Lower Stratospheric Temperature Research Articles

COSMIC-RAY-DRIVEN REACTION AND GREENHOUSE EFFECT OF HALOGENATED MOLECULES: CULPRITS FOR ATMOSPHERIC OZONE DEPLETION AND GLOBAL CLIMATE CHANGE

This study is focused on the effects of cosmic rays (solar activity) and halogen-containing molecules (mainly chlorofluorocarbons — CFCs) on atmospheric ozone depletion and global climate change. Brief reviews are first given on the cosmic-ray-driven electron-induced-reaction (CRE) theory for O3depletion and the warming theory of halogenated molecules for climate change. Then natural and anthropogenic contributions to these phenomena are examined in detail and separated well through in-depth statistical analyses of comprehensive measured datasets of quantities, including cosmic rays (CRs), total solar irradiance, sunspot number, halogenated gases (CFCs, CCl4and HCFCs), CO2, total O3, lower stratospheric temperatures and global surface temperatures. For O3depletion, it is shown that an analytical equation derived from the CRE theory reproduces well 11-year cyclic variations of both polar O3loss and stratospheric cooling, and new statistical analyses of the CRE equation with observed data of total O3and stratospheric temperature give high linear correlation coefficients ≥ 0.92. After the removal of the CR effect, a pronounced recovery by 20 ~ 25 % of the Antarctic O3hole is found, while no recovery of O3loss in mid-latitudes has been observed. These results show both the correctness and dominance of the CRE mechanism and the success of the Montreal Protocol. For global climate change, in-depth analyses of the observed data clearly show that the solar effect and human-made halogenated gases played the dominant role in Earth's climate change prior to and after 1970, respectively. Remarkably, a statistical analysis gives a nearly zero correlation coefficient (R = -0.05) between corrected global surface temperature data by removing the solar effect and CO2concentration during 1850–1970. In striking contrast, a nearly perfect linear correlation with coefficients as high as 0.96–0.97 is found between corrected or uncorrected global surface temperature and total amount of stratospheric halogenated gases during 1970–2012. Furthermore, a new theoretical calculation on the greenhouse effect of halogenated gases shows that they (mainly CFCs) could alone result in the global surface temperature rise of ~0.6°C in 1970–2002. These results provide solid evidence that recent global warming was indeed caused by the greenhouse effect of anthropogenic halogenated gases. Thus, a slow reversal of global temperature to the 1950 value is predicted for coming 5 ~ 7 decades. It is also expected that the global sea level will continue to rise in coming 1 ~ 2 decades until the effect of the global temperature recovery dominates over that of the polar O3hole recovery; after that, both will drop concurrently. All the observed, analytical and theoretical results presented lead to a convincing conclusion that both the CRE mechanism and the CFC-warming mechanism not only provide new fundamental understandings of the O3hole and global climate change but have superior predictive capabilities, compared with the conventional models.

Stratospheric Ozone and Temperature Simulated from the Preindustrial Era to the Present Day

Abstract Results from the simulation of a coupled chemistry–climate model are presented for the period 1860 to 2005 using the observed greenhouse gas (GHG) and halocarbon concentrations. The model is coupled to a simulated ocean and uniquely includes both detailed tropospheric chemistry and detailed middle atmosphere chemistry, seamlessly from the surface to the model top layer centered at 0.02 hPa. It is found that there are only minor changes in simulated stratospheric temperature and ozone prior to the year 1960. As the halocarbon amounts increase after 1970, the model stratospheric ozone decreases approximately continuously until about 2000. The steadily increasing GHG concentrations cool the stratosphere from the beginning of the twentieth century at a rate that increases with height. During the early period the cooling leads to increased stratospheric ozone. The model results show a strong, albeit temporary, response to volcanic eruptions. While chlorofluorocarbon (CFC) concentrations remain low, the effect of eruptions is shown to increase the amount of HNO3, reducing ozone destruction by the NOx catalytic cycle. In the presence of anthropogenic chlorine, after the eruption of El Chichón and Mt. Pinatubo, chlorine radicals increased and the chlorine reservoirs decreased. The net volcanic effect on nitrogen and chlorine chemistry depends on altitude and, for these two volcanoes, leads to an ozone increase in the middle stratosphere and a decrease in the lower stratosphere. Model lower-stratospheric temperatures are also shown to increase during the last three major volcanic eruptions, by about 0.6 K in the global and annual average, consistent with observations.

The Role of High-Latitude Waves in the Intraseasonal to Seasonal Variability of Tropical Upwelling in the Brewer–Dobson Circulation

Abstract The forcing of tropical upwelling in the Brewer–Dobson circulation (BDC) on intraseasonal to seasonal time scales is investigated in integrations of an idealized general circulation model, ECMWF Interim Re-Analysis, and lower-stratospheric temperature measurements from the (Advanced) Microwave Sounding Unit, with a focus on the extended boreal winter season. Enhanced poleward eddy heat fluxes in the high latitudes (45°–90°N) at the 100-hPa level are associated with anomalous tropical cooling and anomalous warming on the poleward side of the polar night jet at the 70-hPa level and above. In both the model and the observations, planetary waves entering the stratosphere at high latitudes propagate equatorward to the subtropics and tropics at levels above 70 hPa over an approximately 10-day period, exerting a force at sufficiently low latitudes to modulate the tropical upwelling in the upper branch of the BDC, even on time scales longer than the radiative relaxation time scale of the lower stratosphere. To the extent that they force the BDC via downward as opposed to sideways control, planetary waves originating in high latitudes contribute to the seasonally varying climatological mean and the interannual variability of tropical upwelling at the 70-hPa level and above. Their influence upon the strength of the tropical upwelling, however, diminishes rapidly with depth below 70 hPa. In particular, tropical upwelling at the cold-point tropopause, near 100 hPa, appears to be modulated by variations in the strength of the lower branch of the BDC.

Long‐term ozone changes and associated climate impacts in CMIP5 simulations

AbstractOzone changes and associated climate impacts in the Coupled Model Intercomparison Project Phase 5 (CMIP5) simulations are analyzed over the historical (1960–2005) and future (2006–2100) period under four Representative Concentration Pathways (RCP). In contrast to CMIP3, where half of the models prescribed constant stratospheric ozone, CMIP5 models all consider past ozone depletion and future ozone recovery. Multimodel mean climatologies and long‐term changes in total and tropospheric column ozone calculated from CMIP5 models with either interactive or prescribed ozone are in reasonable agreement with observations. However, some large deviations from observations exist for individual models with interactive chemistry, and these models are excluded in the projections. Stratospheric ozone projections forced with a single halogen, but four greenhouse gas (GHG) scenarios show largest differences in the northern midlatitudes and in the Arctic in spring (~20 and 40 Dobson units (DU) by 2100, respectively). By 2050, these differences are much smaller and negligible over Antarctica in austral spring. Differences in future tropospheric column ozone are mainly caused by differences in methane concentrations and stratospheric input, leading to ~10 DU increases compared to 2000 in RCP 8.5. Large variations in stratospheric ozone particularly in CMIP5 models with interactive chemistry drive correspondingly large variations in lower stratospheric temperature trends. The results also illustrate that future Southern Hemisphere summertime circulation changes are controlled by both the ozone recovery rate and the rate of GHG increases, emphasizing the importance of simulating and taking into account ozone forcings when examining future climate projections.

Direct and indirect effects of solar variations on stratospheric ozone and temperature

We have used a fully coupled chemistry-climate model (WACCM) to investigate the relative importance of the direct and indirect effects of 11a solar variations on stratospheric temperature and ozone. Although the model does not contain a quasi-biennial oscillation (QBO) and uses fixed sea surface temperature (SST), it is able to produce a second maximum solar response in tropical lower stratospheric (TLS) temperature and ozone of approximately 0.5 K and 3%, respectively. In the TLS, the solar spectral variations in the chemistry scheme play a more important role than solar spectral variations in the radiation scheme in generating temperature and ozone responses. The chemistry effect of solar variations causes significant changes in the Brewer-Dobson (BD) circulation resulting in ozone anomalies in the TLS. The model simulations also show a negative feedback in the upper stratosphere between the temperature and ozone responses. A wavelet analysis of the modeled ozone and temperature time series reveals that the maximum solar responses in ozone and temperature caused by both chemical and radiative effects occur at different altitudes in the upper stratosphere. The analysis also confirms that both the direct radiative and indirect ozone feedback effects are important in generating a solar response in the upper stratospheric temperatures, although the solar spectral variations in the chemistry scheme give the largest solar cycle power in the upper stratospheric temperature.

The Tibetan ozone low and its long-term variation during 1979–2010

A Tibetan ozone low was found in the 1990s after the Antarctic ozone hole. Whether this ozone low has been recovering from the beginning of the 2000s following the global ozone recovery is an intriguing topic. With the most recent merged TOMS/SBUV (Total Ozone Mapping Spectrometer/Solar Backscatter Ultra Violet) ozone data, the Tibetan ozone low and its long-term variation during 1979–2010 are analyzed using a statistical regression model that includes the seasonal cycle, solar cycle, quasi-biennial oscillation (QBO), ENSO signal, and trends. The results show that the Tibetan ozone low maintains and may become more severe on average during 1979–2010, compared with its mean state in the periods before 2000, possibly caused by the stronger downward trend of total ozone concentration over the Tibet. Compared with the ozone variation over the non-Tibetan region along the same latitudes, the Tibetan ozone has a larger downward trend during 1979–2010, with a maximum value of −0.40±0.10 DU yr−1 in January, which suggests the strengthening of the Tibetan ozone low in contrast to the recovery of global ozone. Regression analyses show that the QBO signal plays an important role in determining the total ozone variation over the Tibet. In addition, the long-term ozone variation over the Tibetan region is largely affected by the thermal-dynamical proxies such as the lower stratospheric temperature, with its contribution reaching around 10% of the total ozone change, which is greatly different from that over the non-Tibetan region.

Intensity of climate variability derived from the satellite and MERRA reanalysis temperatures: AO, ENSO, and QBO

Satellite measurements (Atmospheric InfraRed Sounder/Advanced Microwave Sounding Unit-A, MODerate resolution Imaging Spectroradiometer) and the Modern Era Retrospective-analysis for Research and Applications (MERRA) reanalysis have been utilized to analyze the relative influence of the climate variability (AO: Arctic Oscillation, ENSO: El Niño-Southern Oscillation, QBO: Quasi-Biennial Oscillation) on the zonal-mean temperature and wind variations over the globe from September 2002 to August 2011. We also extended the usage of MERRA data for the period of 1979–2011; furthermore, three climate indices of AO, NINO3.4, and QBO were used as the corresponding climate indicators. The correlations between the temperature anomalies and the climate indices indicate that the tropospheric temperature variability in the mid-latitude (30–60N) linked to both AO and ENSO has been more pronounced over ocean than over land. However, the low stratospheric temperature variability in the mid-latitude is mainly associated with ENSO and QBO. The north–south symmetric patterns over the globe are seen in the wind anomaly distributions for ENSO and QBO, but not for AO. The ENSO events are globally vigorous but also localized during the recent 9 years compared with those based on the period of 1979–2011. The tropospheric warming and stratospheric cooling phenomena during this period are more remarkable in the recent 9 years, although according to IPCC (2012). their linkage to the ENSO variability is still uncertain. The ENSO is found to have more significant impact on the tropospheric and low stratosphere temperature variability over the tropics in the recent period, consistent with more active zonal wind meridional circulations. The discrepancies between satellite observations and MERRA are also discussed. The estimated relative impact of the three major concurrent large-scale climate phenomena on regional temperature variability can be of great use in its long-term predictability.

The Aqua-Planet Experiment (APE): CONTROL SST Simulation

Climate simulations by 16 atmospheric general circulation models (AGCMs) are compared on an aqua-planet, a water-covered Earth with prescribed sea surface temperature varying only in latitude. The idealised configuration is designed to expose differences in the circulation simulated by different models. Basic features of the aqua-planet climate are characterised by comparison with Earth. The models display a wide range of behaviour. The balanced component of the tropospheric mean flow, and mid-latitude eddy covariances subject to budget constraints, vary relatively little among the models. In contrast, differences in damping in the dynamical core strongly influence transient eddy amplitudes. Historical uncertainty in modelled lower stratospheric temperatures persists in APE.Aspects of the circulation generated more directly by interactions between the resolved fluid dynamics and parameterized moist processes vary greatly. The tropical Hadley circulation forms either a single or double inter-tropical convergence zone (ITCZ) at the equator, with large variations in mean precipitation. The equatorial wave spectrum shows a wide range of precipitation intensity and propagation characteristics. Kelvin mode-like eastward propagation with remarkably constant phase speed dominates in most models. Westward propagation, less dispersive than the equatorial Rossby modes, dominates in a few models or occurs within an eastward propagating envelope in others. The mean structure of the ITCZ is related to precipitation variability, consistent with previous studies.The aqua-planet global energy balance is unknown but the models produce a surprisingly large range of top of atmosphere global net flux, dominated by differences in shortwave reflection by clouds. A number of newly developed models, not optimised for Earth climate, contribute to this. Possible reasons for differences in the optimised models are discussed.The aqua-planet configuration is intended as one component of an experimental hierarchy used to evaluate AGCMs. This comparison does suggest that the range of model behaviour could be better understood and reduced in conjunction with Earth climate simulations. Controlled experimentation is required to explore individual model behavior and investigate convergence of the aqua-planet climate with increasing resolution.

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 fingerprint) 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.

Extreme ozone depletion in the 2010–2011 Arctic winter stratosphere as observed by MIPAS/ENVISAT using a 2-D tomographic approach

Abstract. We present observations of the 2010–2011 Arctic winter stratosphere from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) onboard ENVISAT. Limb sounding infrared measurements were taken by MIPAS during the Northern polar winter and into the subsequent spring, giving a continuous vertically resolved view of the Arctic dynamics, chemistry and polar stratospheric clouds (PSCs). We adopted a 2-D tomographic retrieval approach to account for the strong horizontal inhomogeneity of the atmosphere present under vortex conditions, self-consistently comparing 2011 to the 2-D analysis of 2003–2010. Unlike most Arctic winters, 2011 was characterized by a strong stratospheric vortex lasting until early April. Lower stratospheric temperatures persistently remained below the threshold for PSC formation, extending the PSC season up to mid-March, resulting in significant chlorine activation leading to ozone destruction. On 3 January 2011, PSCs were detected up to 30.5 ± 0.9 km altitude, representing the highest PSCs ever reported in the Arctic. Through inspection of MIPAS spectra, 83% of PSCs were identified as supercooled ternary solution (STS) or STS mixed with nitric acid trihydrate (NAT), 17% formed mostly by NAT particles, and only two cases by ice. In the lower stratosphere at potential temperature 450 K, vortex average ozone showed a daily depletion rate reaching 100 ppbv day−1. In early April at 18 km altitude, 10% of vortex measurements displayed total depletion of ozone, and vortex average values dropped to 0.6 ppmv. This corresponds to a chemical loss from early winter greater than 80%. Ozone loss was accompanied by activation of ClO, associated depletion of its reservoir ClONO2, and significant denitrification, which further delayed the recovery of ozone in spring. Once the PSC season halted, ClO was reconverted primarily into ClONO2. Compared to MIPAS observed 2003–2010 Arctic average values, the 2010–2011 vortex in late winter had 15 K lower temperatures, 40% lower HNO3 and 50% lower ozone, reaching the largest ozone depletion ever observed in the Arctic. The overall picture of this Arctic winter was remarkably closer to conditions typically found in the Antarctic vortex than ever observed before.

Intense Arctic Ozone Depletion in the Spring of 2011

Observations of record-breaking ozone depletion during the Arctic spring of 2011 were made at 76˚ N in Thule, Greenland. The ozone total column amount of 290 DU measured on 18 March 2011 is the lowest value from the 12-year observation record and represents an ozone depletion of up to 48% of a typical March column. The unique 2010 – 11 vortex was characterized by sustained low stratospheric temperatures and stability that resisted breakup through March. Simultaneous observations of O3, HF, HCl, HNO3, and ClONO2 demonstrate strong subsidence and substantial conversion of chlorine from its normal reservoirs.

Record-breaking ozone loss in the Arctic winter 2010/2011: comparison with 1996/1997

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.

Temperature thresholds for chlorine activation and ozone loss in the polar stratosphere

Abstract. Low stratospheric temperatures are known to be responsible for heterogeneous chlorine activation that leads to polar ozone depletion. Here, we discuss the temperature threshold below which substantial chlorine activation occurs. We suggest that the onset of chlorine activation is dominated by reactions on cold binary aerosol particles, without the formation of polar stratospheric clouds (PSCs), i.e. without any significant uptake of HNO3 from the gas phase. Using reaction rates on cold binary aerosol in a model of stratospheric chemistry, a chlorine activation threshold temperature, TACL, is derived. At typical stratospheric conditions, TACL is similar in value to TNAT (within 1–2 K), the highest temperature at which nitric acid trihydrate (NAT) can exist. TNAT is still in use to parameterise the threshold temperature for the onset of chlorine activation. However, perturbations can cause TACL to differ from TNAT: TACL is dependent upon H2O and potential temperature, but unlike TNAT is not dependent upon HNO3. Furthermore, in contrast to TNAT, TACL is dependent upon the stratospheric sulfate aerosol loading and thus provides a means to estimate the impact on polar ozone of strong volcanic eruptions and some geo-engineering options, which are discussed. A parameterisation of TACL is provided here, allowing it to be calculated for low solar elevation (or high solar zenith angle) over a comprehensive range of stratospheric conditions. Considering TACL as a proxy for chlorine activation cannot replace a detailed model calculation, and polar ozone loss is influenced by other factors apart from the initial chlorine activation. However, TACL provides a more accurate description of the temperature conditions necessary for chlorine activation and ozone loss in the polar stratosphere than TNAT.

The exceptional ozone depletion over the Arctic in January–March 2011

The largest ozone losses ever recorded over the Arctic have been measured by an international network of over 30 ground-based stations and satellite-borne sensors during January–March 2011. We study whether this was an exceptional event or whether it is part of the evolution of an ozone hole in the Arctic. The main finding is that the 2010–2011 winter's record-breaking ozone loss was instigated by the extremely low stratospheric temperatures that are linked to climate change, that is, the coldest winters at the Arctic region have been getting colder leading to larger ozone losses there, which are progressively reaching the levels of the Antarctic ozone hole.

Anthropogenic effects on the distribution of minor chemical constituents in the mesosphere/lower thermosphere – A model study

We investigate the influence that rising concentrations of methane, nitrous oxide and carbon dioxide have had upon the chemistry of the mesosphere since 1961. Calculations were performed using our global 3D-model LIMA (Leibniz-Institute Middle Atmosphere), designed for the investigation of the MLT-region (Mesosphere-Lower Thermosphere) and particularly for the extended mesopause region. LIMA utilizes observed tropospheric and lower stratospheric temperature and horizontal wind data up to 35km altitude by assimilating ECMWF/ERA-40 and ECMWF operational data. Real Lyman-α flux values are employed to determine the variable water vapor dissociation rate. Three different calculations were carried out and analyzed: (1) use of the same annual variation of the model dynamics in the chemical transport model (CTM) for all years according to the dynamics of the solar minimum year 1964 and employment of a realistic growth of the anthropogenic gases; (2) use of constant concentrations of the anthropogenic constituents at the lower border, but employment of the varying model dynamics; (3) the so-called realistic case, which considers both the long-term increase in the anthropogenic minor constituents and the varying dynamics according to LIMA calculations. The analysis of these three cases shows that the dynamics are able to counteract the impact of anthropogenic growth of minor constituents in the upper mesosphere-mesopause-lower thermosphere region in middle to high latitudes in summer. The water vapor mixing ratio increases due to rising methane concentration. The reason for this lies in a positive feedback process of autocatalytic water vapor production. The change in concentration of the minor constituents impacts both the cooling rate and the chemical heating rate. We present the relative and absolute deviations between the solar activity minimum years 1964 and 2008 for the most important minor constituents. We discuss the long-term behavior, particularly of water vapor, with regard to the impact on the NLC-region.

Correction to “Stratospheric heating by potential geoengineering aerosols”

[1] In the paper “Stratospheric heating by potential geoengineering aerosols” by Angus Ferraro, Eleanor Highwood and Andrew Charlton-Perez (Geophysical Research Letters, 38, L24706, doi:10.1029/2011GL049761, 2011), there is an error we would like to correct. [2] The model runs with limestone aerosol used an incorrect control case, which produced incorrect heating rate changes when compared with a ‘perturbed’ case which included limestone aerosol. We attach a corrected Figure 2, which shows stratospheric temperature change for the SMALL/WIDE distribution of each aerosol type. There is now no cooling in the polar lower stratosphere beneath the layer of limestone aerosol. The temperature change pattern for limestone is now very similar to that for titania, albeit of different magnitude. This renders paragraph 16, which refers to the cooling beneath the layer, superfluous. [3] This change slightly affects the calculation of the lower stratospheric pole-Equator temperature differences shown in Figure 3. We attach a corrected version of Figure 3. There is a slight reduction in the pole-Equator temperature differences in DJF. In JJA the SMALL/ WIDE case now slightly reduces the pole-Equator temperature difference. However, the magnitude of these changes are small and do not affect our conclusions that (1) limestone aerosol produces a stratospheric temperature change pattern distinct to other aerosol types, (2) limestone aerosol increases the pole-Equator temperature difference (a proxy for the meridional temperature gradient) in DJF and (3) this pole-Equator temperature difference is extremely sensitive to size for wide size distributions.

Chemistry‐climate model simulations of recent trends in lower stratospheric temperature and stratospheric residual circulation

Observations of the lower stratospheric temperature over the last three decades show seasonal variations in tropical trends together with spatial patterns in southern high latitude trends in late winter‐spring, with regions of cooling and warming of comparable magnitude. Neither aspect is reproduced in climate models used in the Intergovernmental Panel on Climate Change's Fourth Assessment Report (IPCC AR4). Here we show that stratosphere‐resolving chemistry‐climate models can produce these aspects of temperature trends. However, the seasonality of temperature trends can vary greatly among simulations of the same model, and even if one ensemble member reproduces the observed seasonality in trends there may be little agreement with observations for another member. The variability in trends among model ensemble members is related to differences in trends in wave activity propagating into the stratosphere. These results suggest that the seasonality of the observed temperature trends could be the result of natural variability as well as, or instead of, a response to external forcing, and that comparison with these trends may not be a robust test of climate models.

Uptake Measurements of Acetic Acid on Ice and Nitric Acid-Doped Thin Ice Films over Upper Troposphere/Lower Stratosphere Temperatures

The adsorption of gaseous acetic acid (CH(3)C(O)OH) on thin ice films and on ice doped with nitric acid (1.96 and 7.69 wt %) was investigated over upper troposphere and lower stratosphere (UT/LS) temperatures (198-208 K), and at low gas concentrations. Experiments were performed in a Knudsen flow reactor coupled to a quadrupole mass spectrometer. The initial uptake coefficients, γ(0), on thin ice films or HNO(3)-doped ice films were measured at low surface coverage. In all cases, γ(0) showed an inverse temperature dependence, and for pure thin ice films, it was given by the expression γ(0)(T) = (4.73 ± 1.13) × 10(-17) exp[(6496 ± 1798)/T]; the quoted errors are the 2σ precision of the linear fit, and the estimated systematic uncertainties are included in the pre-exponential factor. The inverse temperature dependence suggests that the adsorption process occurs via the formation of an intermediate precursor state. Uptakes were well represented by the Langmuir adsorption model, and the saturation surface coverage, N(max), on pure thin ice films was (2.11 ± 0.16) × 10(14) molecules cm(-2), independent of temperature in the range 198-206 K. Light nitration (1.96 and 7.69 wt %) of ice films resulted in more efficient CH(3)C(O)OH uptakes and larger N(max) values that may be attributed to in-bulk diffusion or change in nature of the gas-ice surface interaction. Finally, it was estimated that the rate of adsorption of acetic acid on high-density cirrus clouds in the UT/LS is fast, and this is reflected in the short atmospheric lifetimes (2-8 min) of acetic acid; however, the extent of this uptake is minor resulting in at most a 5% removal of acetic acid in UT/LS cirrus clouds.

Extreme ozone loss over the Northern Hemisphere high latitudes in the early 2011

ABSTRACTThe satellite ozone data comprising The New Zealand National Institute of Water and Atmospheric Research (NIWA) total ozone database version 2.7, total ozone by the Ozone Monitoring Instrument (OMI) spectrophotometer on the Aura platform, and the ozone mixing ratios by SBUV/2 measurements on The National Oceanic and Atmospheric Administration (NOAA) platforms are analysed for ozone variability over the sunlit part of the Northern Hemisphere polar region. An extended area, with unusually low ozone values, is observed in a two-month period beginning in mid February 2011. The total area with extremely depleted total ozone reached the maximum at the end of March 2011, equal to ~11×106 km2. The area is even larger in the lower/mid stratosphere. A multiple regression model is proposed to attribute the polar total ozone variability to various chemical and dynamical ozone forcings. The model reproduces the ozone loss in early 2011 and the overall picture of the ozone long-term changes. The extreme ozone decline in 2011 could be attributed to the long-lasting period with low stratospheric temperature (<195 K), weaker than the normal Brewer-Dobson circulation, and the Arctic Oscillation in a strong positive phase. A deficit of total ozone in the following summer months (June–July–August), after the total ozone decline in March, was predicted and supported by later OMI observations.

The Seasonal Cycle and Interannual Variability in Stratospheric Temperatures and Links to the Brewer–Dobson Circulation: An Analysis of MSU and SSU Data

Abstract Previous studies have shown that lower-stratosphere temperatures display a near-perfect cancellation between tropical and extratropical latitudes on both annual and interannual time scales. The out-of-phase relationship between tropical and high-latitude lower-stratospheric temperatures is a consequence of variability in the strength of the Brewer–Dobson circulation (BDC). In this study, the signal of the BDC in stratospheric temperature variability is examined throughout the depth of the stratosphere using data from the Stratospheric Sounding Unit (SSU). While the BDC has a seemingly modest signal in the annual cycle in zonal-mean temperatures in the mid- and upper stratosphere, it has a pronounced signal in the month-to-month and interannual variability. Tropical and extratropical temperatures are significantly negatively correlated in all SSU channels on interannual time scales, suggesting that variations in wave driving are a major factor controlling global-scale temperature variability not only in the lower stratosphere (as shown in previous studies), but also in the mid- and upper stratosphere. The out-of-phase relationship between tropical and high latitudes peaks at all levels during the cold-season months: December–March in the Northern Hemisphere and July–October in the Southern Hemisphere. In the upper stratosphere, the out-of-phase relationship with high-latitude temperatures extends beyond the tropics and well into the extratropics of the opposite hemisphere. The seasonal cycle in stratospheric temperatures follows the annual march of insolation at all levels and latitudes except in the mid- to upper tropical stratosphere, where it is dominated by the semiannual oscillation. Mid- to upper-stratospheric temperatures also exhibit a distinct but small semiannual cycle at extratropical latitudes.