2‐D model simulations of anomalous spring variations of ozone,temperature and other minor trace constituents in the southern polar region

Abstract

A 2‐D time‐dependent Eulerian model that takes into account the major interaction between chemistry and dynamical transports in the stratosphere is used to simulate, in a self‐consistent manner, the anomalous spring variations of ozone, temperature and other relevant minor constituents in the southern polar region. The normal transport coefficients and the standard chemistry have been altered to represent the anomalous dynamical and chemical conditions in the extremely cold lower stratosphere of Southern Hemisphere (south of 65° S) spring. The results show that it is necessary to invoke both dynamical and chemical mechanisms in order to explain the observed rapid spring decline of total ozone in the southern polar region.     

Study of ozone distribution over the south-eastern France (ESCOMPTE campaign): discrimination between ozone tendencies due to chemistry and to transport

Ozone tendencies due to chemistry and transport are calculated by a mesoscale model using a fine horizontal resolution (3 km × 3 km), over South-Eastern France. Over that region where the anthropogenic emissions are very strong, ozone pollution is highlighted during two intensive observations periods of the ESCOMPTE campaign, when the sea breeze penetrates far into the Durance and Rhone valleys and the up-slope breezes are developed. From a fine analysis of time series of ozone concentration at different ground stations along these valleys and from numerical results, it is possible to discriminate the tendency due to chemistry from the tendency due to dynamical processes. We can distinguish both processes, either local chemical production/loss or dynamical increase/decrease (transport, deposition) on maps of ozone budget according to the meteorological conditions. In particular, we show that the variations due to transport can be have the same order of magnitude than those due to chemistry, reaching 20 ppbv h⁻¹, whereas those due to chemistry are around 30 ppbv h⁻¹.     

Future changes of the atmospheric composition and the impact of climate change

The development of the future atmospheric chemical composition is investigated with respect to NO _y and O₃ by means of the off‐line coupled dynamic‐chemical general circulation model ECHAM3/CHEM. Two time slice experiments have been performed for the years 1992 and 2015, which include changes in sea surface temperatures, greenhouse gas concentrations, emissions of CFCs, NO _x and other species, i.e., the 2015 simulation accounts for changes in chemically relevant emissions and for a climate change and its impact on air chemistry. The 2015 simulation clearly shows a global increase in ozone except for large areas of the lower stratosphere, where no significant changes or even decreases in the ozone concentration are found. For a better understanding of the importance of (A) emissions like NO _x and CFCs, (B) future changes of air temperature and water vapour concentration, and (C) other dynamical parameters, like precipitation and changes in the circulation, diabatic circulation, stratosphere‐troposphere‐exchange, the simulation of the future atmosphere has been performed stepwise. This method requires a climate‐chemistry model without interactive coupling of chemical species. Model results show that the direct effect of emissions (A) plays a major rôle for the composition of the future atmosphere, but they also clearly show that climate change (B and C) has a significant impact and strongly reduces the NO _y and ozone concentration in the lower stratosphere.     

Canadian middle atmosphere model: Preliminary results from the chemical transport module

Abstract

An important objective of middle atmosphere global climate modelling is the development of the capability of predicting the response of the middle atmosphere to natural or anthropogenic perturbations. To achieve this, a comprehensive chemistry package interactively coupled with radiative and dynamical modules is required. This paper presents preliminary results obtained with a photochemistry module which has been incorporated in the Canadian Middle Atmosphere Model (CMAM). The module contains 42 species including necessary oxygen, hydrogen, nitrogen, chlorine, bromine and methane oxidation cycle species. Photochemical balance equations are solved on‐line throughout the middle atmosphere at every dynamical time step. A full diurnal cycle is simulated with photolysis rates provided by a look‐up table. The chemistry solver is a mass conserving, fully implicit, backward difference scheme which currently uses less than 10% of the GCM run time. We present the results obtained from short integrations and compare them with UARS measurements. The model ozone distribution appears in quantitative agreement with observations showing peak values near 10 ppmv and confined to the 35‐km region. The abundance of nitrogen, chlorine, bromine oxides and their respective contributions to the overall ozone budget is realistic. The study illustrates the capability of the model to simulate middle atmosphere photochemistry for the disparate conditions occurring throughout the region.     

Numerical Modeling of the Influence of Physical and Chemical Factors on the Interannual Variability of Antarctic Ozone

The variability of Antarctic total column ozone in 1980–2018 is considered. The study analyzes trends in Antarctic total column ozone during the study period as well as the physical and chemical processes affecting the seasonal variability of total column ozone. The main attention is paid to the influence of dynamical processes on the stability of the Antarctic polar vortex, to the formation of polar stratospheric clouds, and to the influence of gas-phase and heterogeneous processes on the surface of polar stratospheric clouds and sulfate aerosol. The method of research is the analysis of the results of ground and satellite observations and numerical modeling of physical and chemical processes over the Antarctic using a global chemistry transport model with the dynamical parameters specified from reanalysis data.     

Long-Term Ozone Changes Over the Northern Hemisphere Mid-Latitudes for the 1979–2012 Period

Abstract

The solar backscattered ultraviolet (SBUV/SBUV-2) merged ozone datasets, version 8.6, including column ozone and ozone profiles for the 1979–2012 period are examined for the 35°N–60°N zonal belt in the northern hemisphere mid-latitudes and four sub-regions: central Europe, continental Europe, North America, and East Asia. The residual long-term patterns for total ozone and ozone profiles are extracted by smoothing the time series of differences between the original and the modelled ozone time series. Modelled ozone is obtained using the standard trend model accounting for ozone variability due to changes in stratospheric halogens and various dynamical factors commonly used in previous ozone trend analyses. Since about 2005 spring and summer total ozone in the troposphere and lower stratosphere has decreased in some regions (central and continental Europe, North America, and the 35°N–60°N zonal belt) compared with modelled ozone. The negative departure from modelled ozone in 2010 is approximately 2–3% of the overall 1979–2012 monthly mean level. It seems that this decrease is a result of yet unknown dynamical processes rather than to chemical destruction because the differences have a longitudinal structure, and total ozone in the upper stratosphere still follows changes in stratospheric halogen loading.     

Relative radiative forcing consequences of global emissions of hydrocarbons, carbon monoxide and NOx from human activities estimated with a zonally-averaged two-dimensional model

A global two-dimensional (altitude-latitude) chemistry transport model is used to follow the changes in the tropospheric distribution of the two major radiatively active trace gases, methane and ozone, following step changes to the sustained emissions of the short-lived trace gases methane, carbon monoxide and non-methane hydrocarbons. The radiative impacts were dependent on the latitude chosen for the applied change in emissions. Step change global warming potentials (GWPs) were derived for a range of short-lived trace gases to describe their time-integrated radiative forcing impacts for unit emissions relative to that of carbon dioxide. The GWPs show that the tropospheric chemistry of the hydrocarbons can produce significant indirect radiative impacts through changing the tropospheric distributions of hydroxyl radicals, methane and ozone. For aircraft, the indirect radiative forcing impact of the NO _x emissions appears to be greater than that from their carbon dioxide emissions. Quantitative results from this two-dimensional model study must, however, be viewed against the known inadequacies of zonally-averaged models and their poor representation of many important tropospheric processes.     

The Role of Ozone Depletion in the Lack of Cooling in the Antarctic Upper Stratosphere during Austral Winter

Temperature trends in the upper stratosphere are investigated using satellite measurements from Stratospheric Sounding Unit(SSU) outputs and simulations from chemistry–climate models(CCMs) and the Coupled Model Intercomparison Project Phase 6(CMIP6). Observational evidence shows a lack of cooling in the Antarctic, in contrast to strong cooling at other latitudes, during austral winter over 1979–97. Analysis of CCM simulations for a longer period of1961–97 also shows a significant contrast in the...     

Simulation of Tropospheric Ozone with MOZART-2： An Evaluation Study over East Asia

Climate changes induced by human activities have attracted a great amount of attention. With this, a coupling system of an atmospheric chemistry model and a climate model is greatly needed in China for better understanding the interaction between atmospheric chemical components and the climate. As the first step to realize this coupling goal, the three-dimensional global atmospheric chemistry transport model MOZART-2 (the global Model of Ozone and Related Chemical Tracers, version 2) coupled with CAM2 (the Community Atmosphere Model, version 2) is set up and the model results are compared against observations obtained in East Asia in order to evaluate the model performance. Comparison of simulated ozone mixing ratios with ground level observations at Minamitorishima and Ryori and with ozonesonde data at Naha and Tateno in Japan shows that the observed ozone concentrations can be reproduced reasonably well at Minamitorishima but they tend to be slightly overestimated in winter and autumn while underestimated a little in summer at Ryori. The model also captures the general features of surface CO seasonal variations quite well, while it underestimates CO levels at both Minamitorishima and Ryori. The underestimation is primarily associated with the emission inventory adopted in this study. Compared with the ozonesonde data, the simulated vertical gradient and magnitude of ozone can be reasonably well simulated with a little overestimation in winter, especially in the upper troposphere. The model also generally captures the seasonal, latitudinal and altitudinal variations in ozone concentration. Analysis indicates that the underestimation of tropopause height in February contributes to the overestimation of winter ozone in the upper and middle troposphere at Tateno.     

Impact of increasing stratospheric water vapor on ozone depletion and temperature change

Using a detailed, fully coupled chemistry climate model (CCM), the effect of increasing stratospheric H_{2O on ozone and temperature is investigated. Different CCM time-slice runs have been performed to investigate the chemical and radiative impacts of an assumed 2 ppmv increase in H2O. The chemical effects of this H2O increase lead to an overall decrease of the total column ozone (TCO) by ～1% in the tropics and by a maximum of 12% at southern high latitudes. At northern high latitudes, the TCO is increased by only up to 5% due to stronger transport in the Arctic. A 2-ppmv H2O increase in the model's radiation scheme causes a cooling of the tropical stratosphere of no more than 2 K, but a cooling of more than 4 K at high latitudes. Consequently, the TCO is increased by about 2%--6%. Increasing stratospheric H2O, therefore, cools the stratosphere both directly and indirectly, except in the polar regions where the temperature responds differently due to feedbacks between ozone and H2O changes. The combined chemical and radiative effects of increasing H2O may give rise to more cooling in the tropics and middle latitudes but less cooling in the polar stratosphere. The combined effects of H2O increases on ozone tend to offset each other, except in the Arctic stratosphere where both the radiative and chemical impacts give rise to increased ozone. The chemical and radiative effects of increasing H2O cause dynamical responses in the stratosphere with an evident hemispheric asymmetry. In terms of ozone recovery, increasing the stratospheric H2O is likely to accelerate the recovery in the northern high latitudes and delay it in the southern high latitudes. The modeled ozone recovery is more significant between 2000--2050 than between 2050--2100, driven mainly by the larger relative change in chlorine in the earlier period.}     

Involvement of the Brewer–Dobson circulation in changes of stratospheric temperature and ozone

Wintertime temperature and ozone in the Northern Hemisphere stratosphere vary significantly between years. Largely random, those variations are marked by compensating changes at high and low latitudes, a feature that reflects the residual mean circulation of the stratosphere. Interannual changes of temperature and ozone each track anomalous forcing of the residual circulation. This relationship is shown to be obeyed even over the Arctic, where transport is augmented by heterogeneous chemical processes that destroy ozone. Chlorine activation obeys a similar relationship, reflecting feedback between changes of the residual circulation and anomalous photochemistry.Changes of stratospheric dynamical and chemical structure are found be accompanied by coherent changes in the troposphere. Vertically extensive, they reflect inter-dependent changes in the stratosphere and troposphere, which are coupled by the residual circulation through transfers of mass. The corresponding structure is shown to share major features with empirical modes of interannual variability associated with the AO and its cousin, the NAO.A 3D model of dynamics and photochemistry is used to simulate anomalous temperature and ozone. Driven by anomalous wave activity representative of that observed, the model reproduces the salient structure of observed interannual changes. Anomalous temperature and ozone follow in the integrations from anomalous downwelling, which, under disturbed conditions, renders temperature over the Arctic anomalously warm, and from anomalous poleward transport, which renders Arctic ozone anomalously rich.Accompanying random interannual changes in the observed record was a systematic decline of Northern Hemisphere temperature and ozone during the 1980s and early 1990s. Comprising decadal trends, these systematic changes are shown to have the same essential structure and seasonality as random changes, which, in turn, vary coherently with anomalous forcing of the residual circulation. Implications of the findings to the interpretation of stratospheric trends are discussed in light of anomalous residual motion, photochemistry, and feedback between them.     

Impacts of Future NOx and CO Emissions on Regional Chemistry and Climate over Eastern China

A coupled chemical/dynamical model (SOCOL-SOlar Climate Ozone Links) is applied to study the impacts of future enhanced CO and NOx emissions over eastern China on regional chemistry and climate. The result shows that the increase of CO and NOx emissions has significant effects on regional chemistry, including NOx, CO, O₃, and OH concentrations. During winter, the CO concentration is uniformly increased in the northern hemisphere by about 10 ppbv. During summer, the increase of CO has a regional distribution. The change in O₃, concentrations near eastern China has both strong seasonal and spatial variations. During winter, the surface O₃, concentrations decrease by about 2 ppbv, while during summer they increase by about 2 ppbv in eastern China. The changes of CO, NOx, and O₃, induce important impacts on OH concentrations. The changes in chemistry, especially O₃, induce important effects on regional climate. The analysis suggests that during winter, the surface temperature decreases and air pressure increases in central-eastern China. The changes of temperature and pressure produce decreases in vertical velocity. We should mention that the model resolution is coarse, and the calculated concentrations are generally underestimated when they are compared to measured results. However, because this model is a coupled dynamical/chemical model, it can provide some useful insights regarding the climate impacts due to changes in air pollutant emissions.     

On aspects of the concept of radiative forcing

 The concept of radiative forcing has been extensively used as an indicator of the potential importance of climate change mechanisms. It allows a first order estimate of the global-mean surface temperature change; and it is possible to compare forcings from different mechanisms, on the assumption that similar global-mean forcings produce similar global-mean surface temperature changes. This study illustrates two circumstances where simple models show that the conventional definition of radiative forcing needs refining. These problems arise mainly with the calculation of forcing due to stratospheric ozone depletion. The first part uses simple arguments to produce an alternative definition of radiative forcing, using a time-dependent stratospheric adjustment method, which can give different forcings from those calculated using the standard definition. A seasonally varying ozone depletion can produce a quite different seasonal evolution of forcing than fixed dynamical heating arguments would suggest. This is especially true of an idealised and extreme “Antarctic ozone hole” type scenario where a sudden loss of ozone is followed by a sudden recovery. However, for observed ozone changes the annually averaged forcing is usually within 5% of the forcing calculated using the fixed dynamical heating approximation. Another problem with the accepted view of radiative forcing arises from the definition of the tropopause considered in the second part of this study. For a correct radiative forcing estimate the “tropopause” needs to separate the atmosphere into regions with a purely radiative response and those with a radiative-convective response. From radiative-convective model results it is found that radiative equilibrium conditions persist for several kilometres below the tropopause (the tropopause being defined as where the lapse rate reaches 2 K km^-1). This region needs to be included in stratospheric adjustment calculations for an accurate calculation of forcing, as it is only the region between the surface and the top of the convection that can be considered as a single, forced, system. Including temperature changes in this region has a very large effect on stratospheric ozone forcing estimates, and can reduce the magnitude of the forcing by more than a factor of two. Although these experiments are performed using simple climate models, the results are of equal importance for the analysis of forcing-response relationships using general circulation models. Received: 25 October 1996/Accepted: 14 April 1997     

Solar ultraviolet absorption by sulphur dioxide in Thessaloniki,Greece

Abstract

This work presents the climatology of the sulphur dioxide column over Thessaloniki derived from three years of observation with the Brewer spectrophotometer. The SO₂ column averages 2.5 m atm‐cm and the shielding of UV‐B by SO₂ is investigated and compared with the changes in shielding resulting from an anticipated ozone reduction. Columnar and surface SO₂ concentrations over Thessaloniki appear to be typical of those in major industrial‐urban regions of the world. It is concluded that, for urban regions, predictions of changes in UV‐B as a result of man's activities must consider projections of changes in the SO₂ column as well as ozone.     

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).     

The UVic earth system climate model: Model description,climatology, and applications to past,present and future climates

Abstract

A new earth system climate model of intermediate complexity has been developed and its climatology compared to observations. The UVic Earth System Climate Model consists of a three‐dimensional ocean general circulation model coupled to a thermodynamic/dynamic sea‐ice model, an energy‐moisture balance atmospheric model with dynamical feedbacks, and a thermomechanical land‐ice model. In order to keep the model computationally efficient a reduced complexity atmosphere model is used. Atmospheric heat and freshwater transports are parametrized through Fickian diffusion, and precipitation is assumed to occur when the relative humidity is greater than 85%. Moisture transport can also be accomplished through advection if desired. Precipitation over land is assumed to return instantaneously to the ocean via one of 33 observed river drainage basins. Ice and snow albedo feedbacks are included in the coupled model by locally increasing the prescribed latitudinal profile of the planetary albedo. The atmospheric model includes a parametrization of water vapour/planetary longwave feedbacks, although the radiative forcing associated with changes in atmospheric CO₂ is prescribed as a modification of the planetary longwave radiative flux. A specified lapse rate is used to reduce the surface temperature over land where there is topography. The model uses prescribed present‐day winds in its climatology, although a dynamical wind feedback is included which exploits a latitudinally‐varying empirical relationship between atmospheric surface temperature and density. The ocean component of the coupled model is based on the Geophysical Fluid Dynamics Laboratory (GFDL) Modular Ocean Model 2.2, with a global resolution of 3.6° (zonal) by 1.8° (meridional) and 19 vertical levels, and includes an option for brine‐rejection parametrization. The sea‐ice component incorporates an elastic‐viscous‐plastic rheology to represent sea‐ice dynamics and various options for the representation of sea‐ice thermodynamics and thickness distribution. The systematic comparison of the coupled model with observations reveals good agreement, especially when moisture transport is accomplished through advection.

Global warming simulations conducted using the model to explore the role of moisture advection reveal a climate sensitivity of 3.0°C for a doubling of CO₂, in line with other more comprehensive coupled models. Moisture advection, together with the wind feedback, leads to a transient simulation in which the meridional overturning in the North Atlantic initially weakens, but is eventually re‐established to its initial strength once the radiative forcing is held fixed, as found in many coupled atmosphere General Circulation Models (GCMs). This is in contrast to experiments in which moisture transport is accomplished through diffusion whereby the overturning is reestablished to a strength that is greater than its initial condition.

When applied to the climate of the Last Glacial Maximum (LGM), the model obtains tropical cooling (30°N‐30°S), relative to the present, of about 2.1°C over the ocean and 3.6°C over the land. These are generally cooler than CLIMAP estimates, but not as cool as some other reconstructions. This moderate cooling is consistent with alkenone reconstructions and a low to medium climate sensitivity to perturbations in radiative forcing. An amplification of the cooling occurs in the North Atlantic due to the weakening of North Atlantic Deep Water formation. Concurrent with this weakening is a shallowing of, and a more northward penetration of, Antarctic Bottom Water.

Climate models are usually evaluated by spinning them up under perpetual present‐day forcing and comparing the model results with present‐day observations. Implicit in this approach is the assumption that the present‐day observations are in equilibrium with the present‐day radiative forcing. The comparison of a long transient integration (starting at 6 KBP), forced by changing radiative forcing (solar, CO₂, orbital), with an equilibrium integration reveals substantial differences. Relative to the climatology from the present‐day equilibrium integration, the global mean surface air and sea surface temperatures (SSTs) are 0.74°C and 0.55°C colder, respectively. Deep ocean temperatures are substantially cooler and southern hemisphere sea‐ice cover is 22% greater, although the North Atlantic conveyor remains remarkably stable in all cases. The differences are due to the long timescale memory of the deep ocean to climatic conditions which prevailed throughout the late Holocene. It is also demonstrated that a global warming simulation that starts from an equilibrium present‐day climate (cold start) underestimates the global temperature increase at 2100 by 13% when compared to a transient simulation, under historical solar, CO₂ and orbital forcing, that is also extended out to 2100. This is larger (13% compared to 9.8%) than the difference from an analogous transient experiment which does not include historical changes in solar forcing. These results suggest that those groups that do not account for solar forcing changes over the twentieth century may slightly underestimate (～3% in our model) the projected warming by the year 2100.     

Nonlinear Dynamics in Atmospheric Chemistry Rate Equations

Nonlinear terms in the gas-phase rate equations of atmospheric trace constituents give rise to unexpected oscillations in the concentrations. For a simplified chemical scheme of the troposphere that contains only the generic reaction paths, the underlying dynamical structure is investigated. It is shown that the source strengths of CO and NO are the controlling parameters of the system. A linear stability analysis reveals that the steady state solutions lose stability due to the occurrence of two Hopf bifurcations. Furthermore, it appears that the dynamical behaviour of the oscillatory solutions is dominated by O₃ and CO. Based on the two-variable system (CO–O₃) it is shown that the oscillatory solution involves an autocatalytic ozone production phase which is followed by a phase in which CO is oxidised quickly. A simple expression is presented from which the period of the oscillation can be obtained. The implications for the present troposphere are unclear, since other hydrocarbons are present and transport is taking place. Nevertheless, the system nicely shows the general nonlinear mechanisms that operate in the tropospheric chemistry equations.     

MANTRA ‐ A Balloon Mission to Study the Odd‐Nitrogen Budget of the Stratosphere

Abstract

The Middle Atmosphere Nitrogen TRend Assessment (MANTRA) series of high‐altitude balloon flights is being undertaken to investigate changes in the concentrations of northern hemisphere mid‐latitude stratospheric ozone, and of nitrogen and chlorine compounds that play a role in ozone chemistry. Four campaigns have been carried out to date, all from Vanscoy, Saskatchewan, Canada (52°01'N, 107°02'W, 511.0 m). The first MANTRA mission took place in August 1998, with the balloon flight on 24 August 1998 being the first Canadian launch of a large high‐altitude balloon in about fifteen years. The balloon carried a payload of instruments to measure atmospheric composition, and made measurements from a float altitude of 32–38 km for one day. Three of these instruments had been flown on the Stratoprobe flights of the Atmospheric Environment Service (now the Meteorological Service of Canada) in the 1970s and early 1980s, providing a link to historical data predating the onset of mid‐latitude ozone loss.

The primary measurements obtained from the balloon‐borne instruments were vertical profiles of ozone, NO₂, HNO₃, HCl, CFC‐11, CFC‐12, N₂O, CH₄, temperature, and aerosol backscatter. Total column measurements of ozone, NO₂, SO₂, and aerosol optical depth were made by three ground‐based spectrometers deployed during the campaign. Regular ozonesonde and radiosonde launches were also conducted during the two weeks prior to the main launch in order to characterize the local atmospheric conditions (winds, pressure, temperature, humidity) in the vicinity of the primary balloon flight. The data have been compared with the Model for Evaluating oZONe Trends (MEZON) chemical transport model, the University of California at Irvine photochemical box model, and the Canadian Middle Atmosphere Model (CMAM) to test our current understanding of model photochemistry and mid‐latitude species correlations. This paper provides an overview of the MANTRA 1998 mission, and serves as an introduction to the accompanying papers in this issue of Atmosphere‐Ocean that describe specific aspects and results of this campaign.     

Chemistry–Climate Interactions of Stratospheric and Mesospheric Ozone in EMAC Long-Term Simulations with Different Boundary Conditions for CO2, CH4, N2O,and ODS

Abstract

To evaluate future climate change in the middle atmosphere and the chemistry–climate interaction of stratospheric ozone, we performed a long-term simulation from 1960 to 2050 with boundary conditions from the Intergovernmental Panel on Climate Change A1B greenhouse gas scenario and the World Meteorological Organization Ab halogen scenario using the chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). In addition to this standard simulation we performed five sensitivity simulations from 2000 to 2050 using the rerun files of the simulation mentioned above. For these sensitivity simulations we used the same model setup as in the standard simulation but changed the boundary conditions for carbon dioxide (CO₂), methane (CH₄), nitrous oxide (N₂O), and ozone-depleting substances (ODS). In the first sensitivity simulation we fixed the mixing ratios of CO₂, CH₄, and N₂O in the boundary conditions to the amounts for 2000. In each of the four other sensitivity simulations we fixed the boundary conditions of only one of CO₂, CH₄, N₂O, or ODS to the year 2000.

In our model simulations the future evolution of greenhouse gases leads to significant cooling in the stratosphere and mesosphere. Increasing CO₂ mixing ratios make the largest contributions to this radiative cooling, followed by increasing stratospheric CH₄, which also forms additional H₂O in the upper stratosphere and mesosphere. Increasing N₂O mixing ratios makes the smallest contributions to the cooling. The simulated ozone recovery leads to warming of the middle atmosphere.

In the EMAC model the future development of ozone is influenced by several factors. 1) Cooler temperatures lead to an increase in ozone in the upper stratosphere. The strongest contribution to this ozone production is cooling due to increasing CO₂ mixing ratios, followed by increasing CH₄. 2) Decreasing ODS mixing ratios lead to ozone recovery, but the contribution to the total ozone increase in the upper stratosphere is only slightly higher than the contribution of the cooling by greenhouse gases. In the polar lower stratosphere a decrease in ODS is mainly responsible for ozone recovery. 3) Higher NO_x and HO_x mixing ratios due to increased N₂O and CH₄ lead to intensified ozone destruction, primarily in the middle and upper stratosphere, from additional NO_x; in the mesosphere the intensified ozone destruction is caused by additional HO_x. In comparison to the increase in ozone due to decreasing ODS, ozone destruction caused by increased NO_x is of similar importance in some regions, especially in the middle stratosphere. 4) In the stratosphere the enhancement of the Brewer-Dobson circulation leads to a change in ozone transport. In the polar stratosphere increased downwelling leads to additional ozone in the future, especially at high northern latitudes. The dynamical impact on ozone development is higher at some altitudes in the polar stratosphere than the ozone increase due to cooler temperatures. In the tropical lower stratosphere increased residual vertical upward transport leads to a decrease in ozone.     

Climate change, ambient ozone, and health in 50 US cities

We investigated how climate change could affect ambient ozone concentrations and the subsequent human health impacts. Hourly concentrations were estimated for 50 eastern US cities for five representative summers each in the 1990s and 2050s, reflecting current and projected future climates, respectively. Estimates of future concentrations were based on the IPCC A2 scenario using global climate, regional climate, and regional air quality models. This work does not explore the effects of future changes in anthropogenic emissions, but isolates the impact of altered climate on ozone and health. The cities’ ozone levels are estimated to increase under predicted future climatic conditions, with the largest increases in cities with present-day high pollution. On average across the 50 cities, the summertime daily 1-h maximum increased 4.8 ppb, with the largest increase at 9.6 ppb. The average number of days/summer exceeding the 8-h regulatory standard increased 68%. Elevated ozone levels correspond to approximately a 0.11% to 0.27% increase in daily total mortality. While actual future ozone concentrations depend on climate and other influences such as changes in emissions of anthropogenic precursors, the results presented here indicate that with other factors constant, climate change could detrimentally affect air quality and thereby harm human health.