Operational retrieval of total and tropospheric ozone from IASI infrared measurements

info:eu-repo/semantics/nonPublished

Tropospheric ozone and winter wheat production in England and Wales: A note

Tropospheric ozone is an air pollutant thought to reduce crop yields across Europe. Much experimental scientific work has been completed or is currently underway to quantify yield effects at ambient ozone levels. In this research, we seek to directly evaluate whether such effects are observed at the farm level. This is done by intersecting a farm level panel dataset for winter wheat farms in England & Wales with information on ambient ozone, and estimating a production function with ozone as a fixed input. Panel data methods, Generalised Method of Moments (GMM) techniques and nested exogeneity tests are employed in the estimation. The results confirm a small, but nevertheless statistically significant negative effect of ambient ozone levels on wheat yields.

Contributions to twentieth century total column ozone change from halocarbons, tropospheric ozone precursors, and climate change

We investigate ozone changes from preindustrial times to the present using a chemistry-climate model. The influence of changes in physical climate, ozone-depleting substances, N2O, and tropospheric ozone precursors is estimated using equilibrium simulations with these different factors set at either preindustrial or present-day values. When these effects are combined, the entire decrease in total column ozone from preindustrial to present day is very small (–1.8 DU) in the global annual average, though with significant decreases in total column ozone over large parts of the Southern Hemisphere during austral spring and widespread increases in column ozone over the Northern Hemisphere during boreal summer. A significant contribution to the total ozone column change is the increase in lower stratospheric ozone associated with the increase in ozone precursors (5.9 DU). Also noteworthy is the near cancellation of the global average climate change effect on ozone (3.5 DU) by the increase in N2O (–3.9 DU).

Development of a sensitive passive sampler using indigotrisulfonate for the determination of tropospheric ozone

Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)

Tropospheric ozone and CO over North Atlantic for the past decade

We investigate how declines in US emissions of CO and O3 precursors have impacted the lower free troposphere over the North Atlantic. We use seasonal observations for O3 and CO from the PICO-NARE project for the period covering 2001 to 2010. Observations are used to verify model output generated by the GEOS-Chem 3-D global chemical transport model. Additional satellite data for CO from AIRS/Aqua and for O3 from TES/Aura were also used to provide additional comparisons; particularly for fall, winter, and spring when PICO-NARE coverage is sparse. We find GEOS-Chem captures the seasonal cycle for CO and O3 well compared to PICO-NARE data. For CO, GEOS-Chem is biased low, particularly in spring which is in agreement with findings from previous studies. GEOS-Chem is 24.7 +/- 5.2 ppbv (1-σ) low compared to PICO-NARE summer CO data while AIRS is 14.2 +/- 6.6 ppbv high. AIRS does not show nearly as much variation as seen with GEOS-Chem or the Pico data, and goes from being lower than PICO-NARE data in winter and spring, to higher in summer and fall. Both TES and GEOS-Chem match the seasonal ozone cycle well for all seasons when compared with observations. Model results for O3 show GEOS-Chem is 6.67 +/- 2.63 ppbv high compared to PICO-NARE summer measurements and TES was 3.91 +/- 4.2 ppbv higher. Pico data, model results, and AIRS all show declines in CO and O3 for the summer period from 2001 to 2010. Limited availability of TES data prevents us from using it in trend analysis. For summer CO Pico, GEOS-Chem, and AIRS results show declines of 1.32, 0.368, and 0.548 ppbv/year respectively. For summer O3, Pico and GEOS-Chem show declines of -0.726 and -0.583 ppbv/year respectively. In other seasons, both model and AIRS show declining CO, particularly in the fall. GEOS-Chem results show a fall decline of 0.798 ppbv/year and AIRS shows a decline of 0.8372 ppbv/year. Winter and spring CO declines are 0.393 and 0.307 for GEOS-Chem, and 0.455 and 0.566 for AIRS. GEOS-Chem shows declining O3 in other seasons as well; with fall being the season of greatest decrease and winter being the least. Model results for fall, winter, and spring are 0.856, 0.117, and 0.570 ppbv/year respectively. Given the availability of data we are most confident in summer results and thus find that summer CO and O3 have declined in lower free troposphere of the North Atlantic region of the Azores. Sensitivity studies for CO and O3 at Pico were conducted by turning off North American fossil fuel emissions in GEOS-Chem. Model results show that North America fossil fuel emissions contribute 8.57 ppbv CO and 4.03 ppbv O3 to Pico. The magnitude of modeled trends declines in all seasons without North American fossil fuel emissions except for summer CO. The increase in summer CO declines may be due to a decline of 5.24 ppbv/year trend in biomass burning emissions over the study period; this is higher than the 2.33 ppbv/year North American anthropogenic CO model decline. Winter O3 is the only season which goes from showing a negative trend to a positive trend.

Photochemistry and transport of tropospheric ozone and its precursors in urban and remote environments

Tropospheric ozone (O3) adversely affects human health, reduces crop yields, and contributes to climate forcing. To limit these effects, the processes controlling O3 abundance as well as that of its precursor molecules must be fully characterized. Here, I examine three facets of O3 production, both in heavily polluted and remote environments. First, using in situ observations from the DISCOVER-AQ field campaign in the Baltimore/Washington region, I evaluate the emissions of the O3 precursors CO and NOx (NOx = NO + NO2) in the National Emissions Inventory (NEI). I find that CO/NOx emissions ratios derived from observations are 21% higher than those predicted by the NEI. Comparisons to output from the CMAQ model suggest that CO in the NEI is accurate within 15 ± 11%, while NOx emissions are overestimated by 51-70%, likely due to errors in mobile sources. These results imply that ambient ozone concentrations will respond more efficiently to NOx controls than current models suggest. I then investigate the source of high O3 and low H2O structures in the Tropical Western Pacific (TWP). A combination of in situ observations, satellite data, and models show that the high O3 results from photochemical production in biomass burning plumes from fires in tropical Southeast Asia and Central Africa; the low relative humidity results from large-scale descent in the tropics. Because these structures have frequently been attributed to mid-latitude pollution, biomass burning in the tropics likely contributes more to the radiative forcing of climate than previously believed. Finally, I evaluate the processes controlling formaldehyde (HCHO) in the TWP. Convective transport of near surface HCHO leads to a 33% increase in upper tropospheric HCHO mixing ratios; convection also likely increases upper tropospheric CH3OOH to ~230 pptv, enough to maintain background HCHO at ~75 pptv. The long-range transport of polluted air, with NO four times the convectively controlled background, intensifies the conversion of HO2 to OH, increasing OH by a factor of 1.4. Comparisons between the global chemistry model CAM-Chem and observations show that consistent underestimates of HCHO by CAM-Chem throughout the troposphere result from underestimates in both NO and acetaldehyde.

Contrasting fast precipitation responses to tropospheric and stratospheric ozone forcing

The precipitation response to radiative forcing (RF) can be decomposed into a fast precipitation response (FPR), which depends on the atmospheric component of RF, and a slow response, which depends on surface temperature change. We present the first detailed climate model study of the FPR due to tropospheric and stratospheric ozone changes. The FPR depends strongly on the altitude of ozone change. Increases below about 3 km cause a positive FPR; increases above cause a negative FPR. The FPR due to stratospheric ozone change is, per unit RF, about 3 times larger than that due to tropospheric ozone. As historical ozone trends in the troposphere and stratosphere are opposite in sign, so too are the FPRs. Simple climate model calculations of the time-dependent total (fast and slow) precipitation change, indicate that ozone's contribution to precipitation change in 2011, compared to 1765, could exceed 50% of that due to CO2 change.

Ozone-induced signaling in Arabidopsis thaliana

Tropospheric ozone (O3) is one of the most common air pollutants in industrialized countries, and an increasing problem in rapidly industrialising and developing countries in Asia, Africa and South America. Elevated concentrations of tropospheric O3 can lead to decrease in photosynthesis rate and therefore affect the normal metabolism, growth and seed production. Acute and high O3 episodes can lead to extensive damage leading to dead tissue in plants. Thus, O3 derived growth defects can lead to reduction in crop yield thereby leading to economical losses. Despite the extensive research on this area, many questions remain open on how these processes are controlled. In this study, the stress-induced signaling routes and the components involved were elucidated in more detail starting from visual damage to changes in gene expression, signaling routes and plant hormone interactions that are involved in O3-induced cell death. In order to elucidate O3-induced responses in Arabidopsis, mitogen-activated protein kinase (MAPK) signaling was studied using different hormonal signaling mutants. MAPKs were activated at the beginning of the O3 exposure. The activity of MAPKs, which were identified as AtMPK3 and AtMPK6, reached the maximum at 1 and 2 hours after the start of the exposure, respectively. The activity decreased back to clean air levels at 8 hours after the start of the exposure. Both AtMPK3 and AtMPK6 were translocated to nucleus at the beginning of the O3 exposure where they most likely affect gene expression. Differences were seen between different hormonal signaling mutants. Functional SA signaling was shown to be needed for the full protein levels and activation of AtMPK3. In addition, AtMPK3 and AtMPK6 activation was not dependent on ethylene signaling. Finally, jasmonic acid was also shown to have an impact on AtMPK3 protein levels and AtMPK3 activity. To further study O3-induced cell death, an earlier isolated O3 sensitive Arabidopsis mutant rcd1 was mapped, cloned and further characterized. RCD1 was shown to encode a gene with WWE and ADP-ribosylation domains known to be involved in protein-protein interactions and cell signaling. rcd1 was shown to be involved in many processes including hormonal signaling and regulation of stress-responsive genes. rcd1 is sensitive against O3 and apoplastic superoxide, but tolerant against paraquat that produces superoxide in chloroplast. rcd1 is also partially insensitive to glucose and has alterations in hormone responses. These alterations are seen as ABA insensitivity, reduced jasmonic acid sensitivity and reduced ethylene sensitivity. All these features suggest that RCD1 acts as an integrative node in hormonal signaling and it is involved in the hormonal regulation of several specific stress-responsive genes. Further studies with the rcd1 mutant showed that it exhibits the classical features of programmed cell death, PCD, in response to O3. These include nuclear shrinkage, chromatin condensation, nuclear DNA degradation, cytosol vesiculation and accumulation of phenolic compounds and eventually patches of HR-like lesions. rcd1 was found to produce extensive amount of salicylic acid and jasmonic acid in response to O3. Double mutant studies showed that SA independent and dependent processes were involved in the O3-induced PCD in rcd1 and that increased sensitivity against JA led to increased sensitivity against O3. Furthermore, rcd1 had alterations in MAPK signature that resembled changes that were previously seen in mutants defective in SA and JA signaling. Nitric oxide accumulation and its impact on O3-induced cell death were also studied. Transient accumulation of NO was seen at the beginning of the O3 exposure, and during late time points, NO accumulation coincided with the HR-like lesions. NO was shown to modify defense gene expression, such as, SA and ethylene biosynthetic genes. Furthermore, rcd1 was shown to produce more NO in control conditions. In conclusion, NO was shown to be involved in O3-induced signaling leading to attenuation of SA biosynthesis and other defense related genes.

Spatio-temporal Variability of Atmospheric Ozone over Indian Subcontinent and its Relation to Meteorological Parameters

Ozone present in the atmosphere not only absorbs the biologically harmful ultraviolet radiation but also is an important ingredient of the climate system. The radiative absorption properties of ozone make it a determining factor in the structure of the atmosphere. Ozone in the troposphere has many negative impacts on humans and other living beings. Another significant aspect is the absorption of outgoing infrared radiation by ozone thus acting as a greenhouse gas. The variability of ozone in the atmosphere involves many interconnections with the incoming and outgoing radiation, temperature circulation etc. Hence ozone forms an important part of chemistry-climate as well as radiative transfer models. This aspect also makes the quantification of ozone more important. The discovery of Antarctic ozone hole and the role of anthropogenic activities in causing it made it possible to plan and implement necessary preventive measures. Continuous monitoring of ozone is also necessary to identify the effect of these preventive steps. The reactions involving the formation and destruction of ozone are influenced significantly by the temperature fluctuations of the atmosphere. On the other hand the variations in ozone can change the temperature structure of the atmosphere. Indian subcontinent is a region having large weather and climate variability which is evident from the large interannual variability of monsoon system over the region. Nearly half of Indian region comprises the tropical region. Most of ozone is formed in the tropical region and transported to higher latitudes. The formation and transport of ozone can be influenced by changes in solar radiation and various atmospheric circulation features. Besides industrial activities and vehicular traffic is more due to its large population. This may give rise to an increase in the production of tropospheric ozone which is greenhouse gas. Hence it becomes necessary to monitor the atmospheric ozone over this region. This study probes into the spatial distribution and temporal evolution of ozone over Indian subcontinent and discusses the contributing atmospheric parameters.

Four-dimensional variational assimilation of ozone profiles from the Microwave Limb Sounder on the Aura satellite

Ozone profiles from the Microwave Limb Sounder (MLS) onboard the Aura satellite of the NASA's Earth Observing System (EOS) were experimentally added to the European Centre for Medium-range Weather Forecasts (ECMWF) four-dimensional variational (4D-var) data assimilation system of version CY30R1, in which total ozone columns from Scanning Imaging Absorption Spectrometer for Atmospheric CHartographY (SCIAMACHY) onboard the Envisat satellite and partial profiles from the Solar Backscatter Ultraviolet (SBUV/2) instrument onboard the NOAA-16 satellite have been operationally assimilated. As shown by results for the autumn of 2005, additional constraints from MLS data significantly improved the agreement of the analyzed ozone fields with independent observations throughout most of the stratosphere, owing to the daily near-global coverage and good vertical resolution of MLS observations. The largest impacts were seen in the middle and lower stratosphere, where model deficiencies could not be effectively corrected by the operational observations without the additional information on the ozone vertical distribution provided by MLS. Even in the upper stratosphere, where ozone concentrations are mainly determined by rapid chemical processes, dense and vertically resolved MLS data helped reduce the biases related to model deficiencies. These improvements resulted in a more realistic and consistent description of spatial and temporal variations in stratospheric ozone, as demonstrated by cases in the dynamically and chemically active regions. However, combined assimilation of the often discrepant ozone observations might lead to underestimation of tropospheric ozone. In addition, model deficiencies induced large biases in the upper stratosphere in the medium-range (5-day) ozone forecasts.

Radiative forcing since preindustrial times due to ozone change in the troposphere and the lower stratosphere

Changes in atmospheric ozone have occurred since the preindustrial era as a result of increasing anthropogenic emissions. Within ACCENT, a European Network of Excellence, ozone changes between 1850 and 2000 are assessed for the troposphere and the lower stratosphere ( up to 30 km) by a variety of seven chemistry-climate models and three chemical transport models. The modeled ozone changes are taken as input for detailed calculations of radiative forcing. When only changes in chemistry are considered ( constant climate) the modeled global-mean tropospheric ozone column increase since preindustrial times ranges from 7.9 DU to 13.8 DU among the ten participating models, while the stratospheric column reduction lies between 14.1 DU and 28.6 DU in the models considering stratospheric chemistry. The resulting radiative forcing is strongly dependent on the location and altitude of the modeled ozone change and varies between 0.25 Wm(-2) and 0.45 Wm(-2) due to ozone change in the troposphere and - 0.123 Wm(-2) and + 0.066 Wm(-2) due to the stratospheric ozone change. Changes in ozone and other greenhouse gases since preindustrial times have altered climate. Six out of the ten participating models have performed an additional calculation taking into account both chemical and climate change. In most models the isolated effect of climate change is an enhancement of the tropospheric ozone column increase, while the stratospheric reduction becomes slightly less severe. In the three climate-chemistry models with detailed tropospheric and stratospheric chemistry the inclusion of climate change increases the resulting radiative forcing due to tropospheric ozone change by up to 0.10 Wm(-2), while the radiative forcing due to stratospheric ozone change is reduced by up to 0.034 Wm(-2). Considering tropospheric and stratospheric change combined, the total ozone column change is negative while the resulting net radiative forcing is positive.

The impact of traffic emissions on atmospheric ozone and OH: results from QUANTIFY

To estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH in the present-day atmosphere six different atmospheric chemistry models have been used. Based on newly developed global emission inventories for road, ship and aircraft emission data sets each model performed sensitivity simulations reducing the emissions of each transport sector by 5%. The model results indicate that on global annual average lower tropospheric ozone responds most sensitive to ship emissions (50.6%±10.9% of the total traffic induced perturbation), followed by road (36.7%±9.3%) and aircraft exhausts (12.7%±2.9%), respectively. In the northern upper troposphere between 200–300 hPa at 30–60° N the maximum impact from road and ship are 93% and 73% of the maximum effect of aircraft, respectively. The latter is 0.185 ppbv for ozone (for the 5% case) or 3.69 ppbv when scaling to 100%. On the global average the impact of road even dominates in the UTLS-region. The sensitivity of ozone formation per NOx molecule emitted is highest for aircraft exhausts. The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 0.2 DU and occurs over the northern subtropical Atlantic extending to central Europe. Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine lower troposphere over the Atlantic. Based on the 5% perturbation the effect on ozone can exceed 0.6% close to the marine surface (global zonal mean) which is 80% of the total traffic induced ozone perturbation. In the southern hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%–80% throughout the year. Methane lifetime changes against OH are affected strongest by ship emissions up to 0.21 (± 0.05)%, followed by road (0.08 (±0.01)%) and air traffic (0.05 (± 0.02)%). Based on the full scale ozone and methane perturbations positive radiative forcings were calculated for road emissions (7.3±6.2 mWm−2) and for aviation (2.9±2.3 mWm−2). Ship induced methane lifetime changes dominate over the ozone forcing and therefore lead to a net negative forcing (−25.5±13.2 mWm−2).

Report of the 2010 assessment of the scientific assessment panel: future ozone and its impact on surface UV

SCIENTIFIC SUMMARY Globally averaged total column ozone has declined over recent decades due to the release of ozone-depleting substances (ODSs) into the atmosphere. Now, as a result of the Montreal Protocol, ozone is expected to recover from the effects of ODSs as ODS abundances decline in the coming decades. However, a number of factors in addition to ODSs have led to and will continue to lead to changes in ozone. Discriminating between the causes of past and projected ozone changes is necessary, not only to identify the progress in ozone recovery from ODSs, but also to evaluate the effectiveness of climate and ozone protection policy options. Factors Affecting Future Ozone and Surface Ultraviolet Radiation • At least for the next few decades, the decline of ODSs is expected to be the major factor affecting the anticipated increase in global total column ozone. However, several factors other than ODS will affect the future evolution of ozone in the stratosphere. These include changes in (i) stratospheric circulation and temperature due to changes in long-lived greenhouse gas (GHG) abundances, (ii) stratospheric aerosol loading, and (iii) source gases of highly reactive stratospheric hydrogen and nitrogen compounds. Factors that amplify the effects of ODSs on ozone (e.g., stratospheric aerosols) will likely decline in importance as ODSs are gradually eliminated from the atmosphere. • Increases in GHG emissions can both positively and negatively affect ozone. Carbon dioxide (CO2)-induced stratospheric cooling elevates middle and upper stratospheric ozone and decreases the time taken for ozone to return to 1980 levels, while projected GHG-induced increases in tropical upwelling decrease ozone in the tropical lower stratosphere and increase ozone in the extratropics. Increases in nitrous oxide (N2O) and methane (CH4) concentrations also directly impact ozone chemistry but the effects are different in different regions. • The Brewer-Dobson circulation (BDC) is projected to strengthen over the 21st century and thereby affect ozone amounts. Climate models consistently predict an acceleration of the BDC or, more specifically, of the upwelling mass flux in the tropical lower stratosphere of around 2% per decade as a consequence of GHG abundance increases. A stronger BDC would decrease the abundance of tropical lower stratospheric ozone, increase poleward transport of ozone, and could reduce the atmospheric lifetimes of long-lived ODSs and other trace gases. While simulations showing faster ascent in the tropical lower stratosphere to date are a robust feature of chemistry-climate models (CCMs), this has not been confirmed by observations and the responsible mechanisms remain unclear. • Substantial ozone losses could occur if stratospheric aerosol loading were to increase in the next few decades, while halogen levels are high. Stratospheric aerosol increases may be caused by sulfur contained in volcanic plumes entering the stratosphere or from human activities. The latter might include attempts to geoengineer the climate system by enhancing the stratospheric aerosol layer. The ozone losses mostly result from enhanced heterogeneous chemistry on stratospheric aerosols. Enhanced aerosol heating within the stratosphere also leads to changes in temperature and circulation that affect ozone. • Surface ultraviolet (UV) levels will not be affected solely by ozone changes but also by the effects of climate change and by air quality change in the troposphere. These tropospheric effects include changes in clouds, tropospheric aerosols, surface reflectivity, and tropospheric sulfur dioxide (SO2) and nitrogen dioxide (NO2). The uncertainties in projections of these factors are large. Projected increases in tropospheric ozone are more certain and may lead to reductions in surface erythemal (“sunburning”) irradiance of up to 10% by 2100. Changes in clouds may lead to decreases or increases in surface erythemal irradiance of up to 15% depending on latitude. Expected Future Changes in Ozone Full ozone recovery from the effects of ODSs and return of ozone to historical levels are not synonymous. In this chapter a key target date is chosen to be 1980, in part to retain the connection to previous Ozone Assessments. Noting, however, that decreases in ozone may have occurred in some regions of the atmosphere prior to 1980, 1960 return dates are also reported. The projections reported on in this chapter are taken from a recent compilation of CCM simulations. The ozone projections, which also form the basis for the UV projections, are limited in their representativeness of possible futures since they mostly come from CCM simulations based on a single GHG emissions scenario (scenario A1B of Emissions Scenarios. A Special Report of Working Group III of the Intergovernmental Panel on Climate Change, Cambridge University Press, 2000) and a single ODS emissions scenario (adjusted A1 of the previous (2006) Ozone Assessment). Throughout this century, the vertical, latitudinal, and seasonal structure of the ozone distribution will be different from what it was in 1980. For this reason, ozone changes in different regions of the atmosphere are considered separately. • The projections of changes in ozone and surface clear-sky UV are broadly consistent with those reported on in the 2006 Assessment. • The capability of making projections and attribution of future ozone changes has been improved since the 2006 Assessment. Use of CCM simulations from an increased number of models extending through the entire period of ozone depletion and recovery from ODSs (1960–2100) as well as sensitivity simulations have allowed more robust projections of long-term changes in the stratosphere and of the relative contributions of ODSs and GHGs to those changes. • Global annually averaged total column ozone is projected to return to 1980 levels before the middle of the century and earlier than when stratospheric halogen loading returns to 1980 levels. CCM projections suggest that this early return is primarily a result of GHG-induced cooling of the upper stratosphere because the effects of circulation changes on tropical and extratropical ozone largely cancel. Global (90°S–90°N) annually averaged total column ozone will likely return to 1980 levels between 2025 and 2040, well before the return of stratospheric halogens to 1980 levels between 2045 and 2060. • Simulated changes in tropical total column ozone from 1960 to 2100 are generally small. The evolution of tropical total column ozone in models depends on the balance between upper stratospheric increases and lower stratospheric decreases. The upper stratospheric increases result from declining ODSs and a slowing of ozone destruction resulting from GHG-induced cooling. Ozone decreases in the lower stratosphere mainly result from an increase in tropical upwelling. From 1960 until around 2000, a general decline is simulated, followed by a gradual increase to values typical of 1980 by midcentury. Thereafter, although total column ozone amounts decline slightly again toward the end of the century, by 2080 they are no longer expected to be affected by ODSs. Confidence in tropical ozone projections is compromised by the fact that simulated decreases in column ozone to date are not supported by observations, suggesting that significant uncertainties remain. • Midlatitude total column ozone is simulated to evolve differently in the two hemispheres. Over northern midlatitudes, annually averaged total column ozone is projected to return to 1980 values between 2015 and 2030, while for southern midlatitudes the return to 1980 values is projected to occur between 2030 and 2040. The more rapid return to 1980 values in northern midlatitudes is linked to a more pronounced strengthening of the poleward transport of ozone due to the effects of increased GHG levels, and effects of Antarctic ozone depletion on southern midlatitudes. By 2100, midlatitude total column ozone is projected to be above 1980 values in both hemispheres. • October-mean Antarctic total column ozone is projected to return to 1980 levels after midcentury, later than in any other region, and yet earlier than when stratospheric halogen loading is projected to return to 1980 levels. The slightly earlier return of ozone to 1980 levels (2045–2060) results primarily from upper stratospheric cooling and resultant increases in ozone. The return of polar halogen loading to 1980 levels (2050–2070) in CCMs is earlier than in empirical models that exclude the effects of GHG-induced changes in circulation. Our confidence in the drivers of changes in Antarctic ozone is higher than for other regions because (i) ODSs exert a strong influence on Antarctic ozone, (ii) the effects of changes in GHG abundances are comparatively small, and (iii) projections of ODS emissions are more certain than those for GHGs. Small Antarctic ozone holes (areas of ozone <220 Dobson units, DU) could persist to the end of the 21st century. • March-mean Arctic total column ozone is projected to return to 1980 levels two to three decades before polar halogen loading returns to 1980 levels, and to exceed 1980 levels thereafter. While CCM simulations project a return to 1980 levels between 2020 and 2035, most models tend not to capture observed low temperatures and thus underestimate present-day Arctic ozone loss such that it is possible that this return date is biased early. Since the strengthening of the Brewer-Dobson circulation through the 21st century leads to increases in springtime Arctic column ozone, by 2100 Arctic ozone is projected to lie well above 1960 levels. Uncertainties in Projections • Conclusions dependent on future GHG levels are less certain than those dependent on future ODS levels since ODS emissions are controlled by the Montreal Protocol. For the six GHG scenarios considered by a few CCMs, the simulated differences in stratospheric column ozone over the second half of the 21st century are largest in the northern midlatitudes and the Arctic, with maximum differences of 20–40 DU between the six scenarios in 2100. • There remain sources of uncertainty in the CCM simulations. These include the use of prescribed ODS mixing ratios instead of emission fluxes as lower boundary conditions, the range of sea surface temperatures and sea ice concentrations, missing tropospheric chemistry, model parameterizations, and model climate sensitivity. • Geoengineering schemes for mitigating climate change by continuous injections of sulfur-containing compounds into the stratosphere, if implemented, would substantially affect stratospheric ozone, particularly in polar regions. Ozone losses observed following large volcanic eruptions support this prediction. However, sporadic volcanic eruptions provide limited analogs to the effects of continuous sulfur emissions. Preliminary model simulations reveal large uncertainties in assessing the effects of continuous sulfur injections. Expected Future Changes in Surface UV. While a number of factors, in addition to ozone, affect surface UV irradiance, the focus in this chapter is on the effects of changes in stratospheric ozone on surface UV. For this reason, clear-sky surface UV irradiance is calculated from ozone projections from CCMs. • Projected increases in midlatitude ozone abundances during the 21st century, in the absence of changes in other factors, in particular clouds, tropospheric aerosols, and air pollutants, will result in decreases in surface UV irradiance. Clear-sky erythemal irradiance is projected to return to 1980 levels on average in 2025 for the northern midlatitudes, and in 2035 for the southern midlatitudes, and to fall well below 1980 values by the second half of the century. However, actual changes in surface UV will be affected by a number of factors other than ozone. • In the absence of changes in other factors, changes in tropical surface UV will be small because changes in tropical total column ozone are projected to be small. By the middle of the 21st century, the model projections suggest surface UV to be slightly higher than in the 1960s, very close to values in 1980, and slightly lower than in 2000. The projected decrease in tropical total column ozone through the latter half of the century will likely result in clear-sky surface UV remaining above 1960 levels. Average UV irradiance is already high in the tropics due to naturally occurring low total ozone columns and high solar elevations. • The magnitude of UV changes in the polar regions is larger than elsewhere because ozone changes in polar regions are larger. For the next decades, surface clear-sky UV irradiance, particularly in the Antarctic, will continue to be higher than in 1980. Future increases in ozone and decreases in clear-sky UV will occur at slower rates than those associated with the ozone decreases and UV increases that occurred before 2000. In Antarctica, surface clear-sky UV is projected to return to 1980 levels between 2040 and 2060, while in the Arctic this is projected to occur between 2020 and 2030. By 2100, October surface clear-sky erythemal irradiance in Antarctica is likely to be between 5% below to 25% above 1960 levels, with considerable uncertainty. This is consistent with multi-model-mean October Antarctic total column ozone not returning to 1960 levels by 2100. In contrast, by 2100, surface clear-sky UV in the Arctic is projected to be 0–10% below 1960 levels.

Large climate-induced changes in ultraviolet index and stratosphere-to-troposphere ozone flux

Now that stratospheric ozone depletion has been controlled by the Montreal Protocol1, interest has turned to the effects of climate change on the ozone layer. Climate models predict an accelerated stratospheric circulation, leading to changes in the spatial distribution of stratospheric ozone and an increased stratosphere-to-troposphere ozone flux. Here we use an atmospheric chemistry climate model to isolate the effects of climate change from those of ozone depletion and recovery on stratosphere-to-troposphere ozone flux and the clear-sky ultraviolet radiation index—a measure of potential human exposure to ultraviolet radiation. We show that under the Intergovernmental Panel on Climate Change moderate emissions scenario, global stratosphere-to- troposphere ozone flux increases by 23% between 1965 and 2095 as a result of climate change. During this time, the clear-sky ultraviolet radiation index decreases by 9% in northern high latitudes — a much larger effect than that of stratospheric ozone recovery — and increases by 4% in the tropics, and by up to 20% in southern high latitudes in late spring and early summer. The latter increase in the ultraviolet index is equivalent to nearly half of that generated by the Antarctic ‘ozone hole’ that was created by anthropogenic halogens. Our results suggest that climate change will alter the tropospheric ozone budget and the ultraviolet index, which would have consequences for tropospheric radiative forcing, air quality and human and ecosystem health.

Transient climate change simulations with a coupled atmosphere–ocean GCM including the tropospheric sulfur cycle

The time-dependent climate response to changing concentrations of greenhouse gases and sulfate aerosols is studied using a coupled general circulation model of the atmosphere and the ocean (ECHAM4/OPYC3). The concentrations of the well-mixed greenhouse gases like CO2, CH4, N2O, and CFCs are prescribed for the past (1860–1990) and projected into the future according to International Panel on Climate Change (IPCC) scenario IS92a. In addition, the space–time distribution of tropospheric ozone is prescribed, and the tropospheric sulfur cycle is calculated within the coupled model using sulfur emissions of the past and projected into the future (IS92a). The radiative impact of the aerosols is considered via both the direct and the indirect (i.e., through cloud albedo) effect. It is shown that the simulated trend in sulfate deposition since the end of the last century is broadly consistent with ice core measurements, and the calculated radiative forcings from preindustrial to present time are within the uncertainty range estimated by IPCC. Three climate perturbation experiments are performed, applying different forcing mechanisms, and the results are compared with those obtained from a 300-yr unforced control experiment. As in previous experiments, the climate response is similar, but weaker, if aerosol effects are included in addition to greenhouse gases. One notable difference to previous experiments is that the strength of the Indian summer monsoon is not fundamentally affected by the inclusion of aerosol effects. Although the monsoon is damped compared to a greenhouse gas only experiment, it is still more vigorous than in the control experiment. This different behavior, compared to previous studies, is the result of the different land–sea distribution of aerosol forcing. Somewhat unexpected, the intensity of the global hydrological cycle becomes weaker in a warmer climate if both direct and indirect aerosol effects are included in addition to the greenhouse gases. This can be related to anomalous net radiative cooling of the earth’s surface through aerosols, which is balanced by reduced turbulent transfer of both sensible and latent heat from the surface to the atmosphere.