The Impact of Ozone-Depleting Substances on Tropical Upwelling, as Revealed by the Absence of Lower-Stratospheric Cooling since the Late 1990s
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The new generation GISS climate model includes fully interactive chemistry related to ozone in historical and future simulations, and interactive methane in future simulations. Evaluation of ozone, its tropospheric precursors, and methane shows that the model captures much of the largescale spatial structure seen in recent observations. While the model is much improved compared with the previous chemistry-climate model, especially for ozone seasonality in the stratosphere, there is still slightly too rapid stratospheric circulation, too little stratosphere-to-troposphere ozone flux in the Southern Hemisphere and an Antarctic ozone hole that is too large and persists too long. Quantitative metrics of spatial and temporal correlations with satellite datasets as well as spatial autocorrelation to examine transport and mixing are presented to document improvements in model skill and provide a benchmark for future evaluations. The difference in radiative forcing (RF) calculated using modeled tropospheric ozone versus tropospheric ozone observed by TES is only 0.016W/sq. m. Historical 20th Century simulations show a steady increase in whole atmosphere ozone RF through 1970 after which there is a decrease through 2000 due to stratospheric ozone depletion. Ozone forcing increases throughout the 21st century under RCP8.5 owing to a projected recovery of stratospheric ozone depletion and increases in methane, but decreases under RCP4.5 and 2.6 due to reductions in emissions of other ozone precursors. RF from methane is 0.05 to 0.18W/ sq. m higher in our model calculations than in the RCP RF estimates. The surface temperature response to ozone through 1970 follows the increase in forcing due to tropospheric ozone. After that time, surface temperatures decrease as ozone RF declines due to stratospheric depletion. The stratospheric ozone depletion also induces substantial changes in surface winds and the Southern Ocean circulation, which may play a role in a slightly stronger response per unit forcing during later decades. Tropical precipitation shifts south during boreal summer from 1850 to 1970, but then shifts northward from 1970 to 2000, following upper tropospheric temperature gradients more strongly than those at the surface.
Vertical profiles of ozone and temperature have been measured at McMurdo Station, Antarctica, during the springs of 1986 to 1991, roughly every two days from 25 August to 31 October. Comparisons of temporal histories and average vertical structure for these years reveals some striking consistency in the ozone depletion process. Ozone depletion generally begins in early September, and with a half-life of 20-30 days, reaches its maximum in mid-October. The depletion occurs almost exclusively between 12 and 20 km. At the time of maximum depletion total ozone has been decreased roughly 40 percent while ozone between 12 and 20 km has been reduced 80 percent. Recovery generally begins in late October with the influx, above 20 km, of ozone rich air from the lower latitudes. From this record the worst years for ozone depletion were 1987, 1989, and 1990. A new region of ozone depletion, below 12 km, was observed in 1991, coinciding with the entrainment of a volcanic cloud into the polar vortex.
The Montreal protocol on Substances that Deplete the ozone Layer has been hailed as the most successful environmental treaty ever (https://www.unenvironment.org/news-and-stories/story/montreal-protocol-triumph-treaty). Yet, although our main concern about ozone depletion is the subsequent increase in harmful solar UV radiation at the earth’s surface, no studies to date have demonstrated its effectiveness in that regard. Here we use long-term UV Index (UVI) data derived from high-quality UV spectroradiometer measurements to demonstrate its success in curbing increases in UV radiation. Without this landmark agreement, UVi values would have increased at mid-latitude locations by approximately 20% between the early 1990s and today and would approximately quadruple at mid-latitudes by 2100. In contrast, an analysis of UVI data from multiple clean-air sites shows that maximum daily UVI values have remained essentially constant over the last ~20 years in all seasons, and may even have decreased slightly in the southern hemisphere, especially in Antarctica, where effects of ozone depletion were larger. Reconstructions of the UVi from total ozone data show evidence of increasing UVI levels in the 1980s, but unfortunately, there are no high-quality UV measurements available prior to the early 1990s to confirm these increases with direct observations.
Climate in the Southern Hemisphere (SH) has undergone significant changes in recent decades. These changes are closely linked to the shift of the Southern Annular Mode (SAM) towards its positive polarity, which is driven primarily by Antarctic ozone depletion. There is growing evidence that Antarctic ozone depletion has significant impacts on Southern Ocean circulation change. However, it is poorly understood whether and how ocean feedback might impact the SAM and climate change in the SH atmosphere. This outstanding science question is investigated using the Goddard Earth Observing System Coupled Atmosphere-Ocean-Chemistry Climate Model(GEOS-AOCCM).We perform ensemble simulations of the recent past (1960-2010) with and without the interactive ocean. For simulations without the interactive ocean, we use sea surface temperatures and sea ice concentrations produced by the interactive ocean simulations. The differences between these two ensemble simulations quantify the effects of atmosphere-ocean coupling. We will investigate the impacts of atmosphere-ocean coupling on stratospheric processes such as Antarctic ozone depletion and Antarctic polar vortex breakup. We will address whether ocean feedback affects Rossby wave generation in the troposphere and wave propagation into the stratosphere. Another focuson this study is to assess how ocean feedback might affect the tropospheric SAM response to Antarctic ozone depletion
Ozone column amounts obtained by the total ozone mapping spectrometer (TOMS) in the southern polar region are analyzed during late austral winter and spring (days 240-300) for 1980-1991 using area-mapping techniques and area-weighted vortex averages. The vortex here is defined using the -50 PVU (1 PVU = 1.0 x 10(-6) K kg-1 m2 s-1) contour on the 500 K isentropic surface. The principal results are: (1) there is a distinct change after 1985 in the vortex-averaged column ozone depletion rate during September and October, the period of maximum ozone loss, and (2) the vortex-averaged column ozone in late August (day 240) has dropped by 70 Dobson units (DU) in a decade due to the loss in the dark and the dilution effect. The mean ozone depletion rate in the vortex between day 240 and the day of minimum vortex-averaged ozone is about 1 DU d-1 at the beginning of the decade, increasing to about 1.8 DU d-1 by 1985, and then apparently saturating thereafter. The vortex-average column ozone during September and October has declined at the rate of 11.3 DU yr-1 (3.8%) from 1980 to 1987 (90 DU over 8 years) and at a smaller rate of 2 DU yr-1 (0.9%) from 1987 to 1991 (10 DU over 5 years, excluding the anomalous year 1988). We interpret the year-to-year trend in the ozone depletion rate during the earlier part of the decade as due to the rise of anthropogenic chlorine in the atmosphere. The slower trend at the end of the decade indicates saturation of ozone depletion in the vortex interior, in that chlorine amounts in the mid-1980s were already sufficiently high to deplete most of the ozone in air within the isolated regions of the lower-stratospheric polar vortex. In subsequent years, increases in stratospheric chlorine may have enhanced wintertime chemical loss of ozone in the south polar vortex even before major losses during the Antarctic spring.
Nitrous oxide (N2O) is an important greenhouse gas and ozone depleting substance as well as a key component of the nitrogen cascade. While emissions scenarios indicating the range of N2O's potential future contributions to radiative forcing are widely available, the impact of these emissions scenarios on future stratospheric ozone depletion is less clear. This is because N2O's ozone destructiveness is partially dependent on tropospheric warming, which affects ozone depletion rates in the stratosphere. Consequently, in order to understand the possible range of stratospheric ozone depletion that N2O could cause over the 21st century, it is important to decouple the greenhouse gas emissions scenarios and compare different emissions trajectories for individual substances (e.g. business-as-usual carbon dioxide (CO2) emissions versus low emissions of N2O). This study is the first to follow such an approach, running a series of experiments using the NASA Goddard Institute for Space Sciences ModelE2 atmospheric sub-model. We anticipate our results to show that stratospheric ozone depletion will be highest in a scenario where CO2 emissions reductions are prioritized over N2O reductions, as this would constrain ozone recovery while doing little to limit stratospheric NOx levels (the breakdown product of N2O that destroys stratospheric ozone). This could not only delay the recovery of the stratospheric ozone layer, but might also prevent a return to pre-1980 global average ozone concentrations, a key goal of the international ozone regime. Accordingly, we think this will highlight the importance of reducing emissions of all major greenhouse gas emissions, including N2O, and not just a singular policy focus on CO2.
The long-term evolution of the Antarctic ozone hole is studied based on the TOMS data and the JMA data-set of stratospheric temperature in relation with the possible role of polar stratospheric clouds (PSC's). The effective mass of depleted ozone in the ozone hole at its annual mature stage reached a historical maximum of 55 Mt in 1991, 4.3 times larger than in 1981. The ozone depletion rate during 30 days before the mature ozone hole does not show any appreciable long-term trend but the interannual fluctuations do, ranging from 0.169 to 0.689 Mt/day with the average of 0.419 Mt/day for the period of 1979 - 1991. The depleted ozone mass has the highest correlation with the region below 195 K on the 30 mb surface in June, whereas the ozone depletion rate correlates most strongly with that in August. The present result strongly suggests that the long-term evolution of the mature ozone hole is caused both by the interannual change of the latitudinal coverage of the early PSC's, which may control the latitude and date of initiation of ozone decrease, and by that of the spatial coverage of the mature PSC's which may control the ozone depletion rate in the Antarctic spring.
As discussed above, and supported by extensive literature, there is no robust, credible observational evidence for substantial ozone depletion (i.e., an “ozone hole”) in the tropics. It is well known that climatological total ozone in the tropics is much lower than that in the mid-latitudes (e.g., Sahai et al., 2000; Weber et al., 2022). Satellite and ozonesonde measurements indicate a 3%–5% per decade decline of tropical lower stratosphere ozone prior to 2000, far smaller than that reported by L2022. The stronger decline reported by L2022 is caused by inappropriate use of the gap-filled version of the TOST ozone dataset, which is based on sparse tropical ozone sondes before the 1990s. This misuse of data (TOST and total column ozone) shows the importance of collaboratively engaging with groups who obtain the measurements and create climatological datasets before performing such analyses. Furthermore, the study by L2022 has multiple flaws in its discussion of atmospheric chemistry and dynamics, particularly in the proposed, and previously refuted (see Sec. III A), cosmicray- driven electron induced (CRE) mechanism. Evidence for the occurrence of tropical stratospheric clouds, as needed for the tropical CRE mechanism, is lacking, nor do CFC-12 observations show signatures of depletion in the tropical lower stratosphere, which could be associated with dissociative electron attachment-induced loss of CFC-12 on particulate matter (i.e., the CRE mechanism). Finally, it is worth reiterating that the CRE mechanism is also not responsible for polar LS ozone depletion. Polar ozone loss can be well explained by the gas phase and heterogeneous chemistry, based on extensive observations and modeling studies documented in many thousands of scientific papers on the topic [e.g., see WMO (2018) and references therein], which is not acknowledged by L2022. L2022’s research paper is a severely flawed one. There is no tropical ozone hole, and the CRE mechanism does not explain observed changes in stratospheric ozone either in the polar regions or in the tropics.
Recently published findings using satellite and ground-based observations indicate a large winter and summertime decrease in the column abundance of ozone at high and middle latitudes during the last decade. Using a simple ozone depletion profile reflecting the observed decrease in ozone column abundance, Ramaswamy et al. (1992) showed that the negative radiative forcing that results from the ozone decrease between 1979 and 1990 approximately balanced the greenhouse climate forcing due to the chlorofluorocarbons emitted during the same period. Here, we extend the forcing analyses by calculating the equilibrium surface temperature response explicitly, using an updated version of the Atmospheric and Environmental Research two-dimensional radiative-dynamical seasonal model. The calculated steady state responses suggest that the surface cooling due to the ozone depletion in the lower stratosphere offsets about 30% of the surface warming due to greenhouse gases emitted during the same decade. The temperature offset is roughly a factor of 2 larger than the corresponding offset obtained from forcing intercomparisons. This result appears to be related to the climate feedback mechanisms operating in the model troposphere, most notably that associated with atmospheric meridional heat transport. Thus a comprehensive assessment of ozone change effects on the predicted greenhouse warming cannot be accomplished based on forcing evaluations alone. Our results also show that calculations adopting a seasonally and latitudinally dependent ozone depletion profile produce a negative forcing about 50% smaller than that calculated for the depletion profile used by Ramaswamy et al. (1992).
Reduced quantities of ozone in the atmosphere allow greater levels of ultraviolet light (UV) radiation to reach the earth's surface. This is known to cause skin cancer and mutations. Chlorine liberated from Chlorofluorocarbons (CFC's) and natural sources initiate the destruction of stratospheric ozone through a free radical chain reaction. The project goals are to understand the processes which contribute to stratospheric ozone loss, examine ways to prevent ozone loss, and design a vehicle-based system to carry out the prevention scheme. The 1992/1993 design objectives were to accomplish the first two goals and define the requirements for an implementation vehicle to be designed in detail starting next year. Many different ozone intervention schemes have been proposed though few have been researched and none have been tested. A scheme proposed by R.J. Cicerone, Scott Elliot and R.P.Turco late in 1991 was selected because of its research support and economic feasibility. This scheme uses hydrocarbon injected into the Antarctic ozone hole to form stable compounds with free chlorine, thus reducing ozone depletion. Because most polar ozone depletion takes place during a 3-4 week period each year, the hydrocarbon must be injected during this time window. A study of the hydrocarbon injection requirements determined that 100 aircraft traveling Mach 2.4 at a maximum altitude of 66,000 ft. would provide the most economic approach to preventing ozone loss. Each aircraft would require an 8,000 nm. range and be able to carry 35,000 lbs. of propane. The propane would be stored in a three-tank high pressure system. Missions would be based from airport regions located in South America and Australia. To best provide the requirements of mission analysis, an aircraft with L/D(sub cruise) = 10.5, SFC = 0.65 (the faculty advisor suggested that this number is too low) and a 250,000 lb TOGW was selected as a baseline. Modularity and multi-role functionality were selected to be key design features. Modularity provides ease of turnaround for the down-time critical mission. Multi-role functionality allows the aircraft to be used beyond its design mission, perhaps as an High Speed Civil Transport (HSCT) or for high altitude research.
Aircraft, ground-based, and satellite measurements indicate large concentrations of ClO in the lower stratosphere in and near the polar vortex. The amount of local ozone depletion caused by these large ClO concentrations will depend on the relative rates of ozone loss and ClO recovery. ClO recovery occurs when NO(x), from HNO3 photolysis, reacts with ClO to form ClONO2. We show that air parcels with large amounts of ClO will experience a subsequent ozone depletion that depends on the solar zenith angle. When the solar zenith angle is large in the middle of winter, the recovery of the ClO concentration in the parcel is slow relative to ozone depletion. In the spring, when the solar zenith angle is smaller, the ClO recovery is much faster. After ClO recovery, the chlorine chemistry has not returned to normal. The ClO has been converted to ClONO2. ClO production from further encounters with PSCs will be limited by the heterogeneous reaction of ClONO2 with water. Large ozone depletions, of the type seen in the Antarctic, occur only if there is significant irreversible denitrification in the air parcel.
After more than three decades of research, the roles of polar stratospheric clouds (PSCs) in stratospheric ozone depletion are well established. Heterogeneous reactions on PSCs convert the stable chlorine reservoirs HCl and ClONO2 to chlorine radicals that destroy ozone catalytically. PSCs also prolong ozone depletion by delaying chlorine deactivation through the removal of gas-phase HNO3 and H2O by sedimentation of large nitric acid trihydrate (NAT) and ice particles. A substantial recovery of the ozone layer is expected by the middle of this century with reduced global production of ozone depleting substances in accordance with the Montreal Protocol and subsequent amendments. But as climate changes, leading to a colder and perhaps wetter stratosphere and upper troposphere, reliable model predictions of recovery of the Antarctic ozone hole and of potentially more severe ozone depletion in the Arctic are challenging. This is due both to a lack of detailed understanding of the underlying physics and the fact that many global models use simple parameterizations that do not accurately represent PSC processes. A more complete picture of PSC processes on vortex-wide scales has emerged from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) instrument on the CALIPSO satellite that has been observing PSCs at latitudes up to 82 degrees in both hemispheres since June 2006. The CALIOP Version 2.0 (v2) PSC algorithm was recently developed to address known deficiencies in previous algorithms and includes additional refinements to increase the robustness of the inferred PSC composition. In this paper, we present an updated PSC reference data record and comprehensive climatology constructed by applying the v2 algorithm to the more than 17-year CALIOP spaceborne lidar dataset. In addition, we will examine the potential impact of aerosol and water vapor injections into the stratosphere from the January 2022 Hunga Tonga eruption on PSC occurrence in both the Arctic and Antarctic regions.
Efforts for the 2022 Scientific Assessment on Ozone Depletion published by the World Meteorological Organization are well underway. Chapter 3, titled “Update on Global Ozone: Past, Present, and Future”, presents our current understanding of global ozone outside of the polar regions and this talk summarizes some of the highlights and changes from the previous Assessment in 2018. Since the last Assessment, the longer observational records show a small, significant increase in near-global total column ozone. A small significant increase in total column ozone is also seen in the mid-latitudes of both hemispheres, but not yet the tropics. Different processes operating at different altitudes complicate the interpretation of the overall total column trend. However, a significant increase in upper stratospheric ozone noted in the previous Assessment continues, driven by declines in ozone depleting substances and increases in greenhouse gases. Model simulations support our understanding of these trends. Over the coming century, we expect an increase in global stratospheric ozone as the concentrations of ozone depleting substances decline. The future evolution for different latitudes and vertical levels depends on the future concentrations of greenhouse gases and precursors of tropospheric ozone., These other influences may lead to total ozone column levels that remain below 1980 values even after ozone depleting substance concentrations have recovered to pre-1980 levels.
Refrigeration and air conditioning currently account for ~20% of the total electricity consumption in buildings around the world (IEA, 2018). Over the next three decades, as global temperatures are projected to increase, urbanization and economic growth will lead to an increased demand for refrigeration and cooling. While technological advances have led to increased cooling capacity and safer refrigerants over the years, emissions from refrigeration systems can affect the environment by contributing to greenhouse gas emissions or by depleting the ozone layer, depending on the gas emitted. Further, because of ongoing and pending policy and regulatory changes to avert ozone depletion and global climate change, there is an increasing focus on adopting compounds that are efficient at cooling while also reducing emissions and other adverse environmental impacts.
Three simultaneous observations of atomic chlorine (Cl) and the clorine monoxide radical (ClO) are reported which encompass the altitude interval between 25 and 45 kilometers. Together, Cl and ClO form a gas-phase catalytic cycle potentially capable of depleting stratospheric ozone. Observed Cl and ClO densities, although variable, imply that chlorine compounds constitute an important part of the stratospheric ozone budget. The results are compared with recent models of stratospheric photochemistry which have been used as a basis for predicting ozone depletion resulting from fluorocarbon release.
The discovery of Farman et al. of recent large depletions of ozone in the Antarctic stratosphere in the austral spring has aroused great interest because of its serious potential consequences, as well as its surprising nature. An airborne expedition, including 21 experiments on two aircraft, was mounted for Punta Arenas, Chile, in August and September, 1987, to gather a wide range of data to understand the origins and implications of this phenomenon, known as the ozone hole. As a part of this expedition, a high resolution Fourier transform spectrometer was flown on the DC-8, measuring the column amount of a number of trace gases above the flight altitude. Column results are presented only from the flight of September 21; results from other flights are included in an accompanying paper. The deduced column for ozone HCl, and NO2 deduced from the spectra, plotted as a function of latitude are shown. It should be noted that there are many other factors varying as well as the latitude, but latitude seems to be the variable which most clearly provides a passage across the vortex boundary. It can be seen that south 76 degrees S., the column of ozone, HCl, and NO2, all decreas markedly, The ratio of HCl to Hf, normally about 5:1 in midlatitudes, approaches unity. Clearly the chemistry of chlorine and nitrogen are disturbed in the region of low ozone. While dynamical theories could perhaps explain a reduction of these three gases in the same region, since all are of stratospheric origin, it is difficult to see how any purely dynamical mechanism could produce the observed HCl:HF ratio, since the two gases have similar origins. A close look at other species to be reported as well as the correlation with other measurements, such as ClO supports the conclusion that the ozone depletion is a result of chemical processes which deplete HCl and NOx relative to the midlatitude situation.
Mixing ratios are presented for a number of long-lived trace gases in the austral polar atmosphere during August and September of 1987. The recent discovery of a 12-year trend of increasing depletion of ozone over the Antarctic Continent in the spring of each year led to numerous theoretical interpretations and several scientific expeditions to the region. The results herein were obtained as part of a major effort involving penetration of the region of ozone depletion by NASA's multi-instrumented aircraft. One of the 14 instruments on the high-altitude ER-2 aircraft collected pressurized air samples between latitudes of 53 degrees and 72 degrees south at pressure altitudes up to 21 km in a series of 12 flights from Punta Arenas, Chile, over the Palmer Peninsula. The sampling system, located in the nose section of ER-2, has an inlet tube in the free airstream, a metal-bellows air pump, and 14 specially treated 1.6 l stainless-steel canisters for containing the pressurized air at 350 kPa. A typical flight profile consisted of a southbound path on the 428 K potential temperature surface, a descent to a pressure altitude of 13.7 km, a climb to the 460 K surface, and return on this surface. Mixing ratios for the trace gases were obtained from gas chromatographic analyses of the pressurized air samples. Of the species measured, the mixing ratios for CH4, CO, N2O, CF2 Cl2, CFCl3, CH3, CCl3, CCl4, and C2F3Cl3 are reported here.