The representation of solar cycle signals in stratospheric ozone –  Part 2: Analysis of global models

Abstract. The impact of changes in incoming solar irradiance on stratospheric ozone abundances should be included in climate simulations to aid in capturing the atmospheric response to solar cycle variability. This study presents the first systematic comparison of the representation of the 11-year solar cycle ozone response (SOR) in chemistry–climate models (CCMs) and in pre-calculated ozone databases specified in climate models that do not include chemistry, with a special focus on comparing the recommended protocols for the Coupled Model Intercomparison Project Phase 5 and Phase 6 (CMIP5 and CMIP6). We analyse the SOR in eight CCMs from the Chemistry–Climate Model Initiative (CCMI-1) and compare these with results from three ozone databases for climate models: the Bodeker Scientific ozone database, the SPARC/Atmospheric Chemistry and Climate (AC&C) ozone database for CMIP5 and the SPARC/CCMI ozone database for CMIP6. The peak amplitude of the annual mean SOR in the tropical upper stratosphere (1–5 hPa) decreases by more than a factor of 2, from around 5 to 2 %, between the CMIP5 and CMIP6 ozone databases. This substantial decrease can be traced to the CMIP5 ozone database being constructed from a regression model fit to satellite and ozonesonde measurements, while the CMIP6 database is constructed from CCM simulations. The SOR in the CMIP6 ozone database therefore implicitly resembles the SOR in the CCMI-1 models. The structure in latitude of the SOR in the CMIP6 ozone database and CCMI-1 models is considerably smoother than in the CMIP5 database, which shows unrealistic sharp gradients in the SOR across the middle latitudes owing to the paucity of long-term ozone measurements in polar regions. The SORs in the CMIP6 ozone database and the CCMI-1 models show a seasonal dependence with enhanced meridional gradients at mid- to high latitudes in the winter hemisphere. The CMIP5 ozone database does not account for seasonal variations in the SOR, which is unrealistic. Sensitivity experiments with a global atmospheric model without chemistry (ECHAM6.3) are performed to assess the atmospheric impacts of changes in the representation of the SOR and solar spectral irradiance (SSI) forcing between CMIP5 and CMIP6. The larger amplitude of the SOR in the CMIP5 ozone database compared to CMIP6 causes a likely overestimation of the modelled tropical stratospheric temperature response between 11-year solar cycle minimum and maximum by up to 0.55 K, or around 80 % of the total amplitude. This effect is substantially larger than the change in temperature response due to differences in SSI forcing between CMIP5 and CMIP6. The results emphasize the importance of adequately representing the SOR in global models to capture the impact of the 11-year solar cycle on the atmosphere. Since a number of limitations in the representation of the SOR in the CMIP5 ozone database have been identified, we recommend that CMIP6 models without chemistry use the CMIP6 ozone database and the CMIP6 SSI dataset to better capture the climate impacts of solar variability. The SOR coefficients from the CMIP6 ozone database are published with this paper.

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 representation of solar cycle signals in stratospheric ozone – Part 1: A comparison of satellite observations

10.5194/acp-2015-882 ◽

2016 ◽

Author(s):

A. Maycock ◽

K. Matthes ◽

S. Tegtmeier ◽

R. Thiéblemont ◽

L. Hood

Keyword(s):

Solar Cycle ◽

Climate Models ◽

Stratospheric Ozone ◽

Satellite Observations ◽

Solar Variability ◽

Temperature Measurements ◽

Climate Response ◽

Mixing Ratio ◽

Substantial Impact ◽

The Impact

Abstract. The impact of changes in incoming solar ultraviolet irradiance on stratospheric ozone forms an important part of the climate response to solar variability. To realistically simulate the climate response to solar variability using climate models, a minimum requirement is that they should include a solar cycle ozone component that has a realistic amplitude and structure, and which varies with season. For climate models that do not include interactive ozone chemistry, this component must be derived from observations and/or chemistry–climate model simulations and included in an externally prescribed ozone database that also includes the effects of all major external forcings. Part 1 of this two part study presents the solar-ozone responses in a number of updated satellite datasets for the period 1984–2004, including the Stratospheric Aerosol and Gas Experiment (SAGE) II version 6.2 and version 7.0 data, and the Solar Backscatter Ultraviolet Instrument (SBUV) version 8.0 and version 8.6 data. A number of combined datasets, which have extended SAGE II using more recent satellite measurements, are also analysed for the period 1984–2011. It is shown that SAGE II derived solar-ozone signals are sensitive to the independent temperature measurements used to convert ozone number density to mixing ratio units. A change in these temperature measurements in the recent SAGE II v7.0 data leads to substantial differences in the mixing ratio solar-ozone response compared to the previous v6.2, particularly in the tropical upper stratosphere. We also show that alternate satellite ozone datasets have issues (e.g., sparse spatial and temporal sampling, low vertical resolution, and shortness of measurement record), and that the methods of accounting for instrument offsets and drifts in merged satellite datasets can have a substantial impact on the solar cycle signal in ozone. For example, the magnitude of the solar-ozone response varies by around a factor of two across different versions of the SBUV VN8.6 record, which appears to be due to the methods used to combine the separate SBUV timeseries. These factors make it difficult to extract more than an annual-mean solar-ozone response from the available satellite observations. It is therefore unlikely that satellite ozone measurements alone can be applied to estimate the necessary solar cycle ozone component of the prescribed ozone database for future coupled model intercomparison projects (e.g., CMIP6).

Download Full-text

Case studies of the impact of orbital sampling on stratospheric trend detection and derivation of tropical vertical velocities: solar occultation vs. limb emission sounding

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-11521-2016 ◽

2016 ◽

Vol 16 (18) ◽

pp. 11521-11534 ◽

Cited By ~ 9

Author(s):

Luis F. Millán ◽

Nathaniel J. Livesey ◽

Michelle L. Santee ◽

Jessica L. Neu ◽

Gloria L. Manney ◽

...

Keyword(s):

Case Studies ◽

Atmospheric Chemistry ◽

Stratospheric Ozone ◽

Sampling Bias ◽

Nonuniform Sampling ◽

Trend Detection ◽

Trace Gas ◽

Uniform Sampling ◽

Solar Occultation ◽

The Impact

Abstract. This study investigates the representativeness of two types of orbital sampling applied to stratospheric temperature and trace gas fields. Model fields are sampled using real sampling patterns from the Aura Microwave Limb Sounder (MLS), the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The MLS sampling acts as a proxy for a dense uniform sampling pattern typical of limb emission sounders, while HALOE and ACE-FTS represent coarse nonuniform sampling patterns characteristic of solar occultation instruments. First, this study revisits the impact of sampling patterns in terms of the sampling bias, as previous studies have done. Then, it quantifies the impact of different sampling patterns on the estimation of trends and their associated detectability. In general, we find that coarse nonuniform sampling patterns may introduce non-negligible errors in the inferred magnitude of temperature and trace gas trends and necessitate considerably longer records for their definitive detection. Lastly, we explore the impact of these sampling patterns on tropical vertical velocities derived from stratospheric water vapor measurements. We find that coarse nonuniform sampling may lead to a biased depiction of the tropical vertical velocities and, hence, to a biased estimation of the impact of the mechanisms that modulate these velocities. These case studies suggest that dense uniform sampling such as that available from limb emission sounders provides much greater fidelity in detecting signals of stratospheric change (for example, fingerprints of greenhouse gas warming and stratospheric ozone recovery) than coarse nonuniform sampling such as that of solar occultation instruments.

Download Full-text

Sensitivity of the tropical stratospheric ozone response to the solar rotational cycle in observations and chemistry-climate model simulations

10.5194/acp-2016-1102 ◽

2017 ◽

Author(s):

Rémi Thiéblemont ◽

Marion Marchand ◽

Slimane Bekki ◽

Sébastien Bossay ◽

Franck Lefèvre ◽

...

Keyword(s):

Solar Cycle ◽

Climate Model ◽

Time Window ◽

Stratospheric Ozone ◽

Spectral Irradiance ◽

Naval Research ◽

Solar Spectral Irradiance ◽

Model Free ◽

Ozone Sensitivity ◽

Ensemble Mean

Abstract. The tropical stratospheric ozone response to solar UV variations associated with the rotational cycle (~ 27 days) is analysed using MLS satellite observations and numerical simulations from the LMDz-Reprobus chemistry-climate model. The model is used in two configurations, as a chemistry-transport model (CTM) where dynamics are nudged toward ERA-Interim reanalysis and as a chemistry-climate model (free-running) (CCM). An ensemble of five 17 year simulations (1991–2007) is performed with the CCM. All simulations are forced by reconstructed time-varying solar spectral irradiance from the Naval Research Laboratory Solar Spectral Irradiance model. We first examine the ozone response to the solar rotational cycle during two 3 year periods which correspond to the declining phases of solar cycle 22 (10/1991–09/1994) and solar cycle 23 (09/200408/2007) when the satellite ozone observations of the two Microwave Limb Sounders (MLS-UARS and MLS-Aura) are available. In the observations, during the first period, ozone and UV flux are found to be correlated between about 10 and 1 hPa with a maximum of 0.29 at ~ 5 hPa; the ozone sensitivity (% change in ozone for 1 % change in UV) peaks at ~ 0.4. Correlation during the second period is weaker and has a peak ozone sensitivity of only 0.2, possibly due to the fact that the solar forcing is weaker during that period. The CTM simulation reproduces most of these observed features, including the differences between the two periods. The CCM ensemble mean results comparatively show much smaller differences between the two periods, suggesting that the amplitude of the rotational ozone signal estimated from MLS observations or the CTM simulation is strongly influenced by other (non-solar) sources of variability, notably dynamics. The analysis of the ensemble of CCM simulations shows that the estimation of the ensemble mean ozone sensitivity does not vary significantly neither with the amplitude of the solar rotational fluctuations, nor with the size of the time window used for the ozone sensitivity retrieval. In contrast, the uncertainty of the ozone sensitivity estimate significantly increases during periods of decreasing amplitude of solar rotational fluctuations (also coinciding with minimum phases of the solar cycle), and for decreasing size of the time window analysis. We found that a minimum of 3 year and 10 year time window is needed for the 1σ uncertainty to drop below 50 % and 20 %, respectively. These uncertainty sources may explain some of the discrepancies found in previous estimates of the ozone response to the solar rotational cycle.

Download Full-text

Atmospheric impacts of short-lived chlorinated species over the recent past: a chemistry-climate perspective

10.5194/egusphere-egu21-12824 ◽

2021 ◽

Author(s):

Ewa Bednarz ◽

Ryan Hossaini ◽

Luke Abraham ◽

Peter Braesicke ◽

Martyn Chipperfield

Keyword(s):

Atmospheric Chemistry ◽

Climate Model ◽

Stratospheric Ozone ◽

Lower Boundary ◽

Montreal Protocol ◽

Recent Past ◽

Substantial Impact ◽

Ozone Depleting Substances ◽

The Impact

The emissions of most long-lived halogenated ozone-depleting substances (ODSs) are now decreasing, owing to controls on their production introduced by Montreal Protocol and its amendments. However, short-lived halogenated compounds can also have substantial impact on atmospheric chemistry, including stratospheric ozone, particularly if emitted near climatological uplift regions. It has recently become evident that emissions of some chlorinated very short-lived species (VSLSs), such as chloroform (CHCl3) and dichloromethane (CH2Cl2), could be larger than previously believed and increasing, particularly in Asia. While these may exert a significant influence on atmospheric chemistry and climate, their impacts remain poorly characterised.&#160;&#160;We address this issue using the UM-UKCA chemistry-climate model (CCM). While not only the first, to our knowledge, model study addressing this problem using a CCM, it is also the first such study employing a whole atmosphere model, thereby simulating the tropospheric Cl-VSLSs emissions and the resulting stratospheric impacts in a fully consistent manner. We use a newly developed Double-Extended Stratospheric-Tropospheric (DEST) chemistry scheme, which includes emissions of all major chlorinated and brominated VSLSs alongside an extended treatment of long-lived ODSs.&#160;We examine the impacts of rising Cl-VSLSs emissions on atmospheric chlorine tracers and ozone, including their long-term trends. We pay particular attention to the role of &#8216;nudging&#8217;, as opposed to the free-running model set up, for the simulated Cl-VSLSs impacts, thereby demostrating the role of atmospheric dynamics in modulating the atmospheric responses to Cl-VSLSs. In addition, we employ novel estimates of Cl-VSLS emissions over the recent past and compare the results with the simulations that prescribe Cl-VSLSs using simple lower boundary conditions. This allows us to demonstrate the impact such choice has on the dominant location and seasonality of the Cl-VSLSs transport into the stratosphere.

Download Full-text

On the impact of future climate change on tropopause folds and tropospheric ozone

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-14387-2019 ◽

2019 ◽

Vol 19 (22) ◽

pp. 14387-14401 ◽

Cited By ~ 2

Author(s):

Dimitris Akritidis ◽

Andrea Pozzer ◽

Prodromos Zanis

Keyword(s):

Atmospheric Chemistry ◽

Tropospheric Ozone ◽

Eastern Mediterranean ◽

Stratospheric Ozone ◽

Lower Troposphere ◽

Future Climate Change ◽

Identification Algorithm ◽

The Future ◽

Projected Changes ◽

The Impact

Abstract. Using a transient simulation for the period 1960–2100 with the state-of-the-art ECHAM5/MESSy Atmospheric Chemistry (EMAC) global model and a tropopause fold identification algorithm, we explore the future projected changes in tropopause folds, stratosphere-to-troposphere transport (STT) of ozone, and tropospheric ozone under the RCP6.0 scenario. Statistically significant changes in tropopause fold frequencies from 1970–1999 to 2070–2099 are identified in both hemispheres, regionally exceeding 3 %, and are associated with the projected changes in the position and intensity of the subtropical jet streams. A strengthening of ozone STT is projected for the future in both hemispheres, with an induced increase in transported stratospheric ozone tracer throughout the whole troposphere, reaching up to 10 nmol mol−1 in the upper troposphere, 8 nmol mol−1 in the middle troposphere, and 3 nmol mol−1 near the surface. Notably, the regions exhibiting the largest changes of ozone STT at 400 hPa coincide with those with the highest fold frequency changes, highlighting the role of the tropopause folding mechanism in STT processes under a changing climate. For both the eastern Mediterranean and Middle East (EMME) and Afghanistan (AFG) regions, which are known as hotspots of fold activity and ozone STT during the summer period, the year-to-year variability of middle-tropospheric ozone with stratospheric origin is largely explained by the short-term variations in ozone at 150 hPa and tropopause fold frequency. Finally, ozone in the lower troposphere is projected to decrease under the RCP6.0 scenario during MAM (March, April, and May) and JJA (June, July, and August) in the Northern Hemisphere and during DJF (December, January, and February) in the Southern Hemisphere, due to the decline of ozone precursor emissions and the enhanced ozone loss from higher water vapour abundances, while in the rest of the troposphere ozone shows a remarkable increase owing mainly to the STT strengthening and the stratospheric ozone recovery.

Download Full-text

AerChemMIP: quantifying the effects of chemistry and aerosols in CMIP6

Geoscientific Model Development ◽

10.5194/gmd-10-585-2017 ◽

2017 ◽

Vol 10 (2) ◽

pp. 585-607 ◽

Cited By ~ 66

Author(s):

William J. Collins ◽

Jean-François Lamarque ◽

Michael Schulz ◽

Olivier Boucher ◽

Veronika Eyring ◽

...

Keyword(s):

Air Quality ◽

Atmospheric Chemistry ◽

Radiative Forcing ◽

Climate Models ◽

Coupled Model ◽

Climate Impacts ◽

Atmospheric Composition ◽

Historical Period ◽

Model Intercomparison ◽

Intercomparison Project

Abstract. The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) is endorsed by the Coupled-Model Intercomparison Project 6 (CMIP6) and is designed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. These are specifically near-term climate forcers (NTCFs: methane, tropospheric ozone and aerosols, and their precursors), nitrous oxide and ozone-depleting halocarbons. The aim of AerChemMIP is to answer four scientific questions. 1. How have anthropogenic emissions contributed to global radiative forcing and affected regional climate over the historical period? 2. How might future policies (on climate, air quality and land use) affect the abundances of NTCFs and their climate impacts? 3.How do uncertainties in historical NTCF emissions affect radiative forcing estimates? 4. How important are climate feedbacks to natural NTCF emissions, atmospheric composition, and radiative effects? These questions will be addressed through targeted simulations with CMIP6 climate models that include an interactive representation of tropospheric aerosols and atmospheric chemistry. These simulations build on the CMIP6 Diagnostic, Evaluation and Characterization of Klima (DECK) experiments, the CMIP6 historical simulations, and future projections performed elsewhere in CMIP6, allowing the contributions from aerosols and/or chemistry to be quantified. Specific diagnostics are requested as part of the CMIP6 data request to highlight the chemical composition of the atmosphere, to evaluate the performance of the models, and to understand differences in behaviour between them.

Download Full-text

Observed Tropospheric Temperature Response to 11-yr Solar Cycle and What It Reveals about Mechanisms

Journal of the Atmospheric Sciences ◽

10.1175/jas-d-12-0214.1 ◽

2013 ◽

Vol 70 (1) ◽

pp. 9-14 ◽

Cited By ~ 9

Author(s):

Jiansong Zhou ◽

Ka-Kit Tung

Keyword(s):

Solar Cycle ◽

Large Scale ◽

Stratospheric Ozone ◽

Statistical Significance ◽

Temperature Response ◽

Polar Regions ◽

Tropospheric Temperature ◽

Tropical Ocean ◽

Global Data ◽

Difference Projection

Abstract Using 54 yr of NCEP reanalysis global data from 1000 to 10 hPa, this study establishes the existence and the statistical significance of the zonal-mean temperature response to the 11-yr solar cycle throughout the troposphere and parts of the lower stratosphere. Two types of statistical analysis are used: the composite-mean difference projection method, which tests the existence of the solar cycle signal level by level, and the adaptive AR(p)-t test, which tells if a particular local feature is statistically significant at the 95% confidence level. A larger area of statistical significance than that in previous published work is obtained, due to the longer record and a better trend removal process. It reveals a spatial pattern consistent with a “bottom up” mechanism, involving evaporative feedback near the tropical ocean surface and tropical vertical convection, latent heating of the tropical upper troposphere, and poleward large-scale heat transport to the polar regions. It provides an alternative to the currently favored “top down” mechanism involving stratospheric ozone heating.

Download Full-text

Climate forcing and committed global warming: GHGs, aerosols and ozone 1970-2010

10.5194/egusphere-egu2020-19702 ◽

2020 ◽

Author(s):

Alcide Zhao ◽

David Stevenson ◽

Massimi Bollasina

Keyword(s):

Radiative Forcing ◽

Daily Precipitation ◽

Stratospheric Ozone ◽

Temperature Response ◽

Climate Impacts ◽

Climate Projections ◽

Anthropogenic Aerosols ◽

Frequency Distributions ◽

Climate Risks ◽

Global Mean

It is crucial to reduce uncertainties in our understanding of the climate impacts of short&#8208;lived climate forcers, in the context that their emissions/concentrations are anticipated to decrease significantly in the coming decades worldwide. Using the Community Earth System Model (CESM1), we performed time&#8208;slice experiments to investigate the effective radiative forcing (ERF) and climate respons to 1970&#8211;2010 changes in well&#8208;mixed greenhouse gases (GHGs), anthropogenic aerosols, and tropospheric and stratospheric ozone. Once the present&#8208;day climate has fully responded to 1970&#8211;2010 changes in all forcings, both the global mean temperature and precipitation responses are twice as large as the transient ones, with wet regions getting wetter and dry regions drier. The temperature response per unit ERF for short&#8208;lived species varies considerably across many factors including forcing agents and the magnitudes and locations of emission changes. This suggests that the ERF should be used carefully to interpret the climate impacts of short&#8208;lived climate forcers. Changes in both the mean and the probability distribution of global mean daily precipitation are driven mainly by GHG increases. However, changes in the frequency distributions of regional mean daily precipitation are more strongly influenced by changes in aerosols, rather than GHGs. This is particularly true over Asia and Europe where aerosol changes have significant impacts on the frequency of heavy&#8208;to&#8208;extreme precipitation. Our results may help guide more reliable near&#8208;future climate projections and allow us to manage climate risks more effectively.

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