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  • 1
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    Tropospheric ozone in CMIP6 simulations
    Copernicus GmbH ; 2021
    In:  Atmospheric Chemistry and Physics Vol. 21, No. 5 ( 2021-03-18), p. 4187-4218
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 5 ( 2021-03-18), p. 4187-4218
    Abstract: Abstract. The evolution of tropospheric ozone from 1850 to 2100 has been studied using data from Phase 6 of the Coupled Model Intercomparison Project (CMIP6). We evaluate long-term changes using coupled atmosphere–ocean chemistry–climate models, focusing on the CMIP Historical and ScenarioMIP ssp370 experiments, for which detailed tropospheric-ozone diagnostics were archived. The model ensemble has been evaluated against a suite of surface, sonde and satellite observations of the past several decades and found to reproduce well the salient spatial, seasonal and decadal variability and trends. The multi-model mean tropospheric-ozone burden increases from 247 ± 36 Tg in 1850 to a mean value of 356 ± 31 Tg for the period 2005–2014, an increase of 44 %. Modelled present-day values agree well with previous determinations (ACCENT: 336 ± 27 Tg; Atmospheric Chemistry and Climate Model Intercomparison Project, ACCMIP: 337 ± 23 Tg; Tropospheric Ozone Assessment Report, TOAR: 340 ± 34 Tg). In the ssp370 experiments, the ozone burden increases to 416 ± 35 Tg by 2100. The ozone budget has been examined over the same period using lumped ozone production (PO3) and loss (LO3) diagnostics. Both ozone production and chemical loss terms increase steadily over the period 1850 to 2100, with net chemical production (PO3-LO3) reaching a maximum around the year 2000. The residual term, which contains contributions from stratosphere–troposphere transport reaches a minimum around the same time before recovering in the 21st century, while dry deposition increases steadily over the period 1850–2100. Differences between the model residual terms are explained in terms of variation in tropopause height and stratospheric ozone burden.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-21-4187-2021
    DOI: 10.5194/acp-21-4187-2021-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 2
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    Description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in UKESM1
    Copernicus GmbH ; 2020
    In:  Geoscientific Model Development Vol. 13, No. 3 ( 2020-03-17), p. 1223-1266
    Details
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 13, No. 3 ( 2020-03-17), p. 1223-1266
    Abstract: Abstract. Here we present a description of the UKCA StratTrop chemical mechanism, which is used in the UKESM1 Earth system model for CMIP6. The StratTrop chemical mechanism is a merger of previously well-evaluated tropospheric and stratospheric mechanisms, and we provide results from a series of bespoke integrations to assess the overall performance of the model. We find that the StratTrop scheme performs well when compared to a wide array of observations. The analysis we present here focuses on key components of atmospheric composition, namely the performance of the model to simulate ozone in the stratosphere and troposphere and constituents that are important for ozone in these regions. We find that the results obtained for tropospheric ozone and its budget terms from the use of the StratTrop mechanism are sensitive to the host model; simulations with the same chemical mechanism run in an earlier version of the MetUM host model show a range of sensitivity to emissions that the current model does not fall within. Whilst the general model performance is suitable for use in the UKESM1 CMIP6 integrations, we note some shortcomings in the scheme that future targeted studies will address.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    URL: Article
    URL: Article
    DOI: 10.5194/gmd-13-1223-2020
    DOI: 10.5194/gmd-13-1223-2020-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2456725-5
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  • 3
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    Simulating the climate response to atmospheric oxygen variability in the Phanerozoic: a focus on the Holocene, Cretaceous and Permian
    Copernicus GmbH ; 2019
    In:  Climate of the Past Vol. 15, No. 4 ( 2019-08-05), p. 1463-1483
    Details
    In: Climate of the Past, Copernicus GmbH, Vol. 15, No. 4 ( 2019-08-05), p. 1463-1483
    Abstract: Abstract. The amount of dioxygen (O2) in the atmosphere may have varied from as little as 5 % to as much as 35 % during the Phanerozoic eon (54 Ma–present). These changes in the amount of O2 are large enough to have led to changes in atmospheric mass, which may alter the radiative budget of the atmosphere, leading to this mechanism being invoked to explain discrepancies between climate model simulations and proxy reconstructions of past climates. Here, we present the first fully 3-D numerical model simulations to investigate the climate impacts of changes in O2 under different climate states using the coupled atmosphere–ocean Hadley Centre Global Environmental Model version 3 (HadGEM3-AO) and Hadley Centre Coupled Model version 3 (HadCM3-BL) models. We show that simulations with an increase in O2 content result in increased global-mean surface air temperature under conditions of a pre-industrial Holocene climate state, in agreement with idealised 1-D and 2-D modelling studies. We demonstrate the mechanism behind the warming is complex and involves a trade-off between a number of factors. Increasing atmospheric O2 leads to a reduction in incident shortwave radiation at the Earth's surface due to Rayleigh scattering, a cooling effect. However, there is a competing warming effect due to an increase in the pressure broadening of greenhouse gas absorption lines and dynamical feedbacks, which alter the meridional heat transport of the ocean, warming polar regions and cooling tropical regions. Case studies from past climates are investigated using HadCM3-BL and show that, in the warmest climate states in the Maastrichtian (72.1–66.0 Ma), increasing oxygen may lead to a temperature decrease, as the equilibrium climate sensitivity is lower. For the Asselian (298.9–295.0 Ma), increasing oxygen content leads to a warmer global-mean surface temperature and reduced carbon storage on land, suggesting that high oxygen content may have been a contributing factor in preventing a “Snowball Earth” during this period of the early Permian. These climate model simulations reconcile the surface temperature response to oxygen content changes across the hierarchy of model complexity and highlight the broad range of Earth system feedbacks that need to be accounted for when considering the climate response to changes in atmospheric oxygen content.
    Type of Medium: Online Resource
    ISSN: 1814-9332
    URL: Article
    URL: Article
    DOI: 10.5194/cp-15-1463-2019
    DOI: 10.5194/cp-15-1463-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2217985-9
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  • 4
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    Modelling the potential impacts of the recent, unexpected increase in CFC-11 emissions on total column ozone recovery
    Copernicus GmbH ; 2020
    In:  Atmospheric Chemistry and Physics Vol. 20, No. 12 ( 2020-06-19), p. 7153-7166
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 12 ( 2020-06-19), p. 7153-7166
    Abstract: Abstract. The temporal evolution of the abundance of long-lived, anthropogenic chlorofluorocarbons in the atmosphere is a major factor in determining the timing of total column ozone (TCO) recovery. Recent observations have shown that the atmospheric mixing ratio of CFC-11 is not declining as rapidly as expected under full compliance with the Montreal Protocol and indicate a new source of CFC-11 emissions. In this study, the impact of a number of potential future CFC-11 emissions scenarios on the timing of the TCO return to the 1960–1980 mean (an important milestone on the road to recovery) is investigated using the Met Office's Unified Model (Hewitt et al., 2011) coupled with the United Kingdom Chemistry and Aerosol scheme (UM-UKCA). Key uncertainties related to this new CFC-11 source and their impact on the timing of the TCO return date are explored, including the duration of new CFC-11 production and emissions; the impact of any newly created CFC-11 bank; and the effects of co-production of CFC-12. Scenario-independent relationships are identified between cumulative CFC emissions and the timing of the TCO return date, which can be used to establish the impact of future CFC emissions pathways on ozone recovery in the real world. It is found that, for every 200 Gg Cl (∼258 Gg CFC-11) emitted, the timing of the global TCO return to 1960–1980 averaged values is delayed by ∼0.56 years. However, a marked hemispheric asymmetry in the latitudinal impacts of cumulative Cl emissions on the timing of the TCO return date is identified, with longer delays in the Southern Hemisphere than the Northern Hemisphere for the same emission. Together, these results indicate that, if rapid action is taken to curb recently identified CFC-11 production, then no significant delay in the timing of the TCO return to the 1960–1980 mean is expected, highlighting the importance of ongoing, long-term measurement efforts to inform the accountability phase of the Montreal Protocol. However, if the emissions are allowed to continue into the future and are associated with the creation of large banks, then significant delays in the timing of the TCO return date may occur.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-20-7153-2020
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 5
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    Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol
    Copernicus GmbH ; 2017
    In:  Atmospheric Chemistry and Physics Vol. 17, No. 3 ( 2017-02-13), p. 2103-2162
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 3 ( 2017-02-13), p. 2103-2162
    Abstract: Abstract. Oxidation of biogenic volatile organic compounds (BVOC) by the nitrate radical (NO3) represents one of the important interactions between anthropogenic emissions related to combustion and natural emissions from the biosphere. This interaction has been recognized for more than 3 decades, during which time a large body of research has emerged from laboratory, field, and modeling studies. NO3-BVOC reactions influence air quality, climate and visibility through regional and global budgets for reactive nitrogen (particularly organic nitrates), ozone, and organic aerosol. Despite its long history of research and the significance of this topic in atmospheric chemistry, a number of important uncertainties remain. These include an incomplete understanding of the rates, mechanisms, and organic aerosol yields for NO3-BVOC reactions, lack of constraints on the role of heterogeneous oxidative processes associated with the NO3 radical, the difficulty of characterizing the spatial distributions of BVOC and NO3 within the poorly mixed nocturnal atmosphere, and the challenge of constructing appropriate boundary layer schemes and non-photochemical mechanisms for use in state-of-the-art chemical transport and chemistry–climate models. This review is the result of a workshop of the same title held at the Georgia Institute of Technology in June 2015. The first half of the review summarizes the current literature on NO3-BVOC chemistry, with a particular focus on recent advances in instrumentation and models, and in organic nitrate and secondary organic aerosol (SOA) formation chemistry. Building on this current understanding, the second half of the review outlines impacts of NO3-BVOC chemistry on air quality and climate, and suggests critical research needs to better constrain this interaction to improve the predictive capabilities of atmospheric models.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-17-2103-2017
    DOI: 10.5194/acp-17-2103-2017-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 6
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    Improving NO x emission estimates in Beijing using network observations and a perturbed emissions ensemble
    Copernicus GmbH ; 2022
    In:  Atmospheric Chemistry and Physics Vol. 22, No. 13 ( 2022-07-05), p. 8617-8637
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 13 ( 2022-07-05), p. 8617-8637
    Abstract: Abstract. Emissions inventories are crucial inputs to air quality simulations and represent a major source of uncertainty. Various methods have been adopted to optimise emissions inventories, yet in most cases the methods were only applied to total anthropogenic emissions. We have developed a new approach that updates a priori emission estimates by source sector, which are particularly relevant for policy interventions. At its core is a perturbed emissions ensemble (PEE), constructed by perturbing parameters in an a priori emissions inventory within their respective uncertainty ranges. This PEE is then input to an air quality model to generate an ensemble of forward simulations. By comparing the simulation outputs with observations from a dense network, the initial uncertainty ranges are constrained, and a posteriori emission estimates are derived. Using this approach, we were able to derive the transport sector NOx emissions for a study area centred around Beijing in 2016 based on a priori emission estimates for 2013. The absolute emissions were found to be 1.5–9 × 104 Mg, corresponding to a 57 %–93 % reduction from the 2013 levels, yet the night-time fraction of the emissions was 67 %–178 % higher. These results provide robust and independent evidence of the trends of traffic emission in the study area between 2013 and 2016 reported by previous studies. We also highlighted the impacts of the chemical mechanisms in the underlying model on the emission estimates derived, which is often neglected in emission optimisation studies. This work paves forward the route for rapid analysis and update of emissions inventories using air quality models and routine in situ observations, underscoring the utility of dense observational networks. It also highlights some gaps in the current distribution of monitoring sites in Beijing which result in an underrepresentation of large point sources of NOx.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-22-8617-2022
    DOI: 10.5194/acp-22-8617-2022-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 7
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    Evaluation of tropospheric ozone and ozone precursors in simulations from the HTAPII and CCMI model intercomparisons – a focus on the Indian subcontinent
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 9 ( 2019-05-16), p. 6437-6458
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 9 ( 2019-05-16), p. 6437-6458
    Abstract: Abstract. Here we present results from an evaluation of model simulations from the International Hemispheric Transport of Air Pollution Phase II (HTAPII) and Chemistry Climate Model Initiative (CCMI) model inter-comparison projects against a comprehensive series of ground-based, aircraft and satellite observations of ozone mixing ratios made at various locations across India. The study focuses on the recent past (observations from 2008 to 2013, models from 2009–2010) as this is most pertinent to understanding the health impacts of ozone. To our understanding this is the most comprehensive evaluation of these models' simulations of ozone across the Indian subcontinent to date. This study highlights some significant successes and challenges that the models face in representing the oxidative chemistry of the region. The multi-model range in area-weighted surface ozone over the Indian subcontinent is 37.26–56.11 ppb, whilst the population-weighted range is 41.38–57.5 ppb. When compared against surface observations from the Modelling Atmospheric Pollution and Networking (MAPAN) network of eight semi-urban monitoring sites spread across India, we find that the models tend to simulate higher ozone than that which is observed. However, observations of NOx and CO tend to be much higher than modelled mixing ratios, suggesting that the underlying emissions used in the models do not characterise these regions accurately and/or that the resolution of the models is not adequate to simulate the photo-chemical environment of these surface observations. Empirical orthogonal function (EOF) analysis is used in order to identify the extent to which the models agree with regards to the spatio-temporal distribution of the tropospheric ozone column, derived using OMI-MLS observations. We show that whilst the models agree with the spatial pattern of the first EOF of observed tropospheric ozone column, most of the models simulate a peak in the first EOF seasonal cycle represented by principle component 1, which is later than the observed peak. This suggests a widespread systematic bias in the timing of emissions or some other unknown seasonal process. In addition to evaluating modelled ozone mixing ratios, we explore modelled emissions of NOx, CO, volatile organic compounds (VOCs) and the ozone response to the emissions. We find a high degree of variation in emissions from non-anthropogenic sources (e.g. lightning NOx and biomass burning CO) between models. Total emissions of NOx and CO over India vary more between different models in the same model intercomparison project (MIP) than the same model used in different MIPs, making it impossible to diagnose whether differences in modelled ozone are due to emissions or model processes. We therefore recommend targeted experiments to pinpoint the exact causes of discrepancies between modelled and observed ozone and ozone precursors for this region. To this end, a higher density of long-term monitoring sites measuring not only ozone but also ozone precursors including speciated VOCs, located in more rural regions of the Indian subcontinent, would enable improvements in assessing the biases in models run at the resolution found in HTAPII and CCMI.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-19-6437-2019
    DOI: 10.5194/acp-19-6437-2019-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 8
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    Review of the global models used within phase 1 of the Chemistry–Climate Model Initiative (CCMI)
    Copernicus GmbH ; 2017
    In:  Geoscientific Model Development Vol. 10, No. 2 ( 2017-02-13), p. 639-671
    Details
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 10, No. 2 ( 2017-02-13), p. 639-671
    Abstract: Abstract. We present an overview of state-of-the-art chemistry–climate and chemistry transport models that are used within phase 1 of the Chemistry–Climate Model Initiative (CCMI-1). The CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, tropospheric composition, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI-1 recommendations for simulations have been followed is necessary to understand model responses to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI-1 simulations with the aim of informing CCMI data users.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    URL: Article
    URL: Article
    DOI: 10.5194/gmd-10-639-2017
    DOI: 10.5194/gmd-10-639-2017-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 9
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    Tropospheric ozone in CCMI models and Gaussian process emulation to understand biases in the SOCOLv3 chemistry–climate model
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 21 ( 2018-11-13), p. 16155-16172
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 21 ( 2018-11-13), p. 16155-16172
    Abstract: Abstract. Previous multi-model intercomparisons have shown that chemistry–climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC–IGAC (Stratosphere–troposphere Processes And their Role in Climate–International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40 %–50 % in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ∼30 % in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU – approximately 33 % larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, “SOCOLv3.1”, which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N2O5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NOx), carbon monoxide, methane and other volatile organic compounds, VOCs) are responsible for more than 90 % of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20 % more NOx than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry–climate models.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-18-16155-2018
    DOI: 10.5194/acp-18-16155-2018-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 10
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    Description and Evaluation of the specified-dynamics experiment in the Chemistry-Climate Model Initiative
    Copernicus GmbH ; 2020
    In:  Atmospheric Chemistry and Physics Vol. 20, No. 6 ( 2020-03-31), p. 3809-3840
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 6 ( 2020-03-31), p. 3809-3840
    Abstract: Abstract. We provide an overview of the REF-C1SD specified-dynamics experiment that was conducted as part of phase 1 of the Chemistry-Climate Model Initiative (CCMI). The REF-C1SD experiment, which consisted of mainly nudged general circulation models (GCMs) constrained with (re)analysis fields, was designed to examine the influence of the large-scale circulation on past trends in atmospheric composition. The REF-C1SD simulations were produced across various model frameworks and are evaluated in terms of how well they represent different measures of the dynamical and transport circulations. In the troposphere there are large (∼40 %) differences in the climatological mean distributions, seasonal cycle amplitude, and trends of the meridional and vertical winds. In the stratosphere there are similarly large (∼50 %) differences in the magnitude, trends and seasonal cycle amplitude of the transformed Eulerian mean circulation and among various chemical and idealized tracers. At the same time, interannual variations in nearly all quantities are very well represented, compared to the underlying reanalyses. We show that the differences in magnitude, trends and seasonal cycle are not related to the use of different reanalysis products; rather, we show they are associated with how the simulations were implemented, by which we refer both to how the large-scale flow was prescribed and to biases in the underlying free-running models. In most cases these differences are shown to be as large or even larger than the differences exhibited by free-running simulations produced using the exact same models, which are also shown to be more dynamically consistent. Overall, our results suggest that care must be taken when using specified-dynamics simulations to examine the influence of large-scale dynamics on composition.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-20-3809-2020
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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