ALBERT

Description: Simulations of CO, N2O and CH4 from a coupled chemistry-climate model (CMAM) are compared with satellite measurements from Odin Sub-Millimeter Radiometer (Odin/SMR), Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and Aura Microwave Limb Sounder (Aura/MLS). Pressure-latitude cross-sections and seasonal time series demonstrate that CMAM reproduces the observed global distributions and the polar winter time evolutions of the CO, N2O, and CH4 measurements quite well. Generally, excellent agreement with measurements is found in CO monthly zonal mean profiles in the stratosphere and mesosphere for various latitudes and seasons. The difference between the simulations and the observations are generally within 30%, which is comparable with the difference between the instruments in the upper stratosphere and mesosphere. In general, the CO measurements also show an excellent agreement between themselves although MLS retrievals are noisier than other retrievals above 10 hPa (~32 km). The measurements also show large difference in the lower stratosphere and upper troposphere. Comparisons of N2O show that CMAM results usually have a less than 15% difference to the measurements in the lower and middle stratosphere, and the observations are consistent as well. However, the standard version of CMAM has a serious low bias in the upper stratosphere. The CMAM CH4 distribution is also close to the observations in the lower stratosphere, but has a similar but smaller negative bias in the upper stratosphere. These negative biases can be reduced by introducing a vertical diffusion coefficient related to gravity wave drag. CO measurements from 2004 and 2006 show evidence of enhanced descent of air from the mesosphere into the stratosphere in the Arctic after strong stratospheric sudden warmings (SSWs). CMAM also shows strong descent of air after SSWs, but further investigation is needed. In the tropics, CMAM captures the "tape recorder" (or annual oscillation) in the lower stratosphere and the semiannual oscillations (SAO) at the stratopause and mesopause shown in MLS CO and SMR N2O observations. The inter-annual variation of the SAO at the stratopause in SMR N2O observations also shows a biennial oscillation, but CMAM cannot does not reproduce this feature. However, this study confirms that CMAM is able to simulate middle atmospheric transport processes reasonably well.

Description: Five years of OSIRIS (Optical Spectrograph and InfraRed Imager System) NO2 and SMR (Sub-Millimetre Radiometer) HNO3 observations from the Odin satellite, combined with data from a photochemical box model, have been used to construct a stratospheric proxy NOy data set including the gases: NO, NO2, HNO3, 2×N2O5 and CIONO2. This Odin NOy climatology is based on all daytime measurements and contains monthly mean and standard deviation, expressed as mixing ratio or number density, as function of latitude or equivalent latitude (5° bins) on 17 vertical layers (altitude, pressure or potential temperature) between 14 and 46 km. Comparisons with coincident NOy profiles from the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE-FTS) instrument were used to evaluate several methods to combine Odin observations with model data. This comparison indicates that the most appropriate merging technique uses OSIRIS measurements of NO2, scaled with model NO/NO2 ratios, to estimate NO. The sum of 2×N2O5 and CIONO2 is estimated from uncertainty-based weighted averages of scaled observations of SMR HNO3 and OSIRIS NO2. Comparisons with ACE-FTS suggest the precision (random error) and accuracy (systematic error) of Odin NOy profiles are about 15% and 20%, respectively. Further comparisons between Odin and the Canadian Middle Atmosphere Model (CMAM) show agreement to within 20% and 2 ppb throughout most of the stratosphere except in the polar vortices. A particularly large disagreement within the Antarctic vortex in the upper stratosphere during spring indicates too strong descent of air in CMAM. The combination of good temporal and spatial coverage, a relatively long data record, and good accuracy and precision make this a valuable NOy product for various atmospheric studies and model assessments.

Description: Five years of OSIRIS (Optical Spectrograph and InfraRed Imager System) NO2 and SMR (Sub-millimetre and Millimetre Radiometer) HNO3 observations from the Odin satellite, combined with data from a photochemical box model, have been used to construct a stratospheric proxy NOy data set including the gases: NO, NO2, HNO3, 2×N2O5 and ClONO2. This Odin NOy climatology is based on all daytime measurements and contains monthly mean and standard deviation, expressed as mixing ratio or number density, as function of latitude or equivalent latitude (5° bins) on 17 vertical layers (altitude, pressure or potential temperature) between 14 and 46 km. Comparisons with coincident NOy profiles from the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) instrument were used to evaluate several methods to combine Odin observations with model data. This comparison indicates that the most appropriate merging technique uses OSIRIS measurements of NO2, scaled with model NO/NO2 ratios, to estimate NO. The sum of 2×N2O5 and ClONO2 is estimated from uncertainty-based weighted averages of scaled observations of SMR HNO3 and OSIRIS NO2. Comparisons with ACE-FTS suggest the precision (random error) and accuracy (systematic error) of Odin NOy profiles are about 15% and 20%, respectively. Further comparisons between Odin and the Canadian Middle Atmosphere Model (CMAM) show agreement to within 20% and 2 ppb throughout most of the stratosphere except in the polar vortices. The combination of good temporal and spatial coverage, a relatively long data record, and good accuracy and precision make this a valuable NOy product for various atmospheric studies and model assessments.

Description: 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.

Description: The diurnal variation of HOCl and the related species ClO, HO2 and HCl measured by satellites has been compared with the results of a one-dimensional photochemical model. The study compares the data from various limb-viewing instruments with model simulations from the middle stratosphere to the lower mesosphere. Data from three sub-millimetre instruments and two infrared spectrometers are used, namely from the Sub-Millimetre Radiometer (SMR) on board Odin, the Microwave Limb Sounder (MLS) on board Aura, the Superconducting Submillimeter-wave Limb-Emission Sounder (SMILES) on the International Space Station, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board ENVISAT, and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on board SCISAT. Inter-comparison of the measurements from instruments on sun-synchronous satellites (SMR, MLS, MIPAS) and measurements from solar occultation instruments (ACE-FTS) is challenging since the measurements correspond to different solar zenith angles (or local times). However, using a model which covers all solar zenith angles and data from the SMILES instrument which measured at all local times over a period of several months provides the possibility to verify the model and to indirectly compare the diurnally variable species. The satellite data were averaged for latitudes of 20° S to 20° N for the SMILES observation period from November 2009 to April 2010 and were compared at three altitudes: 35, 45 and 55 km. Besides presenting the SMILES data, the study also shows a first comparison of the latest MLS data (version 3.3) of HOCl, ClO, and HO2 with other satellite observations, as well as a first evaluation of HO2 observations made by Odin/SMR. The MISU-1D model has been carefully initialised and run for conditions and locations of the observations. The diurnal cycle features for the species investigated here are generally well reproduced by the model. The satellite observations and the model agree well in terms of absolute mixing ratios. The differences between the day and night values of the model are in good agreement with the observations although the amplitude of the HO2 diurnal variation is 10–20% lower in the model than in the observations. In particular, the data offered the opportunity to study the reaction ClO+HO2 → HOCl+O2 in the lower mesosphere at 55 km. At this altitude the HOCl night-time variation depends only on this reaction. The result of this analysis points towards a value of the rate constant within the range of the JPL 2006 recommendation and the upper uncertainty limit of the JPL 2011 recommendation at 55 km.

Description: 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 GHG-related 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.

Description: Low-resolution atmospheric thermal emission spectra collected by balloon-borne radiometers over the time span of 1990–2002 are used to retrieve vertical profiles of HNO3, CFC-11 and CFC-12 volume mixing ratios between approximately 10 and 35 km altitude. All of the data analyzed have been collected from launches from a Northern Hemisphere mid-latitude site, during late summer, when stratospheric dynamic variability is at a minimum. The retrieval technique incorporates detailed forward modeling of the instrument and the radiative properties of the atmosphere, and obtains a best fit between modeled and measured spectra through a combination of onion-peeling and optimization steps. The retrieved HNO3 profiles are consistent over the 12-year period, and are consistent with recent measurements by the Atmospheric Chemistry Experiment-Fourier transform spectrometer satellite instrument. We therefore find no evidence of long-term changes in the HNO3 summer mid-latitude profile, although the uncertainty of our measurements precludes a conclusive trend analysis.

Description: 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.

Description: The Canadian Middle Atmosphere Model (CMAM) has been used to examine the middle atmosphere response to CO2 doubling. The radiative-photochemical response induced by doubling CO2 alone and the response produced by changes in prescribed SSTs are found to be approximately additive, with the former effect dominating throughout the middle atmosphere. The paper discusses the overall response, with emphasis on the effects of SST changes, which allow a tropospheric response to the CO2 forcing. The overall response is a cooling of the middle atmosphere accompanied by significant increases in the ozone and water vapor abundances. The ozone radiative feedback occurs through both an increase in solar heating and a decrease in infrared cooling, with the latter accounting for up to 15% of the total effect. Changes in global mean water vapor cooling are negligible above ∼30 hPa. Near the polar summer mesopause, the temperature response is weak and not statistically significant. The main effects of SST changes are a warmer troposphere, a warmer and higher tropopause, cell-like structures of heating and cooling at low and middlelatitudes in the middle atmosphere, warming in the summer mesosphere, water vapor increase throughout the domain, and O3 decrease in the lower tropical stratosphere. No noticeable change in upward-propagating planetary wave activity in the extratropical winter–spring stratosphere and no significant temperature response in the polar winter–spring stratosphere have been detected. Increased upwelling in the tropical stratosphere has been found to be linked to changed wave driving at low latitudes.