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  • 1
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 127, No. 16 ( 2022-08-27)
    Abstract: New multi‐model results show significant positive effects of ozone precursors on near‐global ozone offsetting the negative effects of ozone‐depleting substances (ODSs) ODS and greenhouse gases dominate stratospheric ozone changes but with large inter‐model differences due to uncertainties in responses to ODS changes Increases in carbon dioxide and nitrous oxide significantly impact stratospheric ozone, but their net effects on total columns are small due to cancellations
    Type of Medium: Online Resource
    ISSN: 2169-897X , 2169-8996
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2022
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    detail.hit.zdb_id: 2016800-7
    detail.hit.zdb_id: 2969341-X
    SSG: 16,13
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  • 2
    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
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 3
    Online Resource
    Online Resource
    Proceedings of the National Academy of Sciences ; 2020
    In:  Proceedings of the National Academy of Sciences Vol. 117, No. 43 ( 2020-10-27), p. 26651-26659
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 117, No. 43 ( 2020-10-27), p. 26651-26659
    Abstract: The 1257 CE eruption of Mount Samalas (Indonesia) is the source of the largest stratospheric injection of volcanic gases in the Common Era. Sulfur dioxide emissions produced sulfate aerosols that cooled Earth’s climate with a range of impacts on society. The coemission of halogenated species has also been speculated to have led to wide-scale ozone depletion. Here we present simulations from HadGEM3-ES, a fully coupled Earth system model, with interactive atmospheric chemistry and a microphysical treatment of sulfate aerosol, used to assess the chemical and climate impacts from the injection of sulfur and halogen species into the stratosphere as a result of the Mt. Samalas eruption. While our model simulations support a surface air temperature response to the eruption of the order of −1°C, performing well against multiple reconstructions of surface temperature from tree-ring records, we find little evidence to support significant injections of halogens into the stratosphere. Including modest fractions of the halogen emissions reported from Mt. Samalas leads to significant impacts on the composition of the atmosphere and on surface temperature. As little as 20% of the halogen inventory from Mt. Samalas reaching the stratosphere would result in catastrophic ozone depletion, extending the surface cooling caused by the eruption. However, based on available proxy records of surface temperature changes, our model results support only very minor fractions (1%) of the halogen inventory reaching the stratosphere and suggest that further constraints are needed to fully resolve the issue.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    RVK:
    RVK:
    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2020
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    detail.hit.zdb_id: 1461794-8
    SSG: 11
    SSG: 12
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  • 4
    Online Resource
    Online Resource
    Springer Science and Business Media LLC ; 2022
    In:  npj Climate and Atmospheric Science Vol. 5, No. 1 ( 2022-03-23)
    In: npj Climate and Atmospheric Science, Springer Science and Business Media LLC, Vol. 5, No. 1 ( 2022-03-23)
    Abstract: Mitigation of greenhouse gas emissions is crucial for achieving the goals of the Paris climate agreement. One key gas is methane, whose representation in most climate models is limited by using prescribed surface concentrations. Here we use a new, methane emissions-driven version of the UK Earth System Model (UKESM1) and simulate a zero anthropogenic methane emissions scenario (ZAME) in order to (i) attribute the role of anthropogenic methane emissions on the Earth system and (ii) bracket the potential for theoretical maximum mitigation. We find profound, rapid and sustained impacts on atmospheric composition and climate, compared to a counterfactual projection (SSP3-7.0, the ’worst case’ scenario for methane). In ZAME, methane declines to below pre-industrial levels within 12 years and global surface ozone decreases to levels seen in the 1970s. By 2050, 690,000 premature deaths per year and 1° of warming can be attributed to anthropogenic methane in SSP3-7.0. This work demonstrates the significant maximum potential of methane emissions reductions, and their air-quality co-benefits, but also reiterates the need for action on carbon dioxide (CO 2 ) emissions. We show that a methane emissions-driven treatment is essential for simulating the full Earth system impacts and feedbacks of methane emissions changes.
    Type of Medium: Online Resource
    ISSN: 2397-3722
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2022
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  • 5
    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
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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    detail.hit.zdb_id: 2069847-1
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  • 6
    Online Resource
    Online Resource
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 10 ( 2018-05-24), p. 7109-7129
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 10 ( 2018-05-24), p. 7109-7129
    Abstract: Abstract. The hydroxyl radical (OH) plays a crucial role in the chemistry of the atmosphere as it initiates the removal of most trace gases. A number of field campaigns have observed the presence of a missing OH sink in a variety of regions across the planet. A comparison of direct measurements of the OH loss frequency, also known as total OH reactivity (kOH), with the sum of individual known OH sinks (obtained via the simultaneous detection of species such as volatile organic compounds and nitrogen oxides) indicates that, in some cases, up to 80 % of kOH is unaccounted for. In this work, the UM-UKCA chemistry-climate model was used to investigate the wider implications of the missing reactivity on the oxidising capacity of the atmosphere. Simulations of the present-day atmosphere were performed and the model was evaluated against an array of field measurements to verify that the known OH sinks were reproduced well, with a resulting good agreement found for most species. Following this, an additional sink was introduced to simulate the missing OH reactivity as an emission of a hypothetical molecule, X, which undergoes rapid reaction with OH. The magnitude and spatial distribution of this sink were underpinned by observations of the missing reactivity. Model runs showed that the missing reactivity accounted for on average 6 % of the total OH loss flux at the surface and up to 50 % in regions where emissions of the additional sink were high. The lifetime of the hydroxyl radical was reduced by 3 % in the boundary layer, whilst tropospheric methane lifetime increased by 2 % when the additional OH sink was included. As no OH recycling was introduced following the initial oxidation of X, these results can be interpreted as an upper limit of the effects of the missing reactivity on the oxidising capacity of the troposphere. The UM-UKCA simulations also allowed us to establish the atmospheric implications of the newly characterised reactions of peroxy radicals (RO2) with OH. Whilst the effects of this chemistry on kOH were minor, the reaction of the simplest peroxy radical, CH3O2, with OH was found to be a major sink for CH3O2 and source of HO2 over remote regions at the surface and in the free troposphere. Inclusion of this reaction in the model increased tropospheric methane lifetime by up to 3 %, depending on its product branching. Simulations based on the latest kinetic and product information showed that this reaction cannot reconcile models with observations of atmospheric methanol, in contrast to recent suggestions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 7
    Online Resource
    Online Resource
    Copernicus GmbH ; 2016
    In:  Atmospheric Chemistry and Physics Vol. 16, No. 5 ( 2016-03-04), p. 2727-2746
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 5 ( 2016-03-04), p. 2727-2746
    Abstract: Abstract. A stratosphere-resolving configuration of the Met Office's Unified Model (UM) with the United Kingdom Chemistry and Aerosols (UKCA) scheme is used to investigate the atmospheric response to changes in (a) greenhouse gases and climate, (b) ozone-depleting substances (ODSs) and (c) non-methane ozone precursor emissions. A suite of time-slice experiments show the separate, as well as pairwise, impacts of these perturbations between the years 2000 and 2100. Sensitivity to uncertainties in future greenhouse gases and aerosols is explored through the use of the Representative Concentration Pathway (RCP) 4.5 and 8.5 scenarios. The results highlight an important role for the stratosphere in determining the annual mean tropospheric ozone response, primarily through stratosphere–troposphere exchange (STE) of ozone. Under both climate change and reductions in ODSs, increases in STE offset decreases in net chemical production and act to increase the tropospheric ozone burden. This opposes the effects of projected decreases in ozone precursors through measures to improve air quality, which act to reduce the ozone burden. The global tropospheric lifetime of ozone (τO3) does not change significantly under climate change at RCP4.5, but it decreases at RCP8.5. This opposes the increases in τO3 simulated under reductions in ODSs and ozone precursor emissions. The additivity of the changes in ozone is examined by comparing the sum of the responses in the single-forcing experiments to those from equivalent combined-forcing experiments. Whilst the ozone responses to most forcing combinations are found to be approximately additive, non-additive changes are found in both the stratosphere and troposphere when a large climate forcing (RCP8.5) is combined with the effects of ODSs.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 16 ( 2020-08-26), p. 9961-9977
    Abstract: Abstract. Calculating a multi-model mean, a commonly used method for ensemble averaging, assumes model independence and equal model skill. Sharing of model components amongst families of models and research centres, conflated by growing ensemble size, means model independence cannot be assumed and is hard to quantify. We present a methodology to produce a weighted-model ensemble projection, accounting for model performance and model independence. Model weights are calculated by comparing model hindcasts to a selection of metrics chosen for their physical relevance to the process or phenomena of interest. This weighting methodology is applied to the Chemistry–Climate Model Initiative (CCMI) ensemble to investigate Antarctic ozone depletion and subsequent recovery. The weighted mean projects an ozone recovery to 1980 levels, by 2056 with a 95 % confidence interval (2052–2060), 4 years earlier than the most recent study. Perfect-model testing and out-of-sample testing validate the results and show a greater projective skill than a standard multi-model mean. Interestingly, the construction of a weighted mean also provides insight into model performance and dependence between the models. This weighting methodology is robust to both model and metric choices and therefore has potential applications throughout the climate and chemistry–climate modelling communities.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 9
    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
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 10
    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
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2018
    detail.hit.zdb_id: 2553671-0
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