Scenarios of possible changes in atmospheric temperatures and ozone concentrations due to man's activities,estimated with a one-dimensional coupled photochemical climate model

A one-dimensional coupled climate and chemistry model has been developed to estimate past and possible future changes in atmospheric temperatures and chemical composition due to human activities. The model takes into account heat flux into the oceans and uses a new tropospheric temperature lapse rate formulation. As found in other studies, we estimate that the combined greenhouse effect of CH₄, O₃, CF₂Cl₂, CFCl₃ and N₂O in the future will be about as large as that of CO₂. Our model calculates an increase in average global surface temperatures by about 0.6°C since the start of the industrial era and predicts for A.D. 2050 a twice as large additional rise. Substantial depletions of ozone in the upper stratosphere by between 25% and 55% are calculated, depending on scenario. Accompanying temperature changes are between 15°C and 25°C. Bromine compounds are found to be important, if no rigid international regulations on CFC emissions are effective. Our model may, however, concivably underestimate possible effects of CFCl₃, CF₂Cl₂, C₂F₃Cl₃ and other CFC and organic bromine emissions on lower stratospheric ozone, because it can not simulate the rapid breakdown of ozone which is now being observed worldwide. An uncertainty study regarding the photochemistry of stratospheric ozone, especially in the region below about 25 km, is included. We propose a reaction, involving excited molecular oxygen formation from ozone photolysis, as a possible solution to the problem of ozone concentrations calculated to be too low above 45 km. We also estimate that tropospheric ozone concentrations have grown strongly in the northern hemisphere since pre-industrial times and that further large increases may take place, especially if global emissions of NO_x from fossil fuel and biomass burning were to continue to increase. Growing NO_x emissions from aircraft may play an important role in ozone concentrations in the upper troposphere and low stratosphere.     

A model investigation of the impact of increases in anthropogenic NO x emissions between 1967 and 1980 on tropospheric ozone

Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH₄ and NO _x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO _x emissions during this period while the contribution of CH₄ to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO _x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO _x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.     

A reassessment of stratospheric ozone: Credibility of the threat

A recent review of ozone observations and model predictions designed to determine the credibility of current stratospheric models, arrived at the following conclusions. Aside from prompt variations at altitudes above 30 km, observed variations in stratospheric ozone cannot be explained by the process of catalytic destruction; i.e. past variations in the ozone layer have been controlled by processes not included in current models. Past episodic stratospheric injections of oxides of nitrogen and chlorine have not induced changes in total ozone identifiable in the observational data. Species concentrations from different models differ greatly; by up to two orders of magnitude in some features. Even models with highly unlikely chemical reaction rates compute species concentration profiles currently considered to be in reasonable agreement with available observations. Observations of stratospheric species, particularly nitrous oxide and nitric acid, suggest that the natural stratospheric source of odd nitrogen has been underestimated by most models by 2- to 5-fold. These apparent disparities between observations and theory suggest flaws or omissions in our understanding of stratospheric ozone and a need for caution in accepting the predictions of current stratospheric models.A slightly amended but unupdated version of an invited paper presented at the Environmental Health Sciences Symposium: SST Pollution and Skin Cancer at the 50th Anniversary Congress of the Pan American Medical Association, Hollywood, Florida, October 25–29, 1976. Editor's Note: This paper, while containing an unsual number of personal opinions - which are, commendably, stated as such - does focus on an important controversy. Thus, it is published in the interest of stimulating further debate on the subject.     

Tropospheric Ozone at the Swedish Mountain Site Åreskutan: Budget and Trends

Ozone measurements, performed since 1987, at the Swedish TOR/EUROTRACstation Åreskutan (lat. 63.4° N, long. 13.1° E, 1250 m abovesea level) are analyzed. The annual average ozone concentration at the sitehas increased by about 0.4 ppbv (1%) per year during the period1987–1994. The corresponding trends for individual months show adecrease during April–September and an increase during the rest of theyear. The ozone budget at Åreskutan has been investigated using backtrajectories of the air parcels, and the cosmogenic radionuclide⁷Be as a tracer of stratospheric air. From a simple diagnosticmodel, it is estimated that the contribution of stratospheric ozone to theconcentrations measured at Åreskutan is 5 ppbv (or 14% of themeasured values) on average, reaching a maximum of 23 ppbv (50%),during the episodes of direct stratospheric influence. In spring, thestratospheric contribution to ozone budget at Åreskutan is at itsmaximum, and approximately equal to the net photochemical ozone productionin the air mass affecting the site, whereas in winter, it is compensated byozone chemical sink during the transport of air masses from pollutedEuropean regions, to Scandinavia.     

A review of global stratospheric aerosol: Measurements, importance, life cycle, and local stratospheric aerosol

Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm^− 3), increasing by factors of 2–4 (10–10³) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO₂, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO₂ have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.     

Total ozone variations in the tropical belt: An application for quality of ground based measurements

Summary The study of the regime of ozone variations in the huge tropical belt (25° S to 25° N), which are, in general, very small and zonally nearly symmetric, permits to establish a statistical model for estimating the ozone deviations using Total Ozone Mapping Spectrometer (TOMS) data. The equatorial stratospheric winds at 25 and 50hPa and the solar flux at 10.7 cm are used as major predictors and the linear trend was also estimated. The 10m/sec stratospheric wind change is related to1.2% ozone change at the equator, to practically no change in the 8–15° belts and up to 1.4% change with opposite phase over the tropics in spring but nearly zero change in fall. The solar cycle related amplitude is about 1.4% per 100 units of 10.7 cm solar flux. The ozone trends are negative: not significant over the equator and about –2% per decade (significant at 95% level) over the tropics. The latter could have been enforced by the 2 to 4% lower ozone values during 1991–1993, part of which might be related to the effects of the Mt. Pinatubo eruption, but might also be due to the strong QBO. The estimated deviations are verified versus reliable observations and the very good agreement permits applying the model for quantitative quality control of the reported ozone data from previous years. The standard deviation of the difference between observed ozone deviations and those estimated from the model is only 0.9–1.6% for yearly mean, that means instruments used for total ozone observations in the tropical belt should have systematic error of less than 1%. Cases when the discrepancies between the model and reported observations at a given station exceed 2–3% for time interval of 2 or more years should be verified.With 17 Figures     

Impact of the Montreal protocol and its amendments on the rate of change of global radiative forcing

Increases in chlorinated and brominated halocarbons are believed to be responsible for the depletion of stratospheric ozone observed over much of the globe in the past decade or so. Ozone depletion is in turn believed to lead to a negative radiative forcing, tending to cool the stratosphere and the surface. We show that the increasing atmospheric concentrations of ozone-depleting halocarbons and onset of related ozone depletion likely led to a negative forcing of the climate system in the 1980s that slowed significantly the rate of change of total anthropogenic radiative forcing due to the combined effect of all greenhouse gases over that decade. Within the next decade, emissions of these halocarbons are expected to rapidly decrease, with corresponding impacts on ozone and radiative forcing. As the emissions of ozone-depleting gases are reduced and eventually phased out, the rate of ozone depletion is expected to decrease and eventually reverse. All other things being equal, we show that the change from deepening ozone depletion in the 1980s to ozone increases in the future should lead to a pronounced increase in the decadal rate of change of anthropogenic greenhouse forcing of the next few decades, perhaps to levels unprecedented in this century.     

Characteristics of the ozone decline in the northern polar and middle latitudes during the winter-spring

Summary The total ozone decline during the past twenty years, especially strong during the winter-spring season poleward from 50° N, is well established with known average trends of 5–7% per decade. This study presents a number of additional characteristics such as ozone-mass deficiency (O₃MD) from the pre- 1976 base average, and areal extent with negative deviations greater than2 and3. Gridded satellite data combined with ground-based total ozone maps, permit calculations of daily and regional ozone deficiencies from the anthropogenically undisturbed average ozone levels of the 1960s and early 1970s. Then the quantity of the O₃MD and the changes in surface area, with deficiencies larger than-10 and-15% are integrated for the 1 January to 15 April period for each of the last 20 years, and compared. In addition, the polar vortex extent during the last 10 years is determined using the PV at 475°K. The quantity of the O₃MD within the sunlit part of the vortex is shown to contribute from15 to 35% of the overall ozone deficiency within the-10% contours over the area 35–90°N. The ozone deficiency, integrated for the first 105 days of each year, has increased dramatically from 2,800Mt in the early 1980s to7,800Mt in the 1990s, exceeded 12,000Mt in the winter-springs of 1993 and 1995. The latter quantity is comparable with the average O₃MD over the same Southern latitudes in the last ten austral springs. During the 1990s over the 35–90° latitudes the average ozone deficiency in the Southern hemisphere belt is less than over the Northern hemisphere belt by40%. It is known that the main ozone decline is observed in the lower stratosphere and the ozone loss over the Arctic is very sensitive to decreasing stratospheric temperatures; negative 50hPa monthly anomalies greater than 4°C have occurred during 7 of the springs in the last decade, thus possibly facilitating doubling the area with negative ozone deviations greater than-10% in the 1990s to5,000.10⁶km² and nearly tripling the O₃MD as stated above. The changes in total eddy heat fluxes as a proxy indicator of the long wave perturbations are positively correlated with the ozone deficiency in the 45–75°N. The strong anticorrelation between the ozone deficiency in the region>55° N. versus the 35–50° N belt is discussed in relation to possible transport of air masses with low ozone from the sub-tropics, which in some years are the dominant reason for the observed ozone deficiency.With 11 Figures     

Changing trends in tropospheric methane and carbon monoxide: A sensitivity analysis of the OH-radical

A sensitivity analysis is performed in order to study recently observed changes in atmospheric methane and carbon monoxide trends. For the analysis we have adapted a one-dimensional transport/chemistry model in order to comply with changes in vertical transport, stratosphere-troposphere flux of ozone, the water vapour cycle and the short-wave radiative transfer. In addition we have formulated an improved relationship which expresses the steady state OH concentration in terms of longer lived compounds which has a fair agreement with the one-dimensional model results. An analysis of the observed changes and trends in methane and carbon monoxide shows that both emissions and changes in global OH concentrations can be main causes for the observed changes. Average methane emissions have slowed down, particularly in the NH, in the last five years, though perhaps not very significantly. Carbon monoxide emissions are decreasing faster in the last couple of years than in the period 1983–1990. The study suggests that climate fluctuations (tropospheric water vapour, temperature and convective activity) and the stratospheric ozone depletion (tropospheric UV radiation) have a significant influence on tropospheric composition and thus on trends in methane and carbon monoxide concentrations.The IMAU is partner in the Netherlands Centre for Climate Research (CCR).     

Limitations of single-basket trading: lessons from the Montreal Protocol for climate policy

Numerous policy options exist to reduce future greenhouse gas emissions. A single-basket approach, which controls aggregate emissions, was adopted by the Kyoto Protocol. Such an approach allows emissions reductions of one gas to be traded with those of other gases in the “basket”, with the trade “price” determined by some weighting metric like the Global Warming Potential. To reduce stratospheric ozone depletion, the Montreal Protocol also dealt with controlling many compounds, but did so employing an alternative, multi-basket scheme. Trading was allowed within each basket, but not among baskets. While the Montreal Protocol has been highly successful using this approach, we show that if a single-basket approach had been adopted the short-term success could have been at risk due to the non-unique relationship between controls and environmental impacts when using a single basket. Using climate policy as an example, and without considering technological and economic constraints, we further show that the magnitude of the ambiguities in impacts associated with a single-basket approach depends on the rapidity of the emission phaseout. Fast phaseouts lead to less ambiguity than do slow ones. These results suggest that for each set of greenhouse gas control policies considered, the benefit of additional flexibility associated with a single-basket approach should be weighed against the associated increased uncertainties in the impacts to ascertain whether a single- or a multi-basket approach has the greater chance of successfully mitigating climate change.     

Intercomparison of Stratospheric Chemistry Models under Polar Vortex Conditions

Several stratospheric chemistry modules from box, 2-D or 3-D models, have been intercompared. The intercomparison was focused on the ozone loss and associated reactive species under the conditions found in the cold, wintertime Arctic and Antarctic vortices. Comparisons of both gas phase and heterogeneous chemistry modules show excellent agreement between the models under constrained conditions for photolysis and the microphysics of polar stratospheric clouds. While the mean integral ozone loss ranges from 4–80% for different 30–50 days long air parcel trajectories, the mean scatter of model results around these values is only about ±1.5%. In a case study, where the models employed their standard photolysis and microphysical schemes, the variation around the mean percentage ozone loss increases to about ±7%. This increased scatter of model results is mainly due to the different treatment of the PSC microphysics and heterogeneous chemistry in the models, whereby the most unrealistic assumptions about PSC processes consequently lead to the least representative ozone chemistry. Furthermore, for this case study the model results for the ozone mixing ratios at different altitudes were compared with a measured ozone profile to investigate the extent to which models reproduce the stratospheric ozone losses. It was found that mainly in the height range of strong ozone depletion all models underestimate the ozone loss by about a factor of two. This finding corroborates earlier studies and implies a general deficiency in our understanding of the stratospheric ozone loss chemistry rather than a specific problem related to a particular model simulation.     

Solar-hydrogen electricity generation in the context of global CO2 emission reduction

The relative costs and CO₂ emission reduction benefits of advanced centralized fossil fuel electricity generation, hybrid photovoltaic-fossil fuel electricity generation, and total solar electricity generation with hydrogen storage are compared. Component costs appropriate to the year 2000–2010 time frame are assumed throughout. For low insolation conditions (160 W m^–2 mean annual solar radiation), photovoltaic electricity could cost 5–13 cents/kWh by year 2000–2010, while for high insolation conditions (260 W m^–2) the cost could be 4–9 cents/kWh. Advanced fossil fuel-based power generation should achieve efficiencies of 50% using coal and 55% using natural gas. Carbon dioxide emissions would be reduced by a factor of 2 to 3 compared to conventional coal-based electricity production in industrialized countries. In a solar-fossil fuel hybrid, some electricity would be supplied from solar energy whenever the sun is shining and remaining demand satisfied by fossil fuels. This increases total capital costs but saves on fuel costs. For low insolation conditions, the costs of electricity increases by 0–2 cents/kWh, while the cost of electricity decreases in many cases for high insolation conditions. Solar energy would provide 20% or 30% of electricity demand for the low and high insolation cases, respectively. In the solar-hydrogen energy system, some photovoltaic arrays would provide current electricity demand while others would be used to produce hydrogen electrolytically for storage and later use in fuel cells to generate electricity. Electricity costs from the solar-hydrogen system are 0.2–5.4 cents/kWh greater than from a natural gas power plant, and 1.0–4.5 cents/kWh greater than from coal plant for the cost and performance assumptions adopted here. The carbon tax required to make the solar-hydrogen system competitive with fossil fuels ranges from $70–660/tonne, depending on the cost and performance of system components and the future price of fossil fuels.Leakage of hydrogen from storage into the atmosphere, and the eventual transport of a portion of the leaked hydrogen to the stratosphere, would result in the formation of stratospheric water vapor. This could perturb stratospheric ozone amounts and contribute to global warming. Order-of-magnitude calculations indicate that, for a leakage rate of 0.5% yr^–1 of total hydrogen production -which might be characteristic of underground hydrogen storage - the global warming effect of solarhydrogen electricity generation is comparable to that of a natural gas-solar energy hybrid system after one year of emission, but is on the order of 1% the impact of the hybrid system at a 100 year time scale. Impacts on stratospheric ozone are likely to be minuscule.     

Isotopic Composition of Non-Methane Hydrocarbons in Emissions from Biomass Burning

The stable carbon isotope ratios of nonmethane hydrocarbons (NMHC) and methyl chloride emitted from biomass burning were determined by analyzing seven whole air samples collected during different phases of the burning process as part of a laboratory study of wood burning. The average of the stable carbon isotope ratios of emitted alkanes, alkenes and aromatic compounds is identical to that of the burnt fuel; more than 50% of the values are within a range of ±1.5 of thecomposition of the burnt fuel wood. Thus for the majority of NMHC emitted from biomass burning stable carbon isotope ratio of the burnt fuel a good first order approximation for the isotopic composition of the emissions. Of the more than twenty compounds we studied, only methyl chloride and ethyne differed in stable carbon isotope ratios by more than a few per mil from the composition of the fuel. Ethyne is enriched in ¹³C by approximately 20–30, and most of the variability can beexplained by a dependence on flame temperature. The ¹³C values decreaseby 0.019 /K (±0.0053/K) with increasing temperature. Methyl chloride is highly depleted in ¹³C, on average by25. However the results cover a wide range of nearly 30. Specifically, in two measurements with wood from Eucalyptus (Eucalyptus delegatensis) as fuel we observed the emission of extremely light methyl chloride (–68.5and–65.5). This coincides with higher than average emission ratiosfor methyl chloride (15.5 × 10^–5 and 18 ×10^–5 mol CH₃Cl/mol CO₂). These high emission ratios are consistent with the highchlorine content of the burnt fuel, although, due to the limited number of measurements, it would be premature to generalize these findings. The limited number of observations also prevents any conclusion on a systematic dependence between chlorine content of the fuel, emission ratios and stable carbon isotope ratio of methyl chloride emissions. However, our results show that a detailed understanding of the emissions of methyl chloride from chloride rich fuels is important for understanding its global budget. It is also evident that the usefulness of stable carbon isotope ratios to constrain the global budget of methyl chloride will be complicated by the very large variability of the stable carbon isotope ratio of biomass burning emissions. Nevertheless, ultimately the large fractionation may provide additional constraints for the contribution of biomass burning emissions to the atmospheric budget of methyl chloride.     

Extremely low temperatures in the stratosphore and very low total ozone amount above northern and central Europe during winter 1989

On 1 February 1989, -83.5°C was recorded in 27.8 hPa over Hohenpeißenberg, the lowest temperature in the 22-year series. This was measured together with a very low total ozone amount of 266 DU. This may be compared with nearly twice this amount on 27 February 1989. The situation was very unusual: following an extremely cold winter in the Arctic stratosphere, the stratospheric cold pole was located over southern Scandinavia on 1 February in a very southerly position. The analyzed temperatures of -92 °C in 30 hPa were also unusual. Even though the low ozone amounts over Hohenpeißenberg were probably dynamically caused, an additional very small ozone decrease due to heterogeneous reactions in altitudes from 23–28 km, where the temperatures lie below -80 °C, cannot be ruled out. Extinction measurements by the orbitting SAGE II instrument indeed show polar stratospheric clouds over Europe near 50° N during the period 31 January–2 February. Also, polar stratospheric clouds were previously observed over Kiruna at similarly low temperatures and signs of a corresponding small ozone decrease were noted there.     

Ozone production due to emissions from vegetation burning

Ozone has been observed in elevated concentrations by satellites over areas previously believed to be background. There is meteorological evidence, that these ozone plumes found over the Atlantic Ocean originate from vegetation fires on the African continent.In a previous study (DECAFE-88), we have investigated ozone and assumed precursor compounds over African tropical forest regions. Our measurements revealed large photosmog layers at altitudes from 1.5 to 4 km. Both chemical and meteorological evidence point to savanna fires up to several thousand km upwind as sources.Here we describe ozone mixing ratios observed over western Africa and compare ozone production ratios from different field measurement campaigns related to vegetation burning. We find that air masses containing photosmog ingredients require several days to develop their oxidation potential, similar to what is known from air polluted by emissions from fossil fuel burning. Finally, we estimate the global ozone production due to vegetation fires and conclude that this source is comparable in strength to the stratospheric input.     

The Gas Phase Reaction of Unsaturated Oxygenates with Ozone: Carbonyl Products and Comparison with the Alkene-Ozone Reaction

Carbonyl products have been identified and their formation yields measured in the gas phase reaction of ozone with unsaturated oxygenates in experiments carried out at ambient T, p = 1 atm. of purified humid air (RH = 50%) and with sufficient cyclohexane added to scavenge the hydroxyl radical. The compounds studied are the esters methyl acrylate, vinyl acetate and cis-3-hexenyl acetate, the carbonyl crotonaldehyde, the hydroxy-substituted diene linalool, the ether ethylvinyl ether and the keto-ether trans-4-methoxy-3-buten-2-one. The alkene 1-pentene was included for comparison. The nature and formation yields of the carbonyl products from this study and those measured in earlier work under the same conditions are compared to those of alkenes and are supportive of a reaction mechanism that is similar to that for the reaction of ozone with alkenes, i.e. O₃ + R₁R₂C=CR₃X (R₁COR₂ + R₃XCOO) + (1 – )(R₃COX + R₁R₂COO), where R_i are the alkyl substituents, X is the oxygen-containing substituent (–CHO for aldehydes; –C(O)R for ketones; –C(O)OR and –OC(O)R for esters; –OH and hydroxyalkyl for alcohols; and –OR for ethers), R₁COR₂ is the primary carbonyl, R₃COX is the other primary product and R₁R₂COO and R₃XCOO are the carbonyl oxide biradicals. The biradicals lead to carbonyls in reactions that are also analogous to those involved in carbonyl formation from biradicals in the ozone-alkene reaction. These features make it possible to predict the nature and formation yields of the major carbonyl products of the reaction of ozone with unsaturated oxygenates that may be components of biogenic emissions.     

A global model study of natural bromine sources and the effects on tropospheric chemistry using MOZART4

Halogens in the atmosphere chemically destroy ozone. In the troposphere, bromine has higher ozone destruction efficiency than chlorine and is the halogen species with the widest geographical spread of natural sources. We investigate the relative strength of various sources of reactive tropospheric bromine and the influence of bromine on tropospheric chemistry using a 6-year simulation with the global chemistry transport model MOZART4. We consider the following sources: short-lived bromocarbons (CHBr₃, CH₂BrCl, CHBr₂Cl, CHBrCl₂, and CH₂Br₂) and CH₃Br, bromine from airborne sea salt particles, and frost flowers and sea salt on or in the snowpack in polar regions. The total bromine emissions in our simulations add up to 31.7 Gmol(Br)/yr: 63 % from polar sources, 24.6 % from short-lived bromocarbons and 12.4 % from airborne sea salt particles. We conclude from our analysis that our global bromine emission is likely to be on the lower end of the range, because of too low emissions from airborne sea salt. Bromine chemistry has an effect on the oxidation capacity of the troposphere, not only due to its direct influence on ozone concentrations, but also by reactions with other key chemical species like HO _x and NO _x . Globally, the impact of bromine chemistry on tropospheric O₃ is comparable to the impact of gas-phase sulfur chemistry, since the inclusion of bromine chemistry in MOZART4 leads to a decrease of the O₃ burden in the troposphere by 6 Tg, while we get an increase by 5 Tg if gas-phase sulfur chemistry is switched off in the standard model. With decreased ozone burden, the simulated oxidizing capacity of the atmosphere decreases thus affecting species associated with the oxidation capacity of the atmosphere (CH₃OOH, H₂O₂).     

未来百年夏季青藏高原臭氧变化趋势及可能机制

利用全大气气候通用模式(WACCM3)对政府间气候变化专门委员会排放情景特别报告中2001年到2099年A1B、A2、B1三种排放情景进行了模拟,分析了三种排放情景下青藏高原地区未来百年臭氧总量在夏季(6—8月)的变化趋势及引起该变化的可能机制。结果表明:在三种排放情景下未来百年夏季高原区臭氧总量均呈现增长趋势,其中A2情景下臭氧增长最快,B1情景下增长最慢,但相对于同纬度其他地区,高原区的臭氧总量增长较慢,即高原区臭氧谷加深。高原区高空污染物的减少以及局域Hadley环流的减弱是未来高原区臭氧总量增加的原因;而南亚高压的增强,以及与之相对应的辐散增强则可能是高原区臭氧谷继续加深的原因。     

The impact of high altitude aircraft on the ozone layer in the stratosphere

The paper discusses the potential effects on the ozone layer of gases released by the engines of proposed high altitude supersonic aircraft. The major problem arises from the emissions of nitrogen oxides which have the potential to destroy significant quantities of ozone in the stratosphere. The magnitude of the perturbation is highly dependent on the cruise altitude of the aircraft. Furthermore, the depletion of ozone is substantially reduced when heterogeneous conversion of nitrogen oxides into nitric acid on sulfate aerosol particles is taken into account in the calculation. The sensitivity of the aerosol load on stratospheric ozone is investigated. First, the model indicates that the aerosol load induced by the SO₂ released by aircraft is increased by about 10–20% above the background aerosols at mid-high latitude of the Northern Hemisphere at 15 km for the NASA emission scenario A (the NASA emission scenarios are explained in Tables I to III). This increase in aerosol has small effects on stratospheric ozone. Second, when the aerosol load is increased following a volcanic eruption similar to the eruption of El Chichon (Mexico, April 1982), the ozone column in spring increases by as much as 9% in response to the injection of NO _x from the aircraft with the NASA emission scenario A. Finally, the modeled suggests that significant ozone depletion could result from the formation of additional polar stratospheric clouds produced by the injection of H₂O and HNO₃ by the aircraft engines.     

A pro-active stratospheric ozone protection scenario

We explore the consequences of an earlier phase-out of ozone depleting substances, starting 10 years before the Montreal Protocol. Atmospheric chemistry simulations verify the effectiveness of such an early-action scenario: stratospheric chlorine abundance remains below the level at which the ozone hole was discovered, even though countries are permanently allowed to continue using ODS to a non-negligible extent. A sectorally detailed technico-economic analysis finds that the additional cost of the earlier action scenario would have been moderate. We conclude that the Montreal Protocol was only partially successful at precaution: global atmospheric environmental problems could be regulated before surprising non-linearities occur.