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  • 1
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    Stratospheric Injection of Brominated Very Short‐Lived Substances: Aircraft Observations in the Western Pacific and Representation in Global Models
    American Geophysical Union (AGU) ; 2018
    In:  Journal of Geophysical Research: Atmospheres Vol. 123, No. 10 ( 2018-05-27), p. 5690-5719
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 123, No. 10 ( 2018-05-27), p. 5690-5719
    Abstract: Based on winter 2014 observations, very short‐lived bromocarbons produced by oceanic biology contribute 5 ± 2 ppt to stratospheric bromine Of the bromine from very short‐lived substances that reaches the stratosphere, 60% enters as organic species and 40% as inorganic species Representation of stratospheric bromine within global models is greatly improved upon consideration of very short‐lived bromocarbons
    Type of Medium: Online Resource
    ISSN: 2169-897X , 2169-8996
    URL: Article
    DOI: 10.1029/2017JD027978
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2018
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  • 2
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    Attribution of Chemistry-Climate Model Initiative (CCMI) ozone radiative flux bias from satellites
    Copernicus GmbH ; 2020
    In:  Atmospheric Chemistry and Physics Vol. 20, No. 1 ( 2020-01-08), p. 281-301
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 1 ( 2020-01-08), p. 281-301
    Abstract: Abstract. The top-of-atmosphere (TOA) outgoing longwave flux over the 9.6 µm ozone band is a fundamental quantity for understanding chemistry–climate coupling. However, observed TOA fluxes are hard to estimate as they exhibit considerable variability in space and time that depend on the distributions of clouds, ozone (O3), water vapor (H2O), air temperature (Ta), and surface temperature (Ts). Benchmarking present-day fluxes and quantifying the relative influence of their drivers is the first step for estimating climate feedbacks from ozone radiative forcing and predicting radiative forcing evolution. To that end, we constructed observational instantaneous radiative kernels (IRKs) under clear-sky conditions, representing the sensitivities of the TOA flux in the 9.6 µm ozone band to the vertical distribution of geophysical variables, including O3, H2O, Ta, and Ts based upon the Aura Tropospheric Emission Spectrometer (TES) measurements. Applying these kernels to present-day simulations from the Chemistry-Climate Model Initiative (CCMI) project as compared to a 2006 reanalysis assimilating satellite observations, we show that the models have large differences in TOA flux, attributable to different geophysical variables. In particular, model simulations continue to diverge from observations in the tropics, as reported in previous studies of the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP) simulations. The principal culprits are tropical middle and upper tropospheric ozone followed by tropical lower tropospheric H2O. Five models out of the eight studied here have TOA flux biases exceeding 100 mW m−2 attributable to tropospheric ozone bias. Another set of five models have flux biases over 50 mW m−2 due to H2O. On the other hand, Ta radiative bias is negligible in all models (no more than 30 mW m−2). We found that the atmospheric component (AM3) of the Geophysical Fluid Dynamics Laboratory (GFDL) general circulation model and Canadian Middle Atmosphere Model (CMAM) have the lowest TOA flux biases globally but are a result of cancellation of opposite biases due to different processes. Overall, the multi-model ensemble mean bias is -133±98 mW m−2, indicating that they are too atmospherically opaque due to trapping too much radiation in the atmosphere by overestimated tropical tropospheric O3 and H2O. Having too much O3 and H2O in the troposphere would have different impacts on the sensitivity of TOA flux to O3 and these competing effects add more uncertainties on the ozone radiative forcing. We find that the inter-model TOA outgoing longwave radiation (OLR) difference is well anti-correlated with their ozone band flux bias. This suggests that there is significant radiative compensation in the calculation of model outgoing longwave radiation.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-20-281-2020
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2092549-9
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  • 3
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    No robust evidence of future changes in major stratospheric sudden warmings: a multi-model assessment from CCMI
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 15 ( 2018-08-13), p. 11277-11287
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 15 ( 2018-08-13), p. 11277-11287
    Abstract: Abstract. Major mid-winter stratospheric sudden warmings (SSWs) are the largest instance of wintertime variability in the Arctic stratosphere. Because SSWs are able to cause significant surface weather anomalies on intra-seasonal timescales, several previous studies have focused on their potential future change, as might be induced by anthropogenic forcings. However, a wide range of results have been reported, from a future increase in the frequency of SSWs to an actual decrease. Several factors might explain these contradictory results, notably the use of different metrics for the identification of SSWs and the impact of large climatological biases in single-model studies. To bring some clarity, we here revisit the question of future SSW changes, using an identical set of metrics applied consistently across 12 different models participating in the Chemistry–Climate Model Initiative. Our analysis reveals that no statistically significant change in the frequency of SSWs will occur over the 21st century, irrespective of the metric used for the identification of the event. Changes in other SSW characteristics – such as their duration, deceleration of the polar night jet, and the tropospheric forcing – are also assessed: again, we find no evidence of future changes over the 21st century.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-18-11277-2018
    DOI: 10.5194/acp-18-11277-2018-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 4
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    The influence of mixing on the stratospheric age of air changes in the 21st century
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 2 ( 2019-01-24), p. 921-940
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 2 ( 2019-01-24), p. 921-940
    Abstract: Abstract. Climate models consistently predict an acceleration of the Brewer–Dobson circulation (BDC) due to climate change in the 21st century. However, the strength of this acceleration varies considerably among individual models, which constitutes a notable source of uncertainty for future climate projections. To shed more light upon the magnitude of this uncertainty and on its causes, we analyse the stratospheric mean age of air (AoA) of 10 climate projection simulations from the Chemistry-Climate Model Initiative phase 1 (CCMI-I), covering the period between 1960 and 2100. In agreement with previous multi-model studies, we find a large model spread in the magnitude of the AoA trend over the simulation period. Differences between future and past AoA are found to be predominantly due to differences in mixing (reduced aging by mixing and recirculation) rather than differences in residual mean transport. We furthermore analyse the mixing efficiency, a measure of the relative strength of mixing for given residual mean transport, which was previously hypothesised to be a model constant. Here, the mixing efficiency is found to vary not only across models, but also over time in all models. Changes in mixing efficiency are shown to be closely related to changes in AoA and quantified to roughly contribute 10 % to the long-term AoA decrease over the 21st century. Additionally, mixing efficiency variations are shown to considerably enhance model spread in AoA changes. To understand these mixing efficiency variations, we also present a consistent dynamical framework based on diffusive closure, which highlights the role of basic state potential vorticity gradients in controlling mixing efficiency and therefore aging by mixing.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-921-2019
    DOI: 10.5194/acp-19-921-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 5
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    The effect of atmospheric nudging on the stratospheric residual circulation in chemistry–climate models
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 17 ( 2019-09-13), p. 11559-11586
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 17 ( 2019-09-13), p. 11559-11586
    Abstract: Abstract. We perform the first multi-model intercomparison of the impact of nudged meteorology on the stratospheric residual circulation using hindcast simulations from the Chemistry–Climate Model Initiative (CCMI). We examine simulations over the period 1980–2009 from seven models in which the meteorological fields are nudged towards a reanalysis dataset and compare these with their equivalent free-running simulations and the reanalyses themselves. We show that for the current implementations, nudging meteorology does not constrain the mean strength of the stratospheric residual circulation and that the inter-model spread is similar, or even larger, than in the free-running simulations. The nudged models generally show slightly stronger upwelling in the tropical lower stratosphere compared to the free-running versions and exhibit marked differences compared to the directly estimated residual circulation from the reanalysis dataset they are nudged towards. Downward control calculations applied to the nudged simulations reveal substantial differences between the climatological lower-stratospheric tropical upward mass flux (TUMF) computed from the modelled wave forcing and that calculated directly from the residual circulation. This explicitly shows that nudging decouples the wave forcing and the residual circulation so that the divergence of the angular momentum flux due to the mean motion is not balanced by eddy motions, as would typically be expected in the time mean. Overall, nudging meteorological fields leads to increased inter-model spread for most of the measures of the mean climatological stratospheric residual circulation assessed in this study. In contrast, the nudged simulations show a high degree of consistency in the inter-annual variability in the TUMF in the lower stratosphere, which is primarily related to the contribution to variability from the resolved wave forcing. The more consistent inter-annual variability in TUMF in the nudged models also compares more closely with the variability found in the reanalyses, particularly in boreal winter. We apply a multiple linear regression (MLR) model to separate the drivers of inter-annual and long-term variations in the simulated TUMF; this explains up to ∼75 % of the variance in TUMF in the nudged simulations. The MLR model reveals a statistically significant positive trend in TUMF for most models over the period 1980–2009. The TUMF trend magnitude is generally larger in the nudged models compared to their free-running counterparts, but the intermodel range of trends doubles from around a factor of 2 to a factor of 4 due to nudging. Furthermore, the nudged models generally do not match the TUMF trends in the reanalysis they are nudged towards for trends over different periods in the interval 1980–2009. Hence, we conclude that nudging does not strongly constrain long-term trends simulated by the chemistry–climate model (CCM) in the residual circulation. Our findings show that while nudged simulations may, by construction, produce accurate temperatures and realistic representations of fast horizontal transport, this is not typically the case for the slower zonal mean vertical transport in the stratosphere. Consequently, caution is required when using nudged simulations to interpret the behaviour of stratospheric tracers that are affected by the residual circulation.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-11559-2019
    DOI: 10.5194/acp-19-11559-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 6
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    Stratospheric ozone loss over the Eurasian continent induced by the polar vortex shift
    Springer Science and Business Media LLC ; 2018
    In:  Nature Communications Vol. 9, No. 1 ( 2018-01-15)
    Details
    In: Nature Communications, Springer Science and Business Media LLC, Vol. 9, No. 1 ( 2018-01-15)
    Abstract: The Montreal Protocol has succeeded in limiting major ozone-depleting substance emissions, and consequently stratospheric ozone concentrations are expected to recover this century. However, there is a large uncertainty in the rate of regional ozone recovery in the Northern Hemisphere. Here we identify a Eurasia-North America dipole mode in the total column ozone over the Northern Hemisphere, showing negative and positive total column ozone anomaly centres over Eurasia and North America, respectively. The positive trend of this mode explains an enhanced total column ozone decline over the Eurasian continent in the past three decades, which is closely related to the polar vortex shift towards Eurasia. Multiple chemistry-climate-model simulations indicate that the positive Eurasia-North America dipole trend in late winter is likely to continue in the near future. Our findings suggest that the anticipated ozone recovery in late winter will be sensitive not only to the ozone-depleting substance decline but also to the polar vortex changes, and could be substantially delayed in some regions of the Northern Hemisphere extratropics.
    Type of Medium: Online Resource
    ISSN: 2041-1723
    URL: Article
    DOI: 10.1038/s41467-017-02565-2
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2018
    detail.hit.zdb_id: 2553671-0
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  • 7
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    Clear-sky ultraviolet radiation modelling using output from the Chemistry Climate Model Initiative
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 15 ( 2019-08-12), p. 10087-10110
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 15 ( 2019-08-12), p. 10087-10110
    Abstract: Abstract. We have derived values of the ultraviolet index (UVI) at solar noon using the Tropospheric Ultraviolet Model (TUV) driven by ozone, temperature and aerosol fields from climate simulations of the first phase of the Chemistry-Climate Model Initiative (CCMI-1). Since clouds remain one of the largest uncertainties in climate projections, we simulated only the clear-sky UVI. We compared the modelled UVI climatologies against present-day climatological values of UVI derived from both satellite data (the OMI-Aura OMUVBd product) and ground-based measurements (from the NDACC network). Depending on the region, relative differences between the UVI obtained from CCMI/TUV calculations and the ground-based measurements ranged between −5.9 % and 10.6 %. We then calculated the UVI evolution throughout the 21st century for the four Representative Concentration Pathways (RCPs 2.6, 4.5, 6.0 and 8.5). Compared to 1960s values, we found an average increase in the UVI in 2100 (of 2 %–4 %) in the tropical belt (30∘ N–30∘ S). For the mid-latitudes, we observed a 1.8 % to 3.4 % increase in the Southern Hemisphere for RCPs 2.6, 4.5 and 6.0 and found a 2.3 % decrease in RCP 8.5. Higher increases in UVI are projected in the Northern Hemisphere except for RCP 8.5. At high latitudes, ozone recovery is well identified and induces a complete return of mean UVI levels to 1960 values for RCP 8.5 in the Southern Hemisphere. In the Northern Hemisphere, UVI levels in 2100 are higher by 0.5 % to 5.5 % for RCPs 2.6, 4.5 and 6.0 and they are lower by 7.9 % for RCP 8.5. We analysed the impacts of greenhouse gases (GHGs) and ozone-depleting substances (ODSs) on UVI from 1960 by comparing CCMI sensitivity simulations (1960–2100) with fixed GHGs or ODSs at their respective 1960 levels. As expected with ODS fixed at their 1960 levels, there is no large decrease in ozone levels and consequently no sudden increase in UVI levels. With fixed GHG, we observed a delayed return of ozone to 1960 values, with a corresponding pattern of change observed on UVI, and looking at the UVI difference between 2090s values and 1960s values, we found an 8 % increase in the tropical belt during the summer of each hemisphere. Finally we show that, while in the Southern Hemisphere the UVI is mainly driven by total ozone column, in the Northern Hemisphere both total ozone column and aerosol optical depth drive UVI levels, with aerosol optical depth having twice as much influence on the UVI as total ozone column does.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-19-10087-2019
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
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  • 8
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    The representation of solar cycle signals in stratospheric ozone – Part 2: Analysis of global models
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 15 ( 2018-08-13), p. 11323-11343
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 15 ( 2018-08-13), p. 11323-11343
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-18-11323-2018
    DOI: 10.5194/acp-18-11323-2018-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 9
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    A machine learning examination of hydroxyl radical differences among model simulations for CCMI-1
    Copernicus GmbH ; 2020
    In:  Atmospheric Chemistry and Physics Vol. 20, No. 3 ( 2020-02-05), p. 1341-1361
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 3 ( 2020-02-05), p. 1341-1361
    Abstract: Abstract. The hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting methane lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among 10 models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D), the mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapour, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, methane, the photolysis frequency of NO2 by visible light (JNO2), overhead ozone column, and temperature account for little to no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapour on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, ozone column, and temperature are also in reasonably good agreement between the two studies.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-20-1341-2020
    DOI: 10.5194/acp-20-1341-2020-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 10
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    Large-scale tropospheric transport in the Chemistry–Climate Model Initiative (CCMI) simulations
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 10 ( 2018-05-25), p. 7217-7235
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 10 ( 2018-05-25), p. 7217-7235
    Abstract: Abstract. Understanding and modeling the large-scale transport of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. Here we show that there are large differences in the global-scale atmospheric transport properties among the models participating in the IGAC SPARC Chemistry–Climate Model Initiative (CCMI). Specifically, we find up to 40 % differences in the transport timescales connecting the Northern Hemisphere (NH) midlatitude surface to the Arctic and to Southern Hemisphere high latitudes, where the mean age ranges between 1.7 and 2.6 years. We show that these differences are related to large differences in vertical transport among the simulations, in particular to differences in parameterized convection over the oceans. While stronger convection over NH midlatitudes is associated with slower transport to the Arctic, stronger convection in the tropics and subtropics is associated with faster interhemispheric transport. We also show that the differences among simulations constrained with fields derived from the same reanalysis products are as large as (and in some cases larger than) the differences among free-running simulations, most likely due to larger differences in parameterized convection. Our results indicate that care must be taken when using simulations constrained with analyzed winds to interpret the influence of meteorology on tropospheric composition.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-18-7217-2018
    DOI: 10.5194/acp-18-7217-2018-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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