Beyond model spread: a process-based attribution of uncertainties in stratospheric ozone modelling

Intercomparisons between Chemistry-Climate Models (CCMs) have highlighted shortcomings in our understanding and/or modeling of long-term ozone trends, and there is a growing interest in the impact of stratospheric ozone changes on tropospheric chemistry via both ozone fluxes (e.g. from the projected strengthening of the Brewer-Dobson circulation) and actinic fluxes. Advances in this area require a good understanding of the modelling uncertainties in the present-day distribution of stratospheric ozone, and a correct attribution of these uncertainties to the processes governing this distribution: photolysis, chemistry and transport. These processes depend primarily on solar irradiance, temperature and dynamics.Here we estimate model uncertainties arising from different input datasets, and compare them with typical uncertainties arising from the transport and chemistry schemes. This study is based on four sets of tightly controlled sensititivity experiments which all use temperature and dynamics specified from reanalyses of meteorological observations. The first set of experiments uses one Chemistry-Transport Model (CTM) and evaluates the impact of using 3 different spectra of solar irradiance. In the second set, the CTM is run with 4 different input reanalyses: ERA-5, MERRA-2, ERA-I and JRA-55. The third set of experiments still relies on the same CTM, exploring the impact of the transport algorithm and its configuration. The fourth set is the most sophisticated as it is enabled by model developments for the Copernicus Atmopshere Monitoring Service, where the ECMWF model IFS is run with three different photochemistry modules named according to their parent CTM: IFS(CB05-BASCOE), IFS(MOCAGE) and IFS(MOZART).All modelling experiments start from the same initial conditions and last 2.5 years (2013-2015). The uncertainties arising from different input datasets or different model components are estimated from the spreads in each set of sensitivity experiments and also from the gross error between the corresponding model means and the BASCOE Reanalysis of Aura-MLS (BRAM2). The results are compared across the four sets of experiments, as a function of latitude and pressure, with a focus on two regions of the stratosphere: the polar lower stratosphere in winter and spring - in order to assess and understand the quality of our ozone hole forecasts - and the tropical middle and upper stratosphere - where noticeably large disagreements are found between the experiments.

Download Full-text

The representation of solar cycle signals in stratospheric ozone. Part II: Analysis of global models

10.5194/acp-2017-477 ◽

2017 ◽

Cited By ~ 3

Author(s):

Amanda C. Maycock ◽

Katja Matthes ◽

Susann Tegtmeier ◽

Hauke Schmidt ◽

Rémi Thiéblemont ◽

...

Keyword(s):

Solar Cycle ◽

Solar Irradiance ◽

Climate Models ◽

Climate Model ◽

Stratospheric Ozone ◽

Temperature Response ◽

Solar Variability ◽

High Latitudes ◽

Stratospheric Temperature ◽

The Impact

Abstract. The impact of changes in incoming solar irradiance on stratospheric ozone abundances should be included in climate model simulations to fully capture the atmospheric response to solar variability. This study presents the first systematic comparison of the solar-ozone response (SOR) during the 11 year solar cycle amongst different chemistry-climate models (CCMs) and ozone databases specified in climate models that do not include chemistry. We analyse the SOR in eight CCMs from the WCRP/SPARC Chemistry-Climate Model Initiative (CCMI-1) and compare these with three ozone databases: the Bodeker Scientific database, the SPARC/AC&C database for CMIP5, and the SPARC/CCMI database for CMIP6. The results reveal substantial differences in the representation of the SOR between the CMIP5 and CMIP6 ozone databases. The peak amplitude of theSOR in the upper stratosphere (1–5 hPa) decreases from 5 % to 2 % between the CMIP5 and CMIP6 databases. This difference is because the CMIP5 database was constructed from a regression model fit to satellite observations, whereas the CMIP6 database is constructed from CCM simulations, which use a spectral solar irradiance (SSI) dataset with relatively weak UV forcing. The SOR in the CMIP6 ozone database is therefore implicitly more similar to the SOR in the CCMI-1 models than to the CMIP5 ozone database, which shows a greater resemblance in amplitude and structure to the SOR in the Bodeker database. The latitudinal structure of the annual mean SOR in the CMIP6 ozone database and CCMI-1 models is considerably smoother than in the CMIP5 database, which shows strong gradients in the SOR across the midlatitudes owing to the paucity of observations at high latitudes. The SORs in the CMIP6 ozone database and in the CCMI-1 models show a strong seasonal dependence, including large meridional gradients at mid to high latitudes during winter; such seasonal variations in the SOR are not included in the CMIP5 ozone database. Sensitivity experiments with a global atmospheric model without chemistry (ECHAM6.3) are performed to assess the impact of changes in the representation of the SOR and SSI forcing between CMIP5 and CMIP6. The experiments show that the smaller amplitude of the SOR in the CMIP6 ozone database compared to CMIP5 causes a decrease in the modelled tropical stratospheric temperature response over the solar cycle of up to 0.6 K, or around 50 % of the total amplitude. The changes in the SOR explain most of the difference in the amplitude of the tropical stratospheric temperature response in the case with combined changes in SOR and SSI between CMIP5 and CMIP6. The results emphasise the importance of adequately representing the SOR in climate models to capture the impact of solar variability on the atmosphere. Since a number of limitations in the representation of the SOR in the CMIP5 ozone database have been identified, CMIP6 models without chemistry are encouraged to use the CMIP6 ozone database to capture the climate impacts of solar variability.

Download Full-text

The Impact of Different Absolute Solar Irradiance Values on Current Climate Model Simulations

Journal of Climate ◽

10.1175/jcli-d-13-00136.1 ◽

2014 ◽

Vol 27 (3) ◽

pp. 1100-1120 ◽

Cited By ~ 8

Author(s):

David H. Rind ◽

Judith L. Lean ◽

Jeffrey Jonas

Keyword(s):

Climate Change ◽

Solar Irradiance ◽

Cloud Cover ◽

Climate Models ◽

Climate Model ◽

Middle Atmosphere ◽

Global Climate ◽

Stratospheric Ozone ◽

Model Simulations ◽

The Impact

Abstract Simulations of the preindustrial and doubled CO2 climates are made with the GISS Global Climate Middle Atmosphere Model 3 using two different estimates of the absolute solar irradiance value: a higher value measured by solar radiometers in the 1990s and a lower value measured recently by the Solar Radiation and Climate Experiment. Each of the model simulations is adjusted to achieve global energy balance; without this adjustment the difference in irradiance produces a global temperature change of 0.4°C, comparable to the cooling estimated for the Maunder Minimum. The results indicate that by altering cloud cover the model properly compensates for the different absolute solar irradiance values on a global level when simulating both preindustrial and doubled CO2 climates. On a regional level, the preindustrial climate simulations and the patterns of change with doubled CO2 concentrations are again remarkably similar, but there are some differences. Using a higher absolute solar irradiance value and the requisite cloud cover affects the model’s depictions of high-latitude surface air temperature, sea level pressure, and stratospheric ozone, as well as tropical precipitation. In the climate change experiments it leads to an underestimation of North Atlantic warming, reduced precipitation in the tropical western Pacific, and smaller total ozone growth at high northern latitudes. Although significant, these differences are typically modest compared with the magnitude of the regional changes expected for doubled greenhouse gas concentrations. Nevertheless, the model simulations demonstrate that achieving the highest possible fidelity when simulating regional climate change requires that climate models use as input the most accurate (lower) solar irradiance value.

Download Full-text

Forecasts and assimilation experiments of the Antarctic ozone hole 2008

Atmospheric Chemistry and Physics ◽

10.5194/acp-11-1961-2011 ◽

2011 ◽

Vol 11 (5) ◽

pp. 1961-1977 ◽

Cited By ~ 32

Author(s):

J. Flemming ◽

A. Inness ◽

L. Jones ◽

H. J. Eskes ◽

V. Huijnen ◽

...

Keyword(s):

Transport Model ◽

Initial Conditions ◽

Stratospheric Ozone ◽

Satellite Observations ◽

Ozone Hole ◽

Chemical Mechanism ◽

Ozone Monitoring Instrument ◽

Variable Effect ◽

Antarctic Ozone ◽

Antarctic Ozone Hole

Abstract. The 2008 Antarctic ozone hole was one of the largest and most long-lived in recent years. Predictions of the ozone hole were made in near-real time (NRT) and hindcast mode with the Integrated Forecast System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The forecasts were carried out both with and without assimilation of satellite observations from multiple instruments to provide more realistic initial conditions. Three different chemistry schemes were applied for the description of stratospheric ozone chemistry: (i) a linearization of the ozone chemistry, (ii) the stratospheric chemical mechanism of the Model of Ozone and Related Chemical Tracers, version 3, (MOZART-3) and (iii) the relaxation to climatology as implemented in the Transport Model, version 5, (TM5). The IFS uses the latter two schemes by means of a two-way coupled system. Without assimilation, the forecasts showed model-specific shortcomings in predicting start time, extent and duration of the ozone hole. The assimilation of satellite observations from the Microwave Limb Sounder (MLS), the Ozone Monitoring Instrument (OMI), the Solar Backscattering Ultraviolet radiometer (SBUV-2) and the SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY) led to a significant improvement of the forecasts when compared with total columns and vertical profiles from ozone sondes. The combined assimilation of observations from multiple instruments helped to overcome limitations of the ultraviolet (UV) sensors at low solar elevation over Antarctica. The assimilation of data from MLS was crucial to obtain a good agreement with the observed ozone profiles both in the polar stratosphere and troposphere. The ozone analyses by the three model configurations were very similar despite the different underlying chemistry schemes. Using ozone analyses as initial conditions had a very beneficial but variable effect on the predictability of the ozone hole over 15 days. The initialized forecasts with the MOZART-3 chemistry produced the best predictions of the increasing ozone hole whereas the linear scheme showed the best results during the ozonehole closure.

Download Full-text

Influences of hydroxyl radicals (OH) on top-down estimates of the global and regional methane budgets

10.5194/acp-2019-1208 ◽

2020 ◽

Cited By ~ 1

Author(s):

Yuanhong Zhao ◽

Marielle Saunois ◽

Philippe Bousquet ◽

Xin Lin ◽

Antoine Berchet ◽

...

Keyword(s):

Spatial Distribution ◽

Climate Models ◽

Transport Model ◽

Atmospheric Transport ◽

Temporal Variations ◽

Oh Radicals ◽

Chemical Transport Model ◽

Top Down ◽

Ch4 Emissions ◽

The Impact

Abstract. The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role to close the global methane budget. Previous research that assessed the impact of OH changes on the CH4 budget mostly relied on box modeling inversions with a very simplified atmospheric transport and no representation of the heterogeneous spatial distribution of OH radicals. Here using a variational Bayesian inversion framework and a 3D chemical transport model, LMDz, combined with 10 different OH fields derived from chemistry-climate models (CCMI experiment), we evaluate the influence of OH burden, spatial distribution, and temporal variations on the global CH4 budget. The global tropospheric mean CH4-reaction-weighted [OH] ([OH]GM-CH4) ranges 10.3–16.3 × 105 molec cm−3 across 10 OH fields during the early 2000s, resulting in inversion-based global CH4 emissions between 518 and 757 Tg yr−1. The uncertainties in CH4 inversions induced by the different OH fields are comparable to, or even larger than the uncertainty typically given by bottom-up and top-down estimates. Based on the LMDz inversions, we estimate that a 1 %-increase in OH burden leads to an increase of 4 Tg yr−1 in the estimate of global methane emissions, which is about 25 % smaller than what is estimated by box-models. The uncertainties in emissions induced by OH are largest over South America, corresponding to large inter-model differences of [OH] in this region. From the early to the late 2000s, the optimized CH4 emissions increased by 21.9 ± 5.7 Tg yr−1 (16.6–30.0 Tg yr−1), of which ~ 25 % (on average) is contributed by −0.5 to +1.8 % increase in OH burden. If the CCMI models represent the OH trend properly over the 2000s, our results show that a higher increasing trend of CH4 emissions is needed to match the CH4 observations compared to the CH4 emission trend derived using constant OH. This study strengthens the importance to reach a better representation of OH burden and of OH spatial and temporal distributions to reduce the uncertainties on the global CH4 budget.

Download Full-text

The influence of biogenic emissions on upper-tropospheric methanol as revealed from space

Atmospheric Chemistry and Physics ◽

10.5194/acp-7-6119-2007 ◽

2007 ◽

Vol 7 (24) ◽

pp. 6119-6129 ◽

Cited By ~ 44

Author(s):

G. Dufour ◽

S. Szopa ◽

D. A. Hauglustaine ◽

C. D. Boone ◽

C. P. Rinsland ◽

...

Keyword(s):

Northern Hemisphere ◽

Biomass Burning ◽

Transport Model ◽

Tropospheric Chemistry ◽

Biogenic Emissions ◽

Chemistry Transport Model ◽

Mixing Ratios ◽

Oxygenated Compounds ◽

Global Space ◽

The Impact

Abstract. The distribution and budget of oxygenated organic compounds in the atmosphere and their impact on tropospheric chemistry are still poorly constrained. Near-global space-borne measurements of seasonally resolved upper tropospheric profiles of methanol (CH3OH) by the ACE Fourier transform spectrometer provide a unique opportunity to evaluate our understanding of this important oxygenated organic species. ACE-FTS observations from March 2004 to August 2005 period are presented. These observations reveal the pervasive imprint of surface sources on upper tropospheric methanol: mixing ratios observed in the mid and high latitudes of the Northern Hemisphere reflect the seasonal cycle of the biogenic emissions whereas the methanol cycle observed in the southern tropics is highly influenced by biomass burning emissions. The comparison with distributions simulated by the state-of-the-art global chemistry transport model, LMDz-INCA, suggests that: (i) the background methanol (high southern latitudes) is correctly represented by the model considering the measurement uncertainties; (ii) the current emissions from the continental biosphere are underestimated during spring and summer in the Northern Hemisphere leading to an underestimation of modelled upper tropospheric methanol; (iii) the seasonal variation of upper tropospheric methanol is shifted to the fall in the model suggesting either an insufficient destruction of CH3OH (due to too weak chemistry and/or deposition) in fall and winter months or an unfaithful representation of transport; (iv) the impact of tropical biomass burning emissions on upper tropospheric methanol is rather well reproduced by the model. This study illustrates the potential of these first global profile observations of oxygenated compounds in the upper troposphere to improve our understanding of their global distribution, fate and budget.

Download Full-text

Investigation of strongly enhanced methane Part I: Chemical feedbacks and rapid adjustments.

10.5194/egusphere-egu2020-9786 ◽

2020 ◽

Author(s):

Franziska Winterstein ◽

Patrick Jöckel ◽

Martin Dameris ◽

Michael Ponater ◽

Fabian Tanalski ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Radiative Forcing ◽

Climate Model ◽

Numerical Study ◽

Stratospheric Ozone ◽

Lower Boundary ◽

Tropospheric Chemistry ◽

Substantial Part ◽

Mixing Ratios ◽

The Impact

Methane (CH4) is the second most important greenhouse gas, which atmospheric concentration is influenced by human activities and currently on a sharp rise. We present a study with numerical simulations using a Chemistry-Climate-Model (CCM), which are performed to assess possible consequences of strongly enhanced CH4 concentrations in the Earth's atmosphere for the climate.Our analysis includes experiments with 2xCH4 and 5xCH4 present day (2010) lower boundary mixing ratios using the CCM EMAC. The simulations are conducted with prescribed oceanic conditions, mimicking present day tropospheric temperatures as its changes are largely suppressed. By doing so we are able to investigate the quasi-instantaneous chemical impact on the atmosphere. We find that the massive increase in CH4 strongly influences the tropospheric chemistry by reducing the OH abundance and thereby extending the tropospheric CH4 lifetime as well as the residence time of other chemical pollutants. The region above the tropopause is impacted by a substantial rise in stratospheric water vapor (SWV). The stratospheric ozone (O3) column increases overall, but SWV induced stratospheric cooling also leads to enhanced ozone depletion in the Antarctic lower stratosphere. Regional&#160; patterns of ozone change are affected by modification of stratospheric dynamics, i.e. increased tropical up-welling and stronger meridional transport&#160; towards the polar regions. We calculate the net radiative impact (RI) of the 2xCH4 experiment to be 0.69 W m-2 and for the 5xCH4 experiment to be 1.79 W m-2. A substantial part of the RI is contributed by chemically induced O3 and SWV changes, in line with previous radiative forcing estimates and is for the first time splitted and spatially asigned to its chemical contributors.This numerical study using a CCM with prescibed oceanic conditions shows the rapid responses to significantly enhanced CH4 mixing ratios, which is the first step towards investigating the impact of possible strong future CH4 emissions on atmospheric chemistry and its feedback on climate.

Download Full-text

Reduction of Climate Sensitivity to Solar Forcing due to Stratospheric Ozone Feedback

Journal of Climate ◽

10.1175/jcli-d-15-0721.1 ◽

2016 ◽

Vol 29 (12) ◽

pp. 4651-4663 ◽

Cited By ~ 13

Author(s):

G. Chiodo ◽

L. M. Polvani

Keyword(s):

Climate Models ◽

Stratospheric Ozone ◽

Computational Cost ◽

Sunspot Cycle ◽

System Response ◽

Solar Forcing ◽

Surface Solar Radiation ◽

Surface Warming ◽

Stratospheric Photochemistry ◽

The Impact

Abstract An accurate assessment of the role of solar variability is a key step toward a proper quantification of natural and anthropogenic climate change. To this end, climate models have been extensively used to quantify the solar contribution to climate variability. However, owing to the large computational cost, the bulk of modeling studies to date have been performed without interactive stratospheric photochemistry: the impact of this simplification on the modeled climate system response to solar forcing remains largely unknown. Here this impact is quantified by comparing the response of two model configurations, with and without interactive ozone chemistry. Using long integrations, robust surface temperature and precipitation responses to an idealized irradiance increase are obtained. Then, it is shown that the inclusion of interactive stratospheric chemistry significantly reduces the surface warming (by about one-third) and the accompanying precipitation response. This behavior is linked to photochemically induced stratospheric ozone changes, and their modulation of the surface solar radiation. The results herein suggest that neglecting stratospheric photochemistry leads to a sizable overestimate of the surface response to changes in solar irradiance. This has implications for simulations of the climate in the last millennium and geoengineering applications employing irradiance changes larger than those observed over the 11-yr sunspot cycle, where models often use simplified treatments of stratospheric ozone that are inconsistent with the imposed solar forcing.

Download Full-text

Impact of transport model errors on the global and regional methane emissions estimated by inverse modelling

Atmospheric Chemistry and Physics ◽

10.5194/acp-13-9917-2013 ◽

2013 ◽

Vol 13 (19) ◽

pp. 9917-9937 ◽

Cited By ~ 45

Author(s):

R. Locatelli ◽

P. Bousquet ◽

F. Chevallier ◽

A. Fortems-Cheney ◽

S. Szopa ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Transport Model ◽

Initial Conditions ◽

Spatial Scales ◽

Global Scale ◽

Methane Emissions ◽

Inverse Modelling ◽

Model Errors ◽

Inverse Systems ◽

The Impact

Abstract. A modelling experiment has been conceived to assess the impact of transport model errors on methane emissions estimated in an atmospheric inversion system. Synthetic methane observations, obtained from 10 different model outputs from the international TransCom-CH4 model inter-comparison exercise, are combined with a prior scenario of methane emissions and sinks, and integrated into the three-component PYVAR-LMDZ-SACS (PYthon VARiational-Laboratoire de Météorologie Dynamique model with Zooming capability-Simplified Atmospheric Chemistry System) inversion system to produce 10 different methane emission estimates at the global scale for the year 2005. The same methane sinks, emissions and initial conditions have been applied to produce the 10 synthetic observation datasets. The same inversion set-up (statistical errors, prior emissions, inverse procedure) is then applied to derive flux estimates by inverse modelling. Consequently, only differences in the modelling of atmospheric transport may cause differences in the estimated fluxes. In our framework, we show that transport model errors lead to a discrepancy of 27 Tg yr−1 at the global scale, representing 5% of total methane emissions. At continental and annual scales, transport model errors are proportionally larger than at the global scale, with errors ranging from 36 Tg yr−1 in North America to 7 Tg yr−1 in Boreal Eurasia (from 23 to 48%, respectively). At the model grid-scale, the spread of inverse estimates can reach 150% of the prior flux. Therefore, transport model errors contribute significantly to overall uncertainties in emission estimates by inverse modelling, especially when small spatial scales are examined. Sensitivity tests have been carried out to estimate the impact of the measurement network and the advantage of higher horizontal resolution in transport models. The large differences found between methane flux estimates inferred in these different configurations highly question the consistency of transport model errors in current inverse systems. Future inversions should include more accurately prescribed observation covariances matrices in order to limit the impact of transport model errors on estimated methane fluxes.

Download Full-text

Evaluation of the interactive stratospheric ozone (O3v2 module) for the E3SM version 2 Earth System Model

10.5194/gmd-2020-293 ◽

2020 ◽

Author(s):

Qi Tang ◽

Michael J. Prather ◽

Juno Hsu ◽

Daniel J. Ruiz ◽

Philip J. Cameron-Smith ◽

...

Keyword(s):

Climate Models ◽

Transport Model ◽

Stratospheric Ozone ◽

Earth System Model ◽

System Model ◽

Earth System ◽

Heating Rates ◽

Quasi Biennial Oscillation ◽

Column Ozone ◽

The University

Abstract. Stratospheric ozone affects climate directly as the predominant heat source in the stratosphere and indirectly through chemical feedbacks controlling other greenhouse gases. The U.S. Department of Energy's Energy Exascale Earth System Model version 1 (E3SMv1) implemented a new ozone chemistry module that improves the simulation of the sharp tropopause gradients, replacing a version based partly on long-term average climatologies that poorly represented heating rates in the lowermost stratosphere. The new O3v2 module extends seamlessly into the troposphere and preserves the naturally sharp cross-tropopause gradient, with 20-40% less ozone in this region. Additionally, O3v2 enables the diagnosis of stratosphere-troposphere exchange flux of ozone, a key budget term lacking in E3SMv1. Here, we evaluate key features in ozone abundance and other closely related quantities in atmosphere-only E3SMv1 simulations driven by observed sea surface temperatures (SSTs, years 1990-2014), comparing with satellite observations and the University of California, Irvine chemistry transport model (UCI CTM) using the same stratospheric chemistry scheme but driven by European Centre forecast fields for the same period. In terms of stratospheric column ozone, O3v2 shows improved mean bias and northern mid-latitude variability, but not quite as good as the UCI CTM. As expected, SST forcing does not match the observed quasi-biennial oscillation, which is mostly matched with the UCI CTM. This new O3v2 E3SM model retains mostly the same climate state and climate sensitivity as the previous version, and we recommend its use for other climate models that still use ozone climatologies.

Download Full-text

Stratospheric lifetime ratio of CFC-11 and CFC-12 from satellite and model climatologies

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-14-16865-2014 ◽

2014 ◽

Vol 14 (11) ◽

pp. 16865-16906 ◽

Cited By ~ 3

Author(s):

L. Hoffmann ◽

C. M. Hoppe ◽

R. Müller ◽

G. S. Dutton ◽

J. C. Gille ◽

...

Keyword(s):

Global Warming ◽

Atmospheric Chemistry ◽

Climate Model ◽

Transport Model ◽

Stratospheric Ozone ◽

Michelson Interferometer ◽

Coupled Model ◽

Model System ◽

Satellite Observations ◽

The Impact

Abstract. Chlorofluorocarbons (CFCs) play a key role in stratospheric ozone loss and are strong infrared absorbers that contribute to global warming. The stratospheric lifetimes of CFCs are a measure of their global loss rates that are needed to determine global warming and ozone depletion potentials. We applied the tracer-tracer correlation approach to zonal mean climatologies from satellite measurements and model data to assess the lifetimes of CFCl3 (CFC-11) and CF2Cl2 (CFC-12). We present estimates of the CFC-11/CFC-12 lifetime ratio and the absolute lifetime of CFC-12, based on a reference lifetime of 52 yr for CFC-11. We analyzed climatologies from three satellite missions, the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), the HIgh Resolution Dynamics Limb Sounder (HIRDLS), and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). We found a CFC-11/CFC-12 lifetime ratio of 0.47±0.08 and a CFC-12 lifetime of 111(96–132) yr for ACE-FTS, a ratio of 0.46±0.07 and a lifetime of 112(97–133) yr for HIRDLS, and a ratio of 0.46±0.08 and a lifetime of 112(96–135) yr for MIPAS. The error-weighted, combined CFC-11/CFC-12 lifetime ratio is 0.47±0.04 and the CFC-12 lifetime estimate is 112(102–123) yr. These results agree with the recent Stratosphere-troposphere Processes And their Role in Climate (SPARC) reassessment, which recommends lifetimes of 52(43–67) yr and 102(88–122) yr, respectively. Having smaller uncertainties than the results from other recent studies, our estimates can help to better constrain CFC-11 and CFC-12 lifetime recommendations in future scientific studies and assessments. Furthermore, the satellite observations were used to validate first simulation results from a new coupled model system, which integrates a Lagrangian chemistry transport model into a climate model. For the coupled model we found a CFC-11/CFC-12 lifetime ratio of 0.48±0.07 and a CFC-12 lifetime of 110(95–129) yr, based on a ten-year perpetual run. Closely reproducing the satellite observations, the new model system will likely become a useful tool to assess the impact of advective transport, mixing, and photochemistry as well as climatological variability on the stratospheric lifetimes of long-lived tracers.

Download Full-text