Identifying human influences on atmospheric temperature

We perform a multimodel detection and attribution study with climate model simulation output and satellite-based measurements of tropospheric and stratospheric temperature change. We use simulation output from 20 climate models participating in phase 5 of the Coupled Model Intercomparison Project. This multimodel archive provides estimates of the signal pattern in response to combined anthropogenic and natural external forcing (the finger-print) and the noise of internally generated variability. Using these estimates, we calculate signal-to-noise (S/N) ratios to quantify the strength of the fingerprint in the observations relative to fingerprint strength in natural climate noise. For changes in lower stratospheric temperature between 1979 and 2011, S/N ratios vary from 26 to 36, depending on the choice of observational dataset. In the lower troposphere, the fingerprint strength in observations is smaller, but S/N ratios are still significant at the 1% level or better, and range from three to eight. We find no evidence that these ratios are spuriously inflated by model variability errors. After removing all global mean signals, model fingerprints remain identifiable in 70% of the tests involving tropospheric temperature changes. Despite such agreement in the large-scale features of model and observed geographical patterns of atmospheric temperature change, most models do not replicate the size of the observed changes. On average, the models analyzed underestimate the observed cooling of the lower stratosphere and overestimate the warming of the troposphere. Although the precise causes of such differences are unclear, model biases in lower stratospheric temperature trends are likely to be reduced by more realistic treatment of stratospheric ozone depletion and volcanic aerosol forcing.

The kinetics of the gas-phase reactions of selected monoterpenes and cyclo-alkenes with ozone and the NO3 radical

The relative rate method has been used to measure the room-temperature rate constants for the gasphase reactions of ozone and NO3 with selected monoterpenes and cyclo-alkenes with structural similarities to monoterpenes. Measurements were carried out at 298 ! 2 K and 760 ! 10 Torr. The following rate constants (in units of 10"18 cm3 molecule"1 s"1) were obtained for the reaction with ozone: methyl cyclohexene (132 ! 17), terpinolene (1290 ! 360), ethylidene cyclohexane (223 ! 57), norbornene (860 ! 240), t-butyl isopropylidene cyclohexane (1500 ! 460), cyclopentene (543 ! 94), cyclohexene (81 ! 18), cyclooctene (451 ! 66), dicyclopentadiene (1460 ! 170) and a-pinene (107 ! 13). For the reaction with NO3 the rate constants obtained (in units of 10"12 cm3 molecule"1 s"1) were: methyl cyclohexene (7.92 ! 0.95), terpinolene (47.9 ! 4.0), ethylidene cyclohexane (4.30 ! 0.24), norbornene (0.266 ! 0.029), cyclohexene (0.540 ! 0.017), cyclooctene (0.513 ! 0.029), dicyclopentadiene (1.20 ! 0.10) and a-pinene (5.17 ! 0.62). Errors are quoted as the root mean square of the statistical error (95% con!dence) and the quoted error in the rate constant for the reference compound. Combining these results with previous studies, new recommendations for the rate constants are presented. Molecular orbital energies were calculated for each alkene and the kinetic data are discussed in terms of the deviation from the structureeactivity relationship obtained from the rate constants for a series of simple alkenes. Lifetimes with respect to key initiators of atmospheric oxidation have been calculated suggesting that the studied reactions play dominant roles in the night-time removal of these compounds from the atmosphere.

Comment on "Tropospheric temperature response to stratospheric ozone recovery in the 21st century" by Hu et al. (2011)

Abstract. In a recent paper Hu et al. (2011) suggest that the recovery of stratospheric ozone during the first half of this century will significantly enhance free tropospheric and surface warming caused by the anthropogenic increase of greenhouse gases, with the effects being most pronounced in Northern Hemisphere middle and high latitudes. These surprising results are based on a multi-model analysis of CMIP3 model simulations with and without prescribed stratospheric ozone recovery. Hu et al. suggest that in order to properly quantify the tropospheric and surface temperature response to stratospheric ozone recovery, it is necessary to run coupled atmosphere-ocean climate models with stratospheric ozone chemistry. The results of such an experiment are presented here, using a state-of-the-art chemistry-climate model coupled to a three-dimensional ocean model. In contrast to Hu et al., we find a much smaller Northern Hemisphere tropospheric temperature response to ozone recovery, which is of opposite sign. We suggest that their result is an artifact of the incomplete removal of the large effect of greenhouse gas warming between the two different sets of models.

Influence of the Antarctic ozone hole on the polar mesopause region as simulated by the Canadian Middle Atmosphere Model

It is well established that variations in polar stratospheric winds can affect mesospheric temperatures through changes in the filtering of gravity wave fluxes, which drive a residual circulation in the mesosphere. The Canadian Middle Atmosphere Model(CMAM) is used to examine this vertical coupling mechanism in the context of the mesospheric response to the Antarctic ozone hole. It is found that the response differs significantly between late spring and early summer, because of a changing balance between the competing effects of parametrised gravity wavedrag (GWD)and changes in resolved wave drag local to the mesosphere. In late spring, the strengthened stratospheric westerlies arising from the ozone hole lead to reduced eastward GWD in the mesosphere and a warming of the polar mesosphere, just as in the well known mesospheric response to sudden stratospheric warmings, but with an opposite sign.In early summer, with easterly flow revailing over most of the polar stratosphere,the strengthened easterly wind shear within the mesosphere arising from the west ward GWD anomaly induces a positive resolved wave drag anomaly through baroclinic instability. The polar cooling induced by this process completely dominates the upper mesospheric response to the ozone hole in early summer. Consequences for the past and future evolution of noctilucent clouds are discussed

Projections of UV radiation changes in the 21st century: impact of ozone recovery and cloud effects

Monthly averaged surface erythemal solar irradiance (UV-Ery) for local noon from 1960 to 2100 has been derived using radiative transfer calculations and projections of ozone, temperature and cloud change from 14 chemistry climate models (CCM), as part of the CCMVal-2 activity of SPARC. Our calculations show the influence of ozone depletion and recovery on erythemal irradiance. In addition, we investigate UV-Ery changes caused by climate change due to increasing greenhouse gas concentrations. The latter include effects of both stratospheric ozone and cloud changes. The derived estimates provide a global picture of the likely changes in erythemal irradiance during the 21st century. Uncertainties arise from the assumed scenarios, different parameterizations – particularly of cloud effects on UV-Ery – and the spread in the CCM projections. The calculations suggest that relative to 1980, annually mean UV-Ery in the 2090s will be on average 12% lower at high latitudes in both hemispheres, 3% lower at mid latitudes, and marginally higher (1 %) in the tropics. The largest reduction (16 %) is projected for Antarctica in October. Cloud effects are responsible for 2–3% of the reduction in UV-Ery at high latitudes, but they slightly moderate it at mid-latitudes (1 %). The year of return of erythemal irradiance to values of certain milestones (1965 and 1980) depends largely on the return of column ozone to the corresponding levels and is associated with large uncertainties mainly due to the spread of the model projections. The inclusion of cloud effects in the calculations has only a small effect of the return years. At mid and high latitudes, changes in clouds and stratospheric ozone transport by global circulation changes due to greenhouse gases will sustain the erythemal irradiance at levels below those in 1965, despite the removal of ozone depleting substances.

Quantifying the contributions to stratospheric ozone changes from ozone depleting substances and greenhouse gases

A state-of-the-art chemistry climate model coupled to a three-dimensional ocean model is used to produce three experiments, all seamlessly covering the period 1950–2100, forced by different combinations of long-lived Greenhouse Gases (GHGs) and Ozone Depleting Substances (ODSs). The experiments are designed to quantify the separate effects of GHGs and ODSs on the evolution of ozone, as well as the extent to which these effects are independent of each other, by alternately holding one set of these two forcings constant in combination with a third experiment where both ODSs and GHGs vary. We estimate that up to the year 2000 the net decrease in the column amount of ozone above 20 hPa is approximately 75% of the decrease that can be attributed to ODSs due to the offsetting effects of cooling by increased CO2. Over the 21st century, as ODSs decrease, continued cooling from CO2 is projected to account for more than 50% of the projected increase in ozone above 20 hPa. Changes in ozone below 20 hPa show a redistribution of ozone from tropical to extra-tropical latitudes with an increase in the Brewer-Dobson circulation. In addition to a latitudinal redistribution of ozone, we find that the globally averaged column amount of ozone below 20 hPa decreases over the 21st century, which significantly mitigates the effect of upper stratospheric cooling on total column ozone. Analysis by linear regression shows that the recovery of ozone from the effects of ODSs generally follows the decline in reactive chlorine and bromine levels, with the exception of the lower polar stratosphere where recovery of ozone in the second half of the 21st century is slower than would be indicated by the decline in reactive chlorine and bromine concentrations. These results also reveal the degree to which GHGrelated effects mute the chemical effects of N2O on ozone in the standard future scenario used for the WMO Ozone Assessment. Increases in the residual circulation of the atmosphere and chemical effects from CO2 cooling more than halve the increase in reactive nitrogen in the mid to upper stratosphere that results from the specified increase in N2O between 1950 and 2100.

The effect of nonlinearity in CO2 heating rates on the attribution of stratospheric ozone and temperature changes

An analysis of the attribution of past and future changes in stratospheric ozone and temperature to anthropogenic forcings is presented. The analysis is an extension of the study of Shepherd and Jonsson (2008) who analyzed chemistry-climate simulations from the Canadian Middle Atmosphere Model (CMAM) and attributed both past and future changes to changes in the external forcings, i.e. the abundances of ozone-depleting substances (ODS) and well-mixed greenhouse gases. The current study is based on a new CMAM dataset and includes two important changes. First, we account for the nonlinear radiative response to changes in CO2. It is shown that over centennial time scales the radiative response in the upper stratosphere to CO2 changes is significantly nonlinear and that failure to account for this effect leads to a significant error in the attribution. To our knowledge this nonlinearity has not been considered before in attribution analysis, including multiple linear regression studies. For the regression analysis presented here the nonlinearity was taken into account by using CO2 heating rate, rather than CO2 abundance, as the explanatory variable. This approach yields considerable corrections to the results of the previous study and can be recommended to other researchers. Second, an error in the way the CO2 forcing changes are implemented in the CMAM was corrected, which significantly affects the results for the recent past. As the radiation scheme, based on Fomichev et al. (1998), is used in several other models we provide some description of the problem and how it was fixed.

On the attribution of stratospheric ozone and temperature changes to changes in ozone-depleting substances and well-mixed greenhouse gases

The vertical profile of global-mean stratospheric temperature changes has traditionally represented an important diagnostic for the attribution of the cooling effects of stratospheric ozone depletion and CO2 increases. However, CO2-induced cooling alters ozone abundance by perturbing ozone chemistry, thereby coupling the stratospheric ozone and temperature responses to changes in CO2 and ozone-depleting substances (ODSs). Here we untangle the ozone-temperature coupling and show that the attribution of global-mean stratospheric temperature changes to CO2 and ODS changes (which are the true anthropogenic forcing agents) can be quite different from the traditional attribution to CO2 and ozone changes. The significance of these effects is quantified empirically using simulations from a three-dimensional chemistry-climate model. The results confirm the essential validity of the traditional approach in attributing changes during the past period of rapid ODS increases, although we find that about 10% of the upper stratospheric ozone decrease from ODS increases over the period 1975–1995 was offset by the increase in CO2, and the CO2-induced cooling in the upper stratosphere has been somewhat overestimated. When considering ozone recovery, however, the ozone-temperature coupling is a first-order effect; fully 2/5 of the upper stratospheric ozone increase projected to occur from 2010–2040 is attributable to CO2 increases. Thus, it has now become necessary to base attribution of global-mean stratospheric temperature changes on CO2 and ODS changes rather than on CO2 and ozone changes.

O_3-N_2O correlations from the Atmospheric Chemistry Experiment: revisiting a diagnostic of transport and chemistry in the stratosphere

Our knowledge of stratospheric O3-N2O correlations is extended, and their potential for model-measurement comparison assessed, using data from the Atmospheric Chemistry Experiment (ACE) satellite and the Canadian Middle Atmosphere Model (CMAM). ACE provides the first comprehensive data set for the investigation of interhemispheric, interseasonal, and height-resolved differences of the O_3-N_2O correlation structure. By subsampling the CMAM data, the representativeness of the ACE data is evaluated. In the middle stratosphere, where the correlations are not compact and therefore mainly reflect the data sampling, joint probability density functions provide a detailed picture of key aspects of transport and mixing, but also trace polar ozone loss. CMAM captures these important features, but exhibits a displacement of the tropical pipe into the Southern Hemisphere (SH). Below about 21 km, the ACE data generally confirm the compactness of the correlations, although chemical ozone loss tends to destroy the compactness during late winter/spring, especially in the SH. This allows a quantitative comparison of the correlation slopes in the lower and lowermost stratosphere (LMS), which exhibit distinct seasonal cycles that reveal the different balances between diabatic descent and horizontal mixing in these two regions in the Northern Hemisphere (NH), reconciling differences found in aircraft measurements, and the strong role of chemical ozone loss in the SH. The seasonal cycles are qualitatively well reproduced by CMAM, although their amplitude is too weak in the NH LMS. The correlation slopes allow a "chemical" definition of the LMS, which is found to vary substantially in vertical extent with season.

Multimodel assessment of the factors driving stratospheric ozone evolution over the 21st century

The evolution of stratospheric ozone from 1960 to 2100 is examined in simulations from 14 chemistry‐climate models, driven by prescribed levels of halogens and greenhouse gases. There is general agreement among the models that total column ozone reached a minimum around year 2000 at all latitudes, projected to be followed by an increase over the first half of the 21st century. In the second half of the 21st century, ozone is projected to continue increasing, level off, or even decrease depending on the latitude. Separation into partial columns above and below 20 hPa reveals that these latitudinal differences are almost completely caused by differences in the model projections of ozone in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21st century and is projected to return to 1960 levels well before the end of the century, although there is a spread among models in the dates that ozone returns to specific historical values. We find decreasing halogens and declining upper atmospheric temperatures, driven by increasing greenhouse gases, contribute almost equally to increases in upper stratospheric ozone. In the tropical lower stratosphere, an increase in upwelling causes a steady decrease in ozone through the 21st century, and total column ozone does not return to 1960 levels in most of the models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21st century, returning to 1960 levels well before the end of the century in most models.

Ozone database in support of CMIP5 simulations: results and corresponding radiative forcing

A continuous tropospheric and stratospheric vertically resolved ozone time series, from 1850 to 2099, has been generated to be used as forcing in global climate models that do not include interactive chemistry. A multiple linear regression analysis of SAGE I+II satellite observations and polar ozonesonde measurements is used for the stratospheric zonal mean dataset during the well-observed period from 1979 to 2009. In addition to terms describing the mean annual cycle, the regression includes terms representing equivalent effective stratospheric chlorine (EESC) and the 11-yr solar cycle variability. The EESC regression fit coefficients, together with pre-1979 EESC values, are used to extrapolate the stratospheric ozone time series backward to 1850. While a similar procedure could be used to extrapolate into the future, coupled chemistry climate model (CCM) simulations indicate that future stratospheric ozone abundances are likely to be significantly affected by climate change, and capturing such effects through a regression model approach is not feasible. Therefore, the stratospheric ozone dataset is extended into the future (merged in 2009) with multimodel mean projections from 13 CCMs that performed a simulation until 2099 under the SRES (Special Report on Emission Scenarios) A1B greenhouse gas scenario and the A1 adjusted halogen scenario in the second round of the Chemistry-Climate Model Validation (CCMVal-2) Activity. The stratospheric zonal mean ozone time series is merged with a three-dimensional tropospheric data set extracted from simulations of the past by two CCMs (CAM3.5 and GISSPUCCINI)and of the future by one CCM (CAM3.5). The future tropospheric ozone time series continues the historical CAM3.5 simulation until 2099 following the four different Representative Concentration Pathways (RCPs). Generally good agreement is found between the historical segment of the ozone database and satellite observations, although it should be noted that total column ozone is overestimated in the southern polar latitudes during spring and tropospheric column ozone is slightly underestimated. Vertical profiles of tropospheric ozone are broadly consistent with ozonesondes and in-situ measurements, with some deviations in regions of biomass burning. The tropospheric ozone radiative forcing (RF) from the 1850s to the 2000s is 0.23Wm−2, lower than previous results. The lower value is mainly due to (i) a smaller increase in biomass burning emissions; (ii) a larger influence of stratospheric ozone depletion on upper tropospheric ozone at high southern latitudes; and possibly (iii) a larger influence of clouds (which act to reduce the net forcing) compared to previous radiative forcing calculations. Over the same period, decreases in stratospheric ozone, mainly at high latitudes, produce a RF of −0.08Wm−2, which is more negative than the central Intergovernmental Panel on Climate Change (IPCC) Fourth Assessment Report (AR4) value of −0.05Wm−2, but which is within the stated range of −0.15 to +0.05Wm−2. The more negative value is explained by the fact that the regression model simulates significant ozone depletion prior to 1979, in line with the increase in EESC and as confirmed by CCMs, while the AR4 assumed no change in stratospheric RF prior to 1979. A negative RF of similar magnitude persists into the future, although its location shifts from high latitudes to the tropics. This shift is due to increases in polar stratospheric ozone, but decreases in tropical lower stratospheric ozone, related to a strengthening of the Brewer-Dobson circulation, particularly through the latter half of the 21st century. Differences in trends in tropospheric ozone among the four RCPs are mainly driven by different methane concentrations, resulting in a range of tropospheric ozone RFs between 0.4 and 0.1Wm−2 by 2100. The ozone dataset described here has been released for the Coupled Model Intercomparison Project (CMIP5) model simulations in netCDF Climate and Forecast (CF) Metadata Convention at the PCMDI website (http://cmip-pcmdi.llnl.gov/).

Northern winter stratospheric temperature and ozone responses to ENSO inferred from an ensemble of Chemistry Climate Models

The connection between the El Ni˜no Southern Oscillation (ENSO) and the Northern polar stratosphere has been established from observations and atmospheric modeling. Here a systematic inter-comparison of the sensitivity of the modeled stratosphere to ENSO in Chemistry Climate Models (CCMs) is reported. This work uses results from a number of the CCMs included in the 2006 ozone assessment. In the lower stratosphere, the mean of all model simulations reports a warming of the polar vortex during strong ENSO events in February–March, consistent with but smaller than the estimate from satellite observations and ERA40 reanalysis. The anomalous warming is associated with an anomalous dynamical increase of column ozone north of 70� N that is accompanied by coherent column ozone decrease in the Tropics, in agreement with that deduced from the NIWA column ozone database, implying an increased residual circulation in the mean of all model simulations during ENSO. The spread in the model responses is partly due to the large internal stratospheric variability and it is shown that it crucially depends on the representation of the tropospheric ENSO teleconnection in the models.

Persistence and photochemical decay of springtime total ozone anomalies in the Canadian Middle Atmosphere Model

The persistence and decay of springtime total ozone anomalies over the entire extratropics (midlatitudes plus polar regions) is analysed using results from the Canadian Middle Atmosphere Model (CMAM), a comprehensive chemistry-climate model. As in the observations, interannual anomalies established through winter and spring persist with very high correlation coefficients (above 0.8) through summer until early autumn, while decaying in amplitude as a result of photochemical relaxation in the quiescent summertime stratosphere. The persistence and decay of the ozone anomalies in CMAM agrees extremely well with observations, even in the southern hemisphere when the model is run without heterogeneous chemistry (in which case there is no ozone hole and the seasonal cycle of ozone is quite different from observations). However in a version of CMAM with strong vertical diffusion, the northern hemisphere anomalies decay far too rapidly compared to observations. This shows that ozone anomaly persistence and decay does not depend on how the springtime anomalies are created or on their magnitude, but reflects the transport and photochemical decay in the model. The seasonality of the long-term trends over the entire extratropics is found to be explained by the persistence of the interannual anomalies, as in the observations, demonstrating that summertime ozone trends reflect winter/spring trends rather than any change in summertime ozone chemistry. However this mechanism fails in the northern hemisphere midlatitudes because of the relatively large impact, compared to observations, of the CMAM polar anomalies. As in the southern hemisphere, the influence of polar ozone loss in CMAM increases the midlatitude summertime loss, leading to a relatively weak seasonal dependence of ozone loss in the Northern Hemisphere compared to the observations.

High resolution simulation of recent Arctic and Antarctic stratospheric chemical ozone loss compared to observations

Simulations of polar ozone losses were performed using the three-dimensional high-resolution (1∘ × 1∘) chemical transport model MIMOSA-CHIM. Three Arctic winters 1999–2000, 2001–2002, 2002–2003 and three Antarctic winters 2001, 2002, and 2003 were considered for the study. The cumulative ozone loss in the Arctic winter 2002–2003 reached around 35% at 475 K inside the vortex, as compared to more than 60% in 1999–2000. During 1999–2000, denitrification induces a maximum of about 23% extra ozone loss at 475 K as compared to 17% in 2002–2003. Unlike these two colder Arctic winters, the 2001–2002 Arctic was warmer and did not experience much ozone loss. Sensitivity tests showed that the chosen resolution of 1∘ × 1∘ provides a better evaluation of ozone loss at the edge of the polar vortex in high solar zenith angle conditions. The simulation results for ozone, ClO, HNO3, N2O, and NO y for winters 1999–2000 and 2002–2003 were compared with measurements on board ER-2 and Geophysica aircraft respectively. Sensitivity tests showed that increasing heating rates calculated by the model by 50% and doubling the PSC (Polar Stratospheric Clouds) particle density (from 5 × 10−3 to 10−2 cm−3) refines the agreement with in situ ozone, N2O and NO y levels. In this configuration, simulated ClO levels are increased and are in better agreement with observations in January but are overestimated by about 20% in March. The use of the Burkholder et al. (1990) Cl2O2 absorption cross-sections slightly increases further ClO levels especially in high solar zenith angle conditions. Comparisons of the modelled ozone values with ozonesonde measurement in the Antarctic winter 2003 and with Polar Ozone and Aerosol Measurement III (POAM III) measurements in the Antarctic winters 2001 and 2002, shows that the simulations underestimate the ozone loss rate at the end of the ozone destruction period. A slightly better agreement is obtained with the use of Burkholder et al. (1990) Cl2O2 absorption cross-sections.

An assessment of the surface ozone trend in Ireland relevant to air pollution and environmental protection

Hourly data (1994–2009) of surface ozone concentrations at eight monitoring sites have been investigated to assess target level and long–term objective exceedances and their trends. The European Union (EU) ozone target value for human health (60 ppb–maximum daily 8–hour running mean) has been exceeded for a number of years for almost all sites but never exceeded the set limit of 25 exceedances in one year. Second highest annual hourly and 4th highest annual 8–hourly mean ozone concentrations have shown a statistically significant negative trend for in–land sites of Cork–Glashaboy, Monaghan and Lough Navar and no significant trend for the Mace Head site. Peak afternoon ozone concentrations averaged over a three year period from 2007 to 2009 have been found to be lower than corresponding values over a three–year period from 1996 to 1998 for two sites: Cork–Glashaboy and Lough Navar sites. The EU long–term objective value of AOT40 (Accumulated Ozone Exposure over a threshold of 40 ppb) for protection of vegetation (3 ppm–hour, calculated from May to July) has been exceeded, on an individual year basis, for two sites: Mace Head and Valentia. The critical level for the protection of forest (10 ppm–hour from April to September) has not been exceeded for any site except at Valentia in the year 2003. AOT40–Vegetation shows a significant negative trend for a 3–year running average at Cork–Glashaboy (–0.13±0.02 ppm–hour per year), at Lough Navar (–0.05±0.02 ppm–hour per year) and at Monaghan (–0.03±0.03 ppm–hour per year–not statistically significant) sites. No statistically significant trend was observed for the coastal site of Mace head. Overall, with the exception of the Mace Head and Monaghan sites, ozone measurement records at Irish sites show a downward negative trend in peak values that affect human health and vegetation.