Emergence of healing in the Antarctic ozone layer

Industrial chlorofluorocarbons that cause ozone depletion have been phased out under the Montreal Protocol. A chemically driven increase in polar ozone (or “healing”) is expected in response to this historic agreement. Observations and model calculations together indicate that healing of the Antarctic ozone layer has now begun to occur during the month of September. Fingerprints of September healing since 2000 include (i) increases in ozone column amounts, (ii) changes in the vertical profile of ozone concentration, and (iii) decreases in the areal extent of the ozone hole. Along with chemistry, dynamical and temperature changes have contributed to the healing but could represent feedbacks to chemistry. Volcanic eruptions have episodically interfered with healing, particularly during 2015, when a record October ozone hole occurred after the Calbuco eruption.National Science Foundation (U.S.) (FESD Grant OCE-1338814)National Science Foundation (U.S.). Atmospheric Chemistry Program (Grant 1539972

Towards the definition of a solar forcing dataset for CMIP7

The solar forcing prepared for Phase 6 of the Coupled Model Intercomparison Project (CMIP6) has been used extensively in climate model experiments and has been tested in various intercomparison studies. Recently, an International Space Science Institute (ISSI) working group has been established to revisit the solar forcing recommendations, based on the lessons learned from CMIP6, and to assess new datasets that have become available, in order to define a road map for building a revised and extended historical solar forcing dataset for the upcoming Phase 7 of CMIP. This paper identifies the possible improvements required and outlines a strategy to address them in the planned new solar forcing dataset. Proposed major changes include the adoption of the new Total and Spectral Solar Irradiance Sensor (TSIS-1) solar reference spectrum for solar spectral irradiance and an improved description of top-of-the-atmosphere energetic electron fluxes, as well as their reconstruction back to 1850 by means of geomagnetic proxy data. In addition, there is an urgent need to consider the proposed updates in the ozone forcing dataset in order to ensure a self-consistent solar forcing in coupled models without interactive chemistry. Regarding future solar forcing, we propose consideration of stochastic ensemble forcing scenarios, ideally in concert with other natural forcings, in order to allow for realistic projections of natural forcing uncertainties

On the Stratospheric Chemistry of Midlatitude Wildfire Smoke

Massive Australian wildfires lofted smoke directly into the stratosphere in the austral summer of 2019/20. The smoke led to increases in optical extinction throughout the midlatitudes of the southern hemisphere that rivalled substantial volcanic perturbations. Previous studies have assumed that the smoke became coated with sulfuric acid and water and would deplete the ozone layer through heterogeneous chemistry on those surfaces, as is routinely observed following volcanic enhancements of the stratospheric sulfate layer. Here, observations of extinction and reactive nitrogen species from multiple independent satellites that sampled the smoke region are compared to one another and to model calculations. The data display a strong decrease in reactive nitrogen concentrations with increased aerosol extinction in the stratosphere, which is a known fingerprint for key heterogeneous chemistry on sulfate/H2O particles (specifically the hydrolysis of N2O5 to form HNO3). This chemical shift affects not only reactive nitrogen but also chlorine and reactive hydrogen species and is expected to cause midlatitude ozone layer depletion. Comparison of the model ozone to observations suggests that N2O5 hydrolysis contributed to reduced ozone, but additional chemical and/or dynamical processes are also important. These findings suggest that if wildfire smoke injection into the stratosphere increases sufficiently in frequency and magnitude as the world warms due to climate change, ozone recovery under the Montreal Protocol could be impeded, at least sporadically. Modeled austral midlatitude total ozone loss was about 1% in March 2020, which is significant compared to expected ozone recovery of about 1% per decade

Asian Monsoon Transport of Pollution to the Stratosphere

Transport of air from the troposphere to the stratosphere occurs primarily in the tropics, associated with the ascending branch of the Brewer-Dobson circulation. Here we identify the transport of air masses from the surface, through the Asian monsoon, and deep into the stratosphere, using satellite observations of hydrogen cyanide (HCN), a tropospheric pollutant produced in biomass burning. A key factor in this identification is that HCN has a strong sink from contact with the ocean; much of the air in the tropical upper troposphere is relatively depleted in HCN, and hence broad tropical upwelling cannot be the main source for the stratosphere. The monsoon circulation provides an effective pathway for pollution from Asia, India and Indonesia to enter the global stratosphere

Monsoon circulations and tropical heterogeneous chlorine chemistry in the stratosphere

Model simulations presented in this paper suggest that transport processes associated with the summer monsoons bring increased abundances of hydrochloric acid into contact with liquid sulfate aerosols in the cold tropical lowermost stratosphere, leading to heterogeneous chemical activation of chlorine species. The calculations indicate that the spatial and seasonal distributions of chlorine monoxide and chlorine nitrate near the monsoon regions of the northern hemisphere tropical and subtropical lowermost stratosphere could provide indicators of heterogeneous chlorine processing. In the model, these processes impact the local ozone budget and decrease ozone abundances, implying a chemical contribution to longer-term northern tropical ozone profile changes at 16-19 km

Trend differences in lower stratospheric water vapour between Boulder and the zonal mean and their role in understanding fundamental observational discrepancies

Trend estimates with different signs are reported in the literature for lower stratospheric water vapour considering the time period between the late 1980s and 2010. The NOAA (National Oceanic and Atmospheric Administration) frost point hygrometer (FPH) observations at Boulder (Colorado, 40.0° N, 105.2° W) indicate positive trends (about 0.1 to 0.45 ppmv decade⁻¹). On the contrary, negative trends (approximately −0.2 to −0.1 ppmv decade⁻¹) are derived from a merged zonal mean satellite data set for a latitude band around the Boulder latitude. Overall, the trend differences between the two data sets range from about 0.3 to 0.5 ppmv decade⁻¹, depending on altitude. It has been proposed that a possible explanation for these discrepancies is a different temporal behaviour at Boulder and the zonal mean. In this work we investigate trend differences between Boulder and the zonal mean using primarily simulations from ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg/Modular Earth Submodel System) Atmospheric Chemistry (EMAC), WACCM (Whole Atmosphere Community Climate Model), CMAM (Canadian Middle Atmosphere Model) and CLaMS (Chemical Lagrangian Model of the Stratosphere). On shorter timescales we address this aspect also based on satellite observations from UARS/HALOE (Upper Atmosphere Research Satellite/Halogen Occultation Experiment), Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding) and Aura/MLS (Microwave Limb Sounder). Overall, both the simulations and observations exhibit trend differences between Boulder and the zonal mean. The differences are dependent on altitude and the time period considered. The model simulations indicate only small trend differences between Boulder and the zonal mean for the time period between the late 1980s and 2010. These are clearly not sufficient to explain the discrepancies between the trend estimates derived from the FPH observations and the merged zonal mean satellite data set. Unless the simulations underrepresent variability or the trend differences originate from smaller spatial and temporal scales than resolved by the model simulations, trends at Boulder for this time period should also be quite representative for the zonal mean and even other latitude bands. Trend differences for a decade of data are larger and need to be kept in mind when comparing results for Boulder and the zonal mean on this timescale. Beyond that, we find that the trend estimates for the time period between the late 1980s and 2010 also significantly differ among the simulations. They are larger than those derived from the merged satellite data set and smaller than the trend estimates derived from the FPH observations

Simulation of polar ozone depletion: An update

We evaluate polar ozone depletion chemistry using the specified dynamics version of the Whole Atmosphere Community Climate Model for the year 2011. We find that total ozone depletion in both hemispheres is dependent on cold temperatures (below 192 K) and associated heterogeneous chemistry on polar stratospheric cloud particles. Reactions limited to warmer temperatures above 192 K, or on binary liquid aerosols, yield little modeled polar ozone depletion in either hemisphere. An imposed factor of three enhancement in stratospheric sulfate increases ozone loss by up to 20 Dobson unit (DU) in the Antarctic and 15 DU in the Arctic in this model. Such enhanced sulfate loads are similar to those observed following recent relatively small volcanic eruptions since 2005 and imply impacts on the search for polar ozone recovery. Ozone losses are strongly sensitive to temperature, with a test case cooler by 2 K producing as much as 30 DU additional ozone loss in the Antarctic and 40 DU in the Arctic. A new finding of this paper is the use of the temporal behavior and variability of ClONO[subscript 2] and HCl as indicators of the efficacy of heterogeneous chemistry. Transport of ClONO[subscript 2] from the southern subpolar regions near 55–65°S to higher latitudes near 65–75°S provides a flux of NO[subscript x] from more sunlit latitudes to the edge of the vortex and is important for ozone loss in this model. Comparisons between modeled and observed total column and profile ozone perturbations, ClONO[subscript 2] abundances, and the rate of change of HCl bolster confidence in these conclusions.National Science Foundation (U.S.) (NSF FESD grant OCE-1338814)National Science Foundation (U.S.) (grant, NSF Atmospheric Chemistry Division

An Arctic ozone hole in 2020 if not for the Montreal Protocol

Abstract. Without the Montreal Protocol, the already extreme Arctic ozone losses in the boreal spring of 2020 would be expected to have produced an Antarctic-like ozone hole, based upon simulations performed using the specified dynamics version of the Whole Atmosphere Community Climate Model (SD-WACCM) and using an alternate emission scenario of 3.5 % growth in ozone-depleting substances from 1985 onwards. In particular, we find that the area of total ozone below 220 DU (Dobson units), a standard metric of Antarctic ozone hole size, would have covered about 20 million km2. Record observed local lows of 0.1 ppmv (parts per million by volume) at some altitudes in the lower stratosphere seen by ozonesondes in March 2020 would have reached 0.01, again similar to the Antarctic. Spring ozone depletion would have begun earlier and lasted longer without the Montreal Protocol, and by 2020, the year-round ozone depletion would have begun to dramatically diverge from the observed case. This extreme year also provides an opportunity to test parameterizations of polar stratospheric cloud impacts on denitrification and, thereby, to improve stratospheric models of both the real world and alternate scenarios. In particular, we find that decreasing the parameterized nitric acid trihydrate number density in SD-WACCM, which subsequently increases denitrification, improves the agreement with observations for both nitric acid and ozone. This study reinforces that the historically extreme 2020 Arctic ozone depletion is not cause for concern over the Montreal Protocol's effectiveness but rather demonstrates that the Montreal Protocol indeed merits celebration for avoiding an Arctic ozone hole.</jats:p

Atmospheric Chemistry Signatures of an Equatorially Symmetric Matsuno–Gill Circulation Pattern

© 2020 American Meteorological Society. For information regarding reuse of this content and general copyright information, consult the AMS Copyright Policy (www.ametsoc.org/PUBSReuseLicenses). Matsuno-Gill circulations have been widely studied in tropical meteorology, but their impact on stratospheric chemistry has seldom been explicitly evaluated. This study demonstrates that, in a model nudged to reanalysis, anticyclonic Rossby wave gyres that form near the tropopause as a result of equatorially symmetric heating in the troposphere provide a dynamical mechanism to influence tropical and subtropical atmospheric chemistry during near-equinox months. The anticyclonic flow entrains extratropical air from higher latitudes into the deep tropics of both hemispheres and induces cooling in the already cold upper-troposphere/lower-stratosphere (UTLS) region. Both of these aspects of the circulation allow heterogeneous chlorine activation on sulfuric acid aerosols to proceed rapidly, primarily via the HCl 1 ClONO2 reaction. Precipitation rates and heating rates from reanalysis are shown to be consistent with these heating and circulation response patterns in the months of interest. This study analyzes specified dynamics simulations from the Whole Atmosphere Community Climate Model (SD-WACCM) with and without tropical heterogeneous chemistry to demonstrate that these circulations influence substantially the distributions of, for example, NO2 and ClO in the UTLS tropics and subtropics of both hemispheres. This provides a previously unrecognized dynamical influence on the spatial structures of atmospheric composition changes in the UTLS during near-equinox months