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NASA NTRS2018

Effect of Gravity Waves from Small Islands in the Southern Ocean on the Southern Hemisphere Atmospheric Circulation

The effect of small islands in the Southern Ocean on the atmospheric circulation in the Southern Hemisphere is considered with a series of simulations using the NASA Goddard Earth Observing System Chemistry-Climate Model in which the gravity wave stress generated by these islands is increased to resemble observed values. The enhanced gravity wave drag leads to a 2 K warming of the springtime polar stratosphere, partially ameliorating biases in this region. Resolved wave drag declines in the stratospheric region in which the added orographic gravity waves deposit their momentum, such that changes in gravity waves are partially compensated by changes in resolved waves, though resolved wave drag increases further poleward. The orographic drag from these islands has impacts for surface climate, as biases in tropospheric jet position are also partially ameliorated. These results suggest that these small islands are likely contributing to the missing drag near 60 degrees S in the upper stratosphere evident in many data assimilation products.

chemistry-climate models↗
NASA NTRS2017

An Update on Ozone Profile Trends for the Period 2000 to 2016

Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data measured by four techniques at stations of the Network for the Detection of Atmospheric Composition Change indicate significant ozone increases in the upper stratosphere, between 35 and 48 kilometers altitude (5 and 1 hectopascals). Near 2 hectopascals (42 kilometers), ozone has been increasing by about 1.5 percent per decade in the tropics (20 degrees S to 20 degrees N), and by 2 to 2.5 percent per decade in the 35 to 60 degree latitude bands of both hemispheres. At levels below 35 kilometers (5 hectopascals), 2000 to 2016 ozone trends are smaller and not statistically significant. The observed trend profiles are consistent with expectations from chemistry climate model simulations. This study confirms positive trends of upper stratospheric ozone already reported, e.g., in the WMO/UNEP (World Meteorological Organization/United Nations Environmental Programme) Ozone Assessment 2014 or by Harris et al. (2015). Compared to those studies, three to four additional years of observations, updated and improved data sets with reduced drift, and the fact that nearly all individual data sets indicate ozone increase in the upper stratosphere, all give enhanced confidence. Uncertainties have been reduced, for example for the trend near 2 hectopascals in the 35 to 60 degree latitude bands from about plus or minus 5 percent (2 sigma) in Harris et al. (2015) to less than plus or minus 2 percent (2 sigma). Nevertheless, a thorough analysis of possible drifts and differences between various data sources is still required, as is a detailed attribution of the observed increases to declining ozone-depleting substances and to stratospheric cooling. Ongoing quality observations from multiple independent platforms are key for verifying that recovery of the ozone layer continues as expected.

chemistry climate model simulations↗
NASA NTRS2016

The Description and Validation of a Computationally-Efficient CH4-CO-OH (ECCOHv1.01) Chemistry Module for 3D Model Applications

We present the Efficient CH4-CO-OH (ECCOH) chemistry module that allows for the simulation of the methane, carbon monoxide, and hydroxyl radical (CH4-CO- OH) system, within a chemistry climate model, carbon cycle model, or Earth system model. The computational efficiency of the module allows many multi-decadal sensitivity simulations of the CH4-CO-OH system, which primarily determines the global atmospheric oxidizing capacity. This capability is important for capturing the nonlinear feedbacks of the CH4-CO-OH system and understanding the perturbations to methane, CO, and OH, and the concomitant impacts on climate. We implemented the ECCOH chemistry module in the NASA GEOS-5 atmospheric global circulation model (AGCM), performed multiple sensitivity simulations of the CH4-CO-OH system over 2 decades, and evaluated the model output with surface and satellite data sets of methane and CO. The favorable comparison of output from the ECCOH chemistry module (as configured in the GEOS- 5 AGCM) with observations demonstrates the fidelity of the module for use in scientific research.

carbon cycle model↗
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 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 (AtmOS) 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) chemistry-climate model through detailed comparisons with earlier CALIOP PSC data products and those developed under this proposal.

CALIPSO↗
NASA NTRS2022

Prescribing Stratospheric Chemistry Overestimates Southern Hemisphere Climate Change During Austral Spring in Response to Quadrupled CO2

The interaction of stratospheric chemistry with a changing climate from an abrupt CO2 quadrupling is assessed using the coupled atmosphere–ocean Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM). Two abrupt 4 × CO2 experiments were performed, one with interactive stratospheric chemistry and the other with a prescribed stratospheric chemistry that does not simulate stratospheric ozone response to 4 × CO2. The interactive and prescribed chemistry experiments simulate similar global mean surface temperature change. Nevertheless, interactive chemistry is critical to capture the Southern Hemisphere tropospheric midlatitude jet response to 4 × CO2. When stratospheric ozone response to 4 × CO2 is neglected, GEOSCCM overestimates Southern Hemisphere tropospheric circulation change. This stratospheric chemistry-induced climate impact has large seasonal variability. During the austral spring season September–October–November (SON), prescribed chemistry yields a stronger poleward shift and intensification of the Southern Hemisphere midlatitude tropospheric jet, surface wind stress, and the Southern Ocean meridional overturning circulation than occurs with interactive chemistry. In other seasons interactive and prescribed chemistry have similar effects on the Southern Hemisphere circulation. The seasonality of stratospheric chemistry-induced climate impact is related to the seasonality of Antarctic lower stratospheric ozone response to 4 × CO2. In contrast to this stratospheric ozone response to 4 × CO2, stratospheric ozone recovery from decline of the ozone depleting substances has its largest impact on the Southern Hemisphere tropospheric circulation in austral summer (December–January–February), but no effects in SON. It is found that the different seasonality for these two stratospheric ozone layer change scenarios is related to the different seasonality of tropopause meridional temperature gradient response.

Stratospheric ozone feedback↗
NASA NTRS2013

A 4-D Climatology (1979-2009) of the Monthly Tropospheric Aerosol Optical Depth Distribution over the Mediterranean Region from a Comparative Evaluation and Blending of Remote Sensing and Model Products

Since the 1980s several spaceborne sensors have been used to retrieve the aerosol optical depth (AOD) over the Mediterranean region. In parallel, AOD climatologies coming from different numerical model simulations are now also available, permitting to distinguish the contribution of several aerosol types to the total AOD. In this work, we perform a comparative analysis of this unique multiyear database in terms of total AOD and of its apportionment by the five main aerosol types (soil dust, seasalt, sulfate, black and organic carbon). We use 9 different satellite-derived monthly AOD products: NOAA/AVHRR, SeaWiFS (2 products), TERRA/MISR, TERRA/MODIS, AQUA/MODIS, ENVISAT/MERIS, PARASOL/POLDER and MSG/SEVIRI, as well as 3 more historical datasets: NIMBUS7/CZCS, TOMS (onboard NIMBUS7 and Earth- Probe) and METEOSAT/MVIRI. Monthly model datasets include the aerosol climatology from Tegen et al. (1997), the climate-chemistry models LMDz-OR-INCA and RegCM-4, the multi-model mean coming from the ACCMIP exercise, and the reanalyses GEMS and MACC. Ground-based Level- 2 AERONET AOD observations from 47 stations around the basin are used here to evaluate the model and satellite data. The sensor MODIS (on AQUA and TERRA) has the best average AOD scores over this region, showing a relevant spatio-temporal variability and highlighting high dust loads over Northern Africa and the sea (spring and summer), and sulfate aerosols over continental Europe (summer). The comparison also shows limitations of certain datasets (especially MERIS and SeaWiFS standard products). Models reproduce the main patterns of the AOD variability over the basin. The MACC reanalysis is the closest to AERONET data, but appears to underestimate dust over Northern Africa, where RegCM-4 is found closer to MODIS thanks to its interactive scheme for dust emissions. The vertical dimension is also investigated using the CALIOP instrument. This study confirms differences of vertical distribution between dust aerosols showing a large vertical spread, and other continental and marine aerosols which are confined in the boundary layer. From this compilation, we propose a 4-D blended product from model and satellite data, consisting in monthly time series of 3-D aerosol distribution at a 50 km horizontal resolution over the Euro-Mediterranean marine and continental region for the 2003-2009 period. The product is based on the total AOD from AQUA/MODIS, apportioned into sulfates, black and organic carbon from the MACC reanalysis, and into dust and sea-salt aerosols from RegCM-4 simulations, which are distributed vertically based on CALIOP climatology.We extend the 2003-2009 reconstruction to the past up to 1979 using the 2003-2009 average and applying the decreasing trend in sulfate aerosols from LMDz-OR-INCA, whose AOD trends over Europe and the Mediterranean are median among the ACCMIP models. Finally optical properties of the different aerosol types in this region are proposed from Mie calculations so that this reconstruction can be included in regional climate models for aerosol radiative forcing and aerosol-climate studies.

troposphere↗
NASA NTRS2016

Stratospheric Aerosol--Observations, Processes, and Impact on Climate

Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfatematter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

Kresmer, Stefanie↗
NASA NTRS2018

Implementation of a Comprehensive Ice Crystal Formation Parameterization for Cirrus and Mixed-Phase Clouds in the EMAC Model (Based on MESSy 2.53)

A comprehensive ice nucleation parameterization has been implemented in the global chemistry-climate model EMAC to realistically represent ice crystal number concentrations. The parameterization of Barahona and Nenes (2009, hereafter BN09) allows the treatment of ice nucleation, taking into account the competition for water vapour between homogeneous and heterogeneous nucleation and pre-existing ice crystals in cold clouds. Furthermore, the influence of chemically-heterogeneous, polydisperse aerosols is considered via multiple ice nucleating particle spectra, which are included in the parameterization to compute the heterogeneously formed ice crystals. BN09 has been implemented to operate both in the cirrus and in the mixed-phase regimes. Compared to the standard EMAC results, BN09 produces fewer ice crystals in the upper troposphere but higher ice crystal number concentrations in the middle troposphere, especially in the Northern Hemisphere where ice nucleating mineral dust particles are relatively abundant. The comparison with a climatological data set of aircraft measurements shows that BN09 used in the cirrus regime improves the model results and, therefore, is recommended for future EMAC simulations.

EMAC↗
NASA NTRS2023

Using Regionalized Air Quality Model Performance and Bayesian Maximum Entropy Data Fusion to Map Global Surface Ozone Concentration and Associated Uncertainty

Estimates of ground-level ozone concentrations have been improved through data fusion of observations and atmospheric chemistry models. Our previous global ozone estimates for the Global Burden of Disease study corrected for bias uniformly across continents and then corrected near monitoring stations using the Bayesian Maximum Entropy (BME) framework for data fusion. Here, we use the Regionalized Air Quality Model Performance (RAMP) framework to correct model bias over a much larger spatial range than BME can, accounting for the spatial inhomogeneity of bias and nonlinearity as a function of modeled ozone. RAMP bias correction is applied to a composite of 9 global chemistry-climate models, based on the nearest set of monitors. These estimates are then fused with observations using BME, which matches observations at measurement stations, with the influence of observations declining with distance in space and time. We create global ozone maps for each year from 1990 to 2017 at fine spatial resolution. RAMP is shown to create unrealistic discontinuities due to the spatial clustering of ozone monitors, which we overcome by applying a weighting for RAMP based on the number of monitors nearby. Incorporating RAMP before BME has little effect on model performance near stations, but strongly increases R 2 by 0.15 at locations farther from stations, shown through a checkerboard cross-validation. Corrections to estimates differ based on location in space and time, confirming heterogeneity. We quantify the likelihood of exceeding selected ozone levels, finding that parts of the Middle East, India, and China are most likely to exceed 55 parts per billion (ppb) in 2017. About 96% of the global population was exposed to ozone levels above the World Health Organization guideline of 60 µg m −3 (30 ppb) in 2017. Our annual fine-resolution ozone estimates may be useful for several applications including epidemiology and assessments of impacts on health, agriculture, and ecosystems.

Ozone↗
NASA NTRS2018

Multidecadal Changes in the UTLS Ozone from the MERRA-2 Reanalysis and the GMI Chemistry Model

Long-term changes of ozone in the UTLS (Upper Troposphere / Lower Stratosphere) reflect the response to decreases in the stratospheric concentrations of ozone-depleting substances as well as changes in the stratospheric circulation induced by climate change. To date, studies of UTLS ozone changes and variability have relied mainly on satellite and in-situ observations as well as chemistry-climate model simulations. By comparison, the potential of reanalysis ozone data remains relatively untapped. This is despite evidence from recent studies, including detailed analyses conducted under SPARC (Scalable Processor Architecture) Reanalysis Intercomparison Project (S-RIP), that demonstrate that stratospheric ozone fields from modern atmospheric reanalyses exhibit good agreement with independent data while delineating issues related to inhomogeneities in the assimilated observations. In this presentation, we will explore the possibility of inferring long-term geographically and vertically resolved behavior of the lower stratospheric (LS) ozone from NASA's MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications -2) reanalysis after accounting for the few known discontinuities and gaps in its assimilated input data. This work builds upon previous studies that have documented excellent agreement between MERRA-2 ozone and ozonesonde observations in the LS. Of particular importance is a relatively good vertical resolution of MERRA-2 allowing precise separation of tropospheric and stratospheric ozone contents. We also compare the MERRA-2 LS ozone results with the recently completed 37-year simulation produced using Goddard Earth Observing System in "replay" mode coupled with the GMI (Global Modeling Initiative) chemistry mechanism. Replay mode dynamically constrains the model with the MERRA-2 reanalysis winds, temperature, and pressure. We will emphasize the areas of agreement of the reanalysis and replay and interpret differences between them in the context of our increasing understanding of model transport driven by assimilated winds.

Ozone↗
NASA NTRS2012

Impacts of the Convective Transport Algorithm on Atmospheric Composition and Ozone-Climate Feedbacks in GEOS-CCM

Convective transport is one of the dominant factors in determining the composition of the troposphere. It is the main mechanism for lofting constituents from near-surface source regions to the middle and upper troposphere, where they can subsequently be advected over large distances. Gases reaching the upper troposphere can also be injected through the tropopause and play a subsequent role in the lower stratospheric ozone balance. Convection codes in climate models remain a great source of uncertainty for both the energy balance of the general circulation and the transport of constituents. This study uses the Goddard Earth Observing System Chemistry-Climate Model (GEOS CCM) to perform a controlled experiment that isolates the impact of convective transport of constituents from the direct changes on the atmospheric energy balance. Two multi-year simulations are conducted. In the first, the thermodynamic variable, moisture, and all trace gases are transported using the multi-plume Relaxed-Arakawa-Schubert (RAS) convective parameterization. In the second simulation, RAS impacts the thermodynamic energy and moisture in this standard manner, but all other constituents are transported differently. The accumulated convective mass fluxes (including entrainment and detrainment) computed at each time step of the GCM are used with a diffusive (bulk) algorithm for the vertical transport, which above all is less efficient at transporting constituents from the lower to the upper troposphere. Initial results show the expected differences in vertical structure of trace gases such as carbon monoxide, but also show differences in lower stratospheric ozone, in a region where it can potentially impact the climate state of the model. This work will investigate in more detail the impact of convective transport changes by comparing the two simulations over many years (1996-2010), focusing on comparisons with observed constituent distributions and similarities and differences of patterns of inter-annual variability caused by the convective transport algorithm. In particular, the impact on lower stratospheric composition will be isolated and the subsequent feedbacks of ozone on the climate forcing and tropopause structure will be assessed.

Pawson, S.↗
NASA NTRS2014

Science Accomplishments from a Decade of Aura OMI/MLS Tropospheric Ozone Measurements

Measurements of tropospheric ozone from combined Aura OMI and MLS instruments have yielded a large number of new and important science discoveries over the last decade. These discoveries have generated a much greater understanding of biomass burning, lightning NO, and stratosphere-troposphere exchange sources of tropospheric ozone, ENSO dynamics and photochemistry, intra-seasonal variability-Madden-Julian Oscillation including convective transport, radiative forcing, measuring ozone pollution from space, improvements to ozone retrieval algorithms, and evaluation of chemical-transport and chemistry-climate models. The OMI-MLS measurements have been instrumental in giving us better understanding of the dynamics and chemistry involving tropospheric ozone and the many drivers affecting the troposphere in general. This discussion will provide an overview focusing on our main science results.

ENSO↗
NASA NTRS2018

Biosignature Anisotropy Modeled on Temperate Tidally Locked M-Dwarf Planets

A planet’s atmospheric constituents (e.g., O2, O3, H2Ov, CO2, CH4, and N2O) can provide clues to its surface habitability, and may offer biosignature targets for remote life detection efforts. The plethora of rocky exoplanets found by recent transit surveys (e.g., the Kepler mission) indicates that potentially habitable systems orbiting K- and M-dwarf stars may have very different orbital and atmospheric characteristics than Earth. To assess the physical distribution and observational prospects of various biosignatures and habitability indicators, it is important to understand how they may change under different astrophysical and geophysical configurations, and to simulate these changes with models that include feedbacks between different subsystems of a planet’s climate. Here we use a three-dimensional (3D) Chemistry–Climate model (CCM) to study the effects of changes in stellar spectral energy distribution (SED), stellar activity, and planetary rotation on Earth analogs and tidally locked planets. Our simulations show that, apart from shifts in stellar SEDs and UV radiation, changes in illumination geometry and rotation-induced circulation can influence the global distribution of atmospheric biosignatures. We find that the stratospheric day-to-nightside mixing ratio differences on tidally locked planets remain low (<20%) across the majority of the canonical biosignatures. Interestingly, however, secondary photosynthetic biosignatures (e.g., C2H6S) show much greater (∼67%) day-to-nightside differences, and point to regimes in which tidal locking could have observationally distinguishable effects on phase curve, transit, and secondary eclipse measurements. Overall, this work highlights the potential and promise for 3D CCMs to study the atmospheric properties and habitability of terrestrial worlds.

Chen, Howard↗
NASA NTRS2020

Influence of Dynamic Ozone Dry Deposition on Ozone Pollution

Identifying the contributions of chemistry and transport to observed ozone pollution using regional‐to‐global models relies on accurate representation of ozone dry deposition. We use a recently developed configuration of the NOAA GFDL chemistry‐climate model – in which the atmosphere and land are coupled through dry deposition—to investigate the influence of ozone dry deposition on ozone pollution over northern midlatitudes. In our model, deposition pathways are tied to dynamic terrestrial processes, such as photosynthesis and water cycling through the canopy and soil. Small increases in winter deposition due to more process‐based representation of snow and deposition to surfaces reduce hemispheric‐scale ozone throughout the lower troposphere by 5–12 ppb, improving agreement with observations relative to a simulation with the standard configuration for ozone dry deposition. Declining snow cover by the end of the 21st‐century tempers the previously identified influence of rising methane on winter ozone. Dynamic dry deposition changes summer surface ozone by −4 to +7 ppb. While previous studies emphasize the importance of uptake by plant stomata, new diagnostic tracking of depositional pathways reveals a widespread impact of nonstomatal deposition on ozone pollution. Daily variability in both stomatal and nonstomatal deposition contribute to daily variability in ozone pollution. Twenty‐first century changes in summer deposition result from a balance among changes in individual pathways, reflecting differing responses to both high carbon dioxide (through plant physiology versus biomass accumulation) and water availability. Our findings highlight a need for constraints on the processes driving ozone dry deposition to test representation in regional‐to‐global models.

dry deposition↗
NASA NTRS2023

Comparison Between Ozone Column Depths and Methane Lifetimes Computed By One- and Three-Dimensional Models at Different Atmospheric O(2) Levels

The calculation of ozone column depth as a function of atmospheric O2concentration has been performed multiple times over the past 40 years using one-dimensional (1-D) photochemical models. Several of these calculations [1–3] have been done by the Kasting group. We refer to the current version of that model as the‘standard’1-D model (see §2). Recently, Cooke et al., henceforth C22 ,performed a similar calculation using a three-dimensional (3-D) coupled chemistry-climate model (WACCM6). They found substantially lower ozone column depths at lower pO2levels. For example, at0.01 times the present atmospheric level (PAL) of O(2), Segura et al. calculated 124 Dobson units(DU), whereas C22 calculated a mean column depth of just 66 DU—almost a factor of two lower. This comparison is shown in figure 1. C22 argued, correctly, that 3-D models should be able to do a better job on this problem than 1-D models because ozone column depths are affected by atmospheric transport, e.g. the Brewer–Dobson circulation in the stratosphere that blows ozone from the tropics towards the poles, as well as vertical transport that carries ozone downward from the stratosphere to the troposphere. Meridional transport is absent in 1-D models, and vertical transport is fixed, so model geometry almost certainly contributes to the observed discrepancies in ozone column depth. The 3-D model also has a variable tropopause height (higher at the equator, lower towards the poles), which is difficult to simulate in one dimension.

Atmospheric chemistry↗
NASA NTRS2003

Climate Impacts on Tropospheric Ozone and Hydroxyl

Climate change may influence tropospheric ozone and OH via several main pathways: (1) altering chemistry via temperature and humidity changes, (2) changing ozone and precursor sources via surface emissions, stratosphere-troposphere exchange, and light- ning, and (3) affecting trace gas sinks via the hydrological cycle and dry deposition. We report results from a set of coupled chemistry-climate model simulations designed to systematically study these effects. We compare the various effects with one another and with past and projected future changes in anthropogenic and natural emissions of ozone precursors. We find that white the overall impact of climate on ozone is probably small compared to emission changes, some significant seasonal and regional effects are apparent. The global effect on hydroxyl is quite large, however, similar in size to the effect of emission changes. Additionally, we show that many of the chemistry-climate links that are not yet adequately modeled are potentially important.

Shindell, Drew T.↗
NASA NTRS2010

Finding the Missing Stratospheric Br(sub y): A Global Modeling Study of CHBr3 and CH2Br2

Recent in situ and satellite measurements suggest a contribution of ~5 pptv to stratospheric inorganic bromine from short-lived bromocarbons. We conduct a modeling study of the two most important short-lived bromocarbons, bromoform (CHBr3) and dibromomethane (CH2Br2), with the Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) to account for this missing stratospheric bromine. We derive a "top-down" emission estimate of CHBr3 and CH2Br2 using airborne measurements in the Pacific and North American troposphere and lower stratosphere obtained during previous NASA aircraft campaigns. Our emission estimate suggests that to reproduce the observed concentrations in the free troposphere, a global oceanic emission of 425 Gg Br yr(exp -1) for CHBr3 and 57 Gg Br yr(exp -l) for CH2Br2 is needed, with 60% of emissions from open ocean and 40% from coastal regions. Although our simple emission scheme assumes no seasonal variations, the model reproduces the observed seasonal variations of the short-lived bromocarbons with high concentrations in winter and low concentrations in summer. This indicates that the seasonality of short-lived bromocarbons is largely due to seasonality in their chemical loss and transport. The inclusion of CHBr3 and CH2Br2 contributes ~5 pptv bromine throughout the stratosphere. Both the source gases and inorganic bromine produced from source gas degradation (Br~SLS) in the troposphere are transported into the stratosphere, and are equally important. Inorganic bromine accounts for half (2.5 pptv) of the bromine from the inclusion of CHBr3 and CHzBr2 near the tropical tropopause and its contribution rapidly increases to ~ 100% as altitude increases. More than 85% of the wet scavenging of Br(sub y)(sup VSLS) occurs in large-scale precipitation below 500 hPa. Our sensitivity study with wet scavenging in convective updrafts switched off suggests that Br(sub y)(sup SLS) in the stratosphere is not sensitive to convection. Convective scavenging only accounts for ~0.2 pptv (4%) difference in inorganic bromine delivered to the stratosphere.

Liang, Q.↗
NASA NTRS2010

Multi-Model Assessment of the Factors Driving the Ozone Evolution Over the 21st Century

The evolution of ozone from 1960 to 2100 is examined in simulations from fourteen chemistry-climate models. There is general agreement among the models at the broadest levels, with all showing column ozone decreasing at all latitudes from 1960 to around 2000, then increasing at all latitudes over the first half of the 21 st century (21 C), and latitudinal variations in the rate of increase and date of return to historical values. In the second half of the century, ozone is projected to carry on increasing, level off or even decrease depending on the latitude, resulting in variable dates of return to historical values at latitudes where column ozone has declined below those levels. Separation into partial column above and below 20 hPa reveals that these latitudinal differences are almost completely due to differences in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21 C and returns to 1960 levels before the end of the century, although there is a spread among the models in dates that ozone returns to historical values. Using multiple linear regression the upper stratospheric ozone increase comes from almost equal contributions due to decrease in halogens and cooling from increased greenhouse gas concentrations. The evolution of lower stratospheric ozone differs with latitude. In the tropical lower stratosphere an increase in tropical upwelling causes a steady decrease in ozone through the 21C, and total column ozone does not return to 1960 levels in all models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21 C and returns to 1960 levels. For all models there is an earlier return for ozone to historical levels in the northern hemisphere. This is thought to be due to interhemispheric differences in transport.

Oman, L.↗