climate Model (GEOSCCM), and evaluate the model hindcast with observations for the last three decades. Comparing the modeled aerosols with a diverse set of observations helps interpret observed and simulated trends, and serves as a benchmark for future GEOSCCM developments and input datasets improvements. We first characterize modeled global and regional temporal changes in surface PM and its components, aerosol optical depth (AOD) and single scattering albedo (SSA) and we interpret their link with emissions drivers. We then compare modeled surface PM with ground-based observations from monitoring networks and with global reconstructed PM datasets from observations-model data fusion. Total AOD is compared with long-term satellite measurements from the Moderate Resolution Imaging Spectroradiometer (MODIS) and measurements from the ground-based Aerosol Robotic Network (AERONET). Additional aerosol optical properties, such as absorption and scattering coefficients, are evaluated with ground-based observations from the Global Atmosphere Watch (GAW) records.

aerosols↗
NASA NTRSDate not supplied

LOTUS Highlights on Ozone Trend Analyses and Phase 3 Direction

LOTUS (Long-term Ozone Trends and Uncertainties in the Stratosphere) is a SPARC (Stratosphere-troposphere Processes And their Role in Climate)-sponsored effort to foster collaboration between established and early career scientists around the world, with expertise in ozone observations, modeling, and trend tools, with an aim toward innovating new climate research that meets the needs of the ozone trends community and provides vital contributions to the WMO Assessment in an organized and cohesive way. Here we will summarize recent studies associated with the LOTUS effort that perform trend analyses on both total column and vertical profiles of ozone. The main findings of the derived trends from both observations and chemistry climate models have important implications for the status of the ozone layer as they pertain to the efficacy of the Montreal Protocol. These results also present new questions and knowledge gaps that will be outlined as areas of future study in Phase 3 of the LOTUS effort over the next few years to inform the next Assessment.

LOTUS↗
NASA NTRS2023

StratoFIRE: Modeling Wildfire Smoke in the Stratosphere

The most extreme manifestation of a fire–weather interaction is the formation of pyrocumulonimbus (pyroCb) thunderstorms, triggered by super-heated updrafts, which can eject smoke at altitudes exceeding 20 Km. In this study, we investigated climate-related impacts from the most intensive pyroCb-triggered injection of smoke in the stratosphere: the Australian New Year wildfires in 2019/2020. We first provide a general overview of the vision and objectives of the StratoFIRE project. With the aid of the global chemistry-climate model EMAC, we then simulate radiative and chemical perturbations in the stratosphere in relation to 0.9 Tg smoke in the stratosphere assuming different injection heights, from 13 to 16 Km. The simulation of stratospheric optical depth perturbations were found to be sensitive to the assumed injection height, with a maximum height at 16 Km showing the best agreement with the GLOSSAC and SAGE-ISS aerosol extinction observations.

PyroCb↗
DOE OSTI2024

Validating a microphysical prognostic stratospheric aerosol implementation in E3SMv2 using observations after the Mount Pinatubo eruption

Abstract. This paper describes the addition of a stratospheric prognostic aerosol (SPA) capability – developed with the goal of accurately simulating sulfate aerosol formation and evolution in the stratosphere – in the Department of Energy (DOE) Energy Exascale Earth System Model, version 2 (E3SMv2). The implementation includes changes to the four-mode Modal Aerosol Module microphysics in the stratosphere to allow for larger particle growth and more accurate stratospheric aerosol lifetime following the Pinatubo eruption. E3SMv2-SPA reasonably reproduces stratospheric aerosol lifetime, burden, aerosol optical depth, and top-of-atmosphere flux when compared to remote sensing observations. E3SMv2-SPA also has close agreement with the interactive chemistry–climate model CESM2-WACCM (Community Earth System Model version 2–Whole Atmosphere Community Climate Model) – which has a more complete chemical treatment – and the observationally constrained, prescribed volcanic aerosol treatment in E3SMv2. Global stratospheric aerosol size distributions identify the nucleation and growth of sulfate aerosol from volcanically injected SO2 from both major and minor volcanic eruptions from 1991 to 1993. The modeled aerosol effective radius is consistently lower than satellite and in situ measurements (max differences of ∼ 30 %). Comparisons with in situ size distribution samples indicate that this simulated underestimation in both E3SMv2-SPA and CESM2-WACCM is due to overly small accumulation and coarse-mode aerosols 6–18 months post-eruption, with E3SMv2-SPA simulating ∼ 50 % of the coarse-mode geometric mean diameters of observations 11 months post-eruption. Effective radii from the models and observations are used to calculate offline scattering and absorption efficiencies to explore the implications of smaller simulated aerosol size for the Pinatubo climate impacts. Scattering efficiencies at wavelengths of peak solar irradiance (∼ 0.5 µm) are 10 %–80 % higher for daily samples in models relative to observations through 1993, suggesting higher diffuse radiation at the surface and a larger cooling effect in the models due to the smaller simulated aerosol; absorption efficiencies at the peak wavelengths of outgoing terrestrial radiation (∼ 10 µm) are 15 %–40 % lower for daily samples in models relative to observations, suggesting an underestimation in stratospheric heating in the models due to the smaller simulated aerosol. These potential biases are based on aerosol size alone and do not take into account differences in the aerosol number. The overall agreement of E3SMv2-SPA with observations and its similar performance to the well-validated CESM2-WACCM makes E3SMv2-SPA a viable alternative to simulating climate impacts from stratospheric sulfate aerosols.

Brown, Hunter York (ORCID:0000000218147874)↗
NASA NTRS2000

Dynamic-Chemical Coupling of the Upper Troposphere and Lower Stratosphere Region

The importance of the interaction of chemistry and dynamics in the upper troposphere and lower stratosphere for chemical species like ozone is investigated using two chemistry-climate models. Species emitted in the upper troposphere, like NOx (=NO+NO2) by lightning or aircraft, have the chance to be transported into the lowermost stratosphere. Trajectory calculations suggest that the main transport pathway runs via the Inter Tropical Convergence Zone, across the tropical tropopause and then to higher latitudes, i.e. into the lowermost stratosphere. Longer lifetimes of NOx in the lower stratosphere yield an accumulation of NO. there, which feeds back on upper troposphere chemistry. This effect has been estimated for lightning NO. emissions and reveals a contribution of at least 25% to 40% to the total northern hemisphere mid-latitude lightning increase of either NOx and ozone.

Grewe, Volker↗
NASA NTRS2016

Silicon Chemistry in the Mesosphere and Lower Thermosphere

Silicon is one of the most abundant elements in cosmic dust, and meteoric ablation injects a significant amount of Si into the atmosphere above 80 km. In this study, a new model for silicon chemistry in the mesosphere lower thermosphere is described, based on recent laboratory kinetic studies of Si, SiO,SiO2, and S(exp +). Electronic structure calculations and statistical rate theory are used to show that the likely fate of SiO2 is a two-step hydration to silicic acid (Si(OH)4), which then polymerizes with metal oxides and hydroxides to form meteoric smoke particles. This chemistry is then incorporated into a whole atmosphere chemistry-climate model. The vertical profiles of Si+ and the Si(exp +)Fe(exp +) ratio are shown to be in good agreement with rocket-borne mass spectrometric measurements between 90 and 110 km. Si(exp +) has consistently been observed to be the major meteoric ion around 110 km; this implies that the relative injection rate of Si from meteoric ablation, compared to metals such as Fe and Mg, is significantly larger than expected based on the irrelative chondritic abundances. Finally, the global abundances of SiO and Si(OH)4 show clear evidence of the seasonal meteoric input function, which is much less pronounced in the case of other meteoric species.

Plane, John M. C.↗
NASA NTRS2022

3-D Atmospheric Modeling of the Global Budget of N2O and its Isotopologues for 1980-2019: The Impact of Anthropogenic Emissions

Nitrous oxide (N2O) is the third most important anthropogenic greenhouse gas (GHG) and a major ozone-depleting substance (ODS). Its main sources include anthropogenic activities (mostly agriculture) and natural emissions from ocean and soils. However, emission estimates for individual sources are highly variable due to uncertainties in N2O lifetime estimates and partitioning among sources. We derive annual global N2O emissions for 1990-2019 using NOAA Global Monitoring Laboratory (GML) surface N2O observations and the N2O lifetime calculated in the NASA GEOS-5 chemistry climate model (CCM). The inferred global mean N2O emissions has gradually increased from ~15.8 TgN/yr in the early 1990s to ~17.8 TgN/yr in the 2010s. This implies that anthropogenic N2O emissions have grown rapidly from ~6.7 TgN/yr in the 1990s to about ~8.7 TgN/yr in the 2010s, a ~30% increase. With specially designed N2O isotopic tracers in 3-D GEOSCCM, we estimate that, on global average, stratospheric enrichment contributes about +7.7‰/yr, +7.6‰/yr, +8.0‰/yr to tropospheric N(sup α)-δ(sup 15), N(sup β)-δ(sup 15), and O-δ(sup 18) budget, respectively. To balance the global mean isotopic signature for pre-industrial terrestrial sources of N(sup α)-δ(sup 15) ~ 6.7‰, N(sup β)-δ(sup 15) ~ -12.6‰, O-δ(sup 18) ~ 35.4‰, our 3-D isotopic budget simulation using the GEOSCCM suggests global mean anthropogenic isotopic signatures in the recent decades are N(sup α)-δ(sup 15) ~ -18‰, N(sup β)-δ(sup 15) ~ -20‰, O-δ(sup 18) ~ 19‰. These anthropogenic isotopic estimates are significantly lighter than results from one-box atmospheric model-based estimates with the largest difference seen for N(sup β)-δ(sup 15). More surface isotopic measurements are needed to better quantify the N2O isotopic signatures.

Nitrous oxide↗
NASA NTRS2014

On the Hiatus in the Acceleration of Tropical Upwelling Since the Beginning of the 21st Century

Chemistry-climate models predict an acceleration of the upwelling branch of the Brewer-Dobson circulation as a consequence of increasing global surface temperatures, resulting from elevated levels of atmospheric greenhouse gases. The observed decrease of ozone in the tropical lower stratosphere during the last decades of the 20th century is consistent with the anticipated acceleration of upwelling. However, more recent satellite observations of ozone reveal that this decrease has unexpectedly stopped in the first decade of the 21st century, challenging the implicit assumption of a continuous acceleration of tropical upwelling. In this study we use three decades of chemistry transport-model simulations (1980-2013) to investigate this phenomenon and resolve this apparent contradiction. Our model reproduces the observed tropical lower stratosphere ozone record, showing a significant decrease in the early period followed by a statistically robust trend-change after 2002. We demonstrate that this trend-change is correlated with corresponding changes in the vertical transport and conclude that a hiatus in the acceleration of tropical upwelling occurred during the last decade.

trends↗
NASA NTRSDate not supplied

Overview of the SPARC Reanalysis Intercomparison Project (S-RIP) during 2013-2020

The Stratosphere-troposphere Processes And their Role in Climate (SPARC) project is one of the four core projects of the World Climate Research Programme (WCRP). Researchers interested in SPARC use global atmospheric reanalysis products to understand a wide range of processes and variability in the atmosphere, to validate chemistry climate models, and to investigate and identify climate change. The SPARC Reanalysis Intercomparison Project (S-RIP) was initiated in 2011 and officially started in 2013 to conduct a coordinated intercomparison of all major global atmospheric reanalysis data sets. The S-RIP has been aiming at writing up an assessment report in the SPARC report series (to be published by the end of 2020) (1) on overall quality of temperature, winds, ozone, and water vapor data, (2) on more process- and region-oriented evaluation of the Brewer–Dobson circulation, extratropical stratosphere-troposphere coupling, extratropical upper troposphere and lower stratosphere, the tropical tropopause layer, the quasi-biennial oscillation, polar processes, and the upper stratosphere and lower mesosphere, and (3) with a coordinated description of the reanalysis systems. We also have an inter-journal special issue on "The SPARC Reanalysis Intercomparison Project (S-RIP)" in Atmospheric Chemistry and Physics (ACP) and Earth System Science Data (ESSD). In the presentation, we will discuss key findings and recommendations as well as the evaluation of this rst phase of the S-RIP activity.

Masatomo Fujiwara↗
NASA NTRS2022

Updated Trends of the Stratospheric Ozone Vertical Distribution in the 60°S-60°N Latitude Range Based on the LOTUS Regression Model

This study presents an updated evaluation of stratospheric ozone profile trends in the 60°S - 60°N latitude range over the 2000 - 2020 period using an updated version of the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) regression model that was used to evaluate such trends up to 2016 for the last WMO Ozone Assessment (2018). In addition to the derivation of detailed trends as a function of latitude and vertical coordinates, the regressions are performed with the data sets averaged over broad latitude bands, i.e., 60°S–35°S, 20°S–20°N and 35°N–60°N. The same methodology as in the last Assessment is applied to combine trends in these broad latitude bands in order to compare the results with the previous studies. Longitudinally resolved merged satellite records are also considered in order to provide a better comparison with trends retrieved from ground-based records, e.g., lidar, ozone sondes, Umkehr, microwave and Fourier Transform Infrared (FTIR) spectrometers at selected stations where long-term time series are available. The study includes a comparison with trends derived from the REF-C2 simulations of the Chemistry Climate Model Initiative (CCMI-1). This work confirms past results showing an ozone increase in the upper stratosphere, which is now significant in the three broad latitude bands. The increase is largest in the northern and southern hemisphere midlatitudes, with ~2.2%/decade at ~2.1 hPa, and ~2.1%/decade at ~3.2 hPa respectively, compared to ~1.6%/decade at ~2.6 hPa in the tropics. New trend signals have emerged from the records, such as a significant decrease of ozone in the tropics around 35 hPa and a non-significant increase of ozone in the southern midlatitudes at about 20 hPa. Non-significant negative ozone trends are derived in the lowermost stratosphere, with the most pronounced trends in the tropics. While a very good agreement is obtained between trends from merged satellite records and the CCMI-1 REF-C2 simulation in the upper stratosphere, observed negative trends in the lower stratosphere are not reproduced by models at southern and, in particular, at northern midlatitudes, where models report an ozone increase. However, the lower stratospheric trend uncertainties are quite large, for both measured and modelled trends. Finally, 2000-2020 stratospheric ozone trends derived from the ground-based and longitudinally resolved satellite records are in reasonable agreement over the European Alpine and tropical regions, while at the Lauder station in the southern hemisphere mid-latitudes they show some differences.

Stratospheric ozone trends↗
NASA NTRS2016

Chemistry Simulations Using MERRA-2 Reanalysis with the GMI CTM and Replay in Support of the Atmospheric Composition Community

Simulations using reanalyzed meteorological conditions have been long used to understand causes of atmospheric composition change over the recent past. Using the new Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) meteorology, chemistry simulations are being conducted to create products covering 1980-2016 for the atmospheric composition community. These simulations use the Global Modeling Initiative (GMI) chemical mechanism in two different models: the GMI Chemical Transport Model (CTM) and the GEOS-5 model developed Replay mode. Replay mode means an integration of the GEOS-5 general circulation model that is incrementally adjusted each time step toward the MERRA-2 analysis. The GMI CTM is a 1 x 1.25 simulation and the MERRA-2 GMI Replay simulation uses the native MERRA-2 approximately horizontal resolution on the cubed sphere. The Replay simulations is driven by the online use of key MERRA-2 meteorological variables (i.e. U, V, T, and surface pressure) with all other variables calculated in response to those variables. A specialized set of transport diagnostics is included in both runs to better understand trace gas transport and changes over the recent past.

Chemistry-Climate Model↗
DOE OSTI2023

Comparing the Effect of Anthropogenically Amplified Halogen Natural Emissions on Tropospheric Ozone Chemistry Between Pre-Industrial and Present-Day

Reactive halogens (X + XO, X = I, Br or Cl) catalytically destroy a fraction of tropospheric ozone under present-day (PD) conditions, however, their distribution and potential impact on tropospheric ozone under pre-industrial (PI) conditions remain largely unexplored. This study uses the Community Atmosphere Model with Chemistry (CAM-Chem) to investigate the effect of anthropogenically amplified natural emissions of halogenated species and their subsequent chemistry on tropospheric ozone under PI and PD atmospheric conditions. Model results show that the global tropospheric ozone depletion due to natural halogens is slightly more sensitive in PI than PD, with percentage changes in tropospheric ozone burden (TOB) of -14.1 ± 0.6% for PI and -12.9 ± 0.6% for PD. Individually, the role of iodine and chlorine in ozone depletion is equivalent in both periods (ΔTOB I : ~-7% and ΔTOB Cl : ~-2.5%), while bromine plays a larger role in PI (ΔTOB Br : -5.5 ± 0.6%) versus PD (ΔTOB Br : -4.3 ± 0.7%). The increase in anthropogenic ozone precursor emissions from PI to PD has amplified the natural emission of inorganic halogens and led to a shift in the partitioning of inorganic halogens from reactive to reservoir species. Consequently, halogen-driven ozone depletion from the surface to the free troposphere is larger in PI than PD. In contrast, in the upper troposphere, the ozone depletion is larger in PD influenced mainly by stratospheric intrusion of reactive halogens from long-lived species. This study highlights the importance of including a complete chemical coupling of natural halogens and atmospheric pollutants in chemistry-climate models to adequately assess their effects on tropospheric ozone in a changing climate.

54 ENVIRONMENTAL SCIENCES↗