Transport and modeling of stratospheric inorganic chlorine

International audienceCorrectly modeling stratospheric inorganic chlorine (Cly) is crucial for modeling the past and future evolution of stratospheric ozone. However, comparisons of the chemistry climate models used in the latest international assessment of stratospheric ozone depletion have shown large differences in the modeled Cly, with these differences explaining differences in the simulated evolution of ozone over the next century. Here in, we examine the role of transport in determining the simulated Cly using three simulations from the same off-line chemical transport model that have the same lower tropospheric boundary conditions and the same chemical solver, but differing resolution and/or meteorological fields. These simulations show that transport plays a key role in determining the Cly distribution, and that Cly depends on both the time scales and pathways of transport. The time air spends in the stratosphere (e.g., the mean age) is an important transport factor determining stratospheric Cly, but the relationship between mean age and Cly is not simple. Lower stratospheric Cly depends on the fraction of air that has been in the upper stratosphere, and transport differences between models having the same mean age can result in differences in the fraction of organic chlorine converted into Cly. Differences in transport pathways result in differences in vertical profiles of CFCs, and comparisons of observed and modeled CFC profiles provides a stringent test of transport pathways in models

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

Small scale structure and mixing at the edge of the Antarctic vortex

Small scale correlations and patterns in the chemical tracers measured from the NASA ER-2 aircraft in the 1987 AAOE campaign can be used to investigate the structure of the edge of the polar vortex and the chemically perturbed region within it. Examples of several types of transport processes can be found in the data. Since ClO and O3 have similar vertical gradients and opposite horizontal gradients near the chemically perturbed region, the correlation between ClO and O3 can be used to study the extent of horizontal transport at the edge of the chemically perturbed region. Horizontal transport dominates the correlation for a latitude band up to 4 degrees on each side of the boundary. This implies a transition zone containing a substantial fraction of the mass of the total polar vortex. Similar horizontal transport can be seen in other tracers as well. It has not been possible to distinguish reversible transport from irreversible mixing. One manifestation of the horizontal transport is that the edge of the chemically perturbed region is often layered rather than a vertical curtain. This can be seen from the frequent reversed vertical gradients of NO2, caused by air with high NO2 overlapping layers with lower mixing ratios. Water and NO2 are positively correlated within the chemically perturbed region. This is the opposite sign to the correlation in the unperturbed stratosphere. The extent of the positive correlation is too great to be attributed solely to horizontal mixing. Instead, it is hypothesized that dehydration and descent are closely connected on a small scale, possibly due to radiative cooling of the clouds that also cause ice to fall to lower altitudes

Sensitivity of stratospheric inorganic chlorine to differences in transport

International audienceCorrectly modeling stratospheric inorganic chlorine (Cly) is crucial for modeling the past and future evolution of stratospheric ozone. However, comparisons of the chemistry climate models used in the latest international assessment of stratospheric ozone depletion have shown large differences in the modeled Cly, with these differences explaining many of the differences in the simulated evolution of ozone over the next century. Here in, we examine the role of transport in determining the simulated Cly using three simulations from the same off-line chemical transport model that have the same lower tropospheric boundary conditions and the same chemical solver, but differing resolution and/or meteorological fields. These simulations show that transport plays a key role in determining the Cly distribution, and that Cly depends on both the time scales and pathways of transport. The time air spends in the stratosphere (e.g., the mean age) is an important transport factor determining stratospheric Cly, but the relationship between mean age and Cly is not simple. Lower stratospheric Cly depends on the fraction of air that has been in the upper stratosphere, and transport differences between models having the same mean age can result in differences in the fraction of organic chlorine converted into Cly. Differences in transport pathways result in differences in vertical profiles of CFCs, and comparisons of observed and modeled CFC profiles provide a stringent test of transport pathways in models

The Impact of New Estimates of Mixing Ratio and Flux-based Halogen Scenarios on Ozone Evolution

The evolution of ozone in the 21st century has been shown to be mainly impacted by the halogen emissions scenario and predicted changes in the circulation of the stratosphere. New estimates of mixing ratio and flux-based emission scenarios have been produced from the SPARC Lifetime Assessment 2013. Simulations using the Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM) are conducted using this new A1 2014 halogen scenario and compared to ones using the A1 2010 scenario. This updated version of GEOSCCM includes a realistic representation of the Quasi-Biennial Oscillation and improvements related to the break up of the Antarctic polar vortex. We will present results of the ozone evolution over the recent past and 21st century to the A1 2010, A1 2014 mixing ratio, and an A1 2014 flux-based halogen scenario. Implications of the uncertainties in these estimates as well as those from possible circulation changes will be discussed

Impact of the North Atlantic Oscillation on transatlantic flight routes and clear-air turbulence

The variation of wind-optimal transatlantic flight routes and their turbulence potential is investigated to understand how upper-level winds and large-scale flow patterns can affect the efficiency and safety of long-haul flights. In this study, the wind-optimal routes (WORs) that minimize the total flight time by considering wind variations are modeled for flights between John F. Kennedy International Airport (JFK) in New York, New York, and Heathrow Airport (LHR) in London, United Kingdom, during two distinct winter periods of abnormally high and low phases of North Atlantic Oscillation (NAO) teleconnection patterns. Eastbound WORs approximate the JFK–LHR great circle (GC) route following northerly shifted jets in the +NAO period. Those WORs deviate southward following southerly shifted jets during the −NAO period, because eastbound WORs fly closely to the prevailing westerly jets to maximize tailwinds. Westbound WORs, however, spread meridionally to avoid the jets near the GC in the +NAO period to minimize headwinds. In the −NAO period, westbound WORs are north of the GC because of the southerly shifted jets. Consequently, eastbound WORs are faster but have higher probabilities of encountering clear-air turbulence than westbound ones, because eastbound WORs are close to the jet streams, especially near the cyclonic shear side of the jets in the northern (southern) part of the GC in the +NAO (−NAO) period. This study suggests how predicted teleconnection weather patterns can be used for long-haul strategic flight planning, ultimately contributing to minimizing aviation’s impact on the environmen

Understanding Differences in Upper Stratospheric Ozone Response to Changes in Chlorine and Temperature as Computed Using CCMVal Models

Projections of future ozone levels are made using models that couple a general circulation model with a representation of atmospheric photochemical processes, allowing interactions among photochemical processes, radiation, and dynamics. Such models are known as chemistry and climate models (CCMs). Although developed from common principles and subject to the same boundary conditions, simulated ozone time series vary for projections of changes in ozone depleting substances (ODSs) and greenhouse gases. In the upper stratosphere photochemical processes control ozone level, and ozone increases as ODSs decrease and temperature decreases due to greenhouse gas increase. Simulations agree broadly but there are quantitative differences in the sensitivity of ozone to chlorine and to temperature. We obtain insight into these differences in sensitivity by examining the relationship between the upper stratosphere annual cycle of ozone and temperature as produced by a suite of models. All simulations conform to expectation in that ozone is less sensitive to temperature when chlorine levels are highest because chlorine catalyzed loss is nearly independent of temperature. Differences in sensitivity are traced to differences in simulated temperature, ozone and reactive nitrogen when chlorine levels are close to background. This work shows that differences in the importance of specific processes underlie differences in simulated sensitivity of ozone to composition change. This suggests a) the multi-model mean is not a best estimate of the sensitivity of upper ozone to changes in ODSs and temperature; b) the spread of values is not an appropriate measure of uncertainty

Reducing Uncertainty in Chemistry Climate Model Predictions of Stratospheric Ozone

Chemistry climate models (CCMs) are used to predict the future evolution of stratospheric ozone as ozone-depleting substances decrease and greenhouse gases increase, cooling the stratosphere. CCM predictions exhibit many common features, but also a broad range of values for quantities such as year of ozone-return-to-1980 and global ozone level at the end of the 21st century. Multiple linear regression is applied to each of 14 CCMs to separate ozone response to chlorine change from that due to climate change. We show that the sensitivity of lower atmosphere ozone to chlorine change deltaO3/deltaCly is a near linear function of partitioning of total inorganic chlorine (Cly) into its reservoirs; both Cly and its partitioning are controlled by lower atmospheric transport. CCMs with realistic transport agree with observations for chlorine reservoirs and produce similar ozone responses to chlorine change. After 2035 differences in response to chlorine contribute little to the spread in CCM results as the anthropogenic contribution to Cly becomes unimportant. Differences among upper stratospheric ozone increases due to temperature decreases are explained by differences in ozone sensitivity to temperature change deltaO3/deltaT due to different contributions from various ozone loss processes, each with their own temperature dependence. In the lower atmosphere, tropical ozone decreases caused by a predicted speed-up in the Brewer-Dobson circulation may or may not be balanced by middle and high latitude increases, contributing most to the spread in late 21st century predictions

Evaluation of MERRA-2-Based Ozone Profile Simulations with the Global Ozonesonde Network

Chemical transport model (CTM) hindcasts of ozone (O3) are useful for filling in observational gaps and providing context for observed O3 variability and trends. We use global networks of ozonesonde stations to evaluate the O3 profiles in two simulations running versions of the NASA Global Modeling Initiative (GMI) chemical mechanism. Both simulations are tied to the NASA Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) meteorological reanalysis: 1) The GMI CTM, and 2) The MERRA-2 GMI Replay (M2 GMI). Both simulations start in 1980, and are compared against >50,000 ozonesonde profiles from 37 global stations from the tropics to the poles. The comparisons allow us to evaluate how the Replay technique affects modeled O3 distribution, how an updated chemical mechanism in the GMI CTM affects simulated tropospheric O3 amounts, and how observed O3 distributions compare to the full set of model output. In general, M2 GMI O3 is ~10% higher than in the GMI CTM, and shows global near-surface and tropical upper troposphere/lower stratosphere (UT/LS) high biases. The updated chemical mechanism in the GMI CTM reduces these high biases. Both simulations show similar negative biases in tropical free-tropospheric O3, especially during typical biomass burning seasons. The simulations are highly-correlated with ozonesonde measurements, particularly in the UT/LS (r > 0.8), showing the ability of MERRA-2 to capture tropopause height variations. Both simulations show improved correlations with ozonesonde data and smaller O3 biases in recent years. We expect to use the sonde/model comparisons to diagnose causes of disagreement and to gauge the feasibility of calculating multidecadal O3 trends from the model output