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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 23 ( 2016-12-12), p. 15397-15412
    Abstract: Abstract. Deliberate injection of aerosol particles into the stratosphere is a potential climate engineering scheme. Particles injected into the stratosphere would scatter solar radiation back to space, thereby reducing the temperature at the Earth's surface and hence the impacts of global warming. Minerals such as TiO2 or SiO2 are among the potentially suitable aerosol materials for stratospheric particle injection due to their greater light-scattering ability than stratospheric sulfuric acid particles. However, the heterogeneous reactivity of mineral particles towards trace gases important for stratospheric chemistry largely remains unknown, precluding reliable assessment of their impacts on stratospheric ozone, which is of key environmental significance. In this work we have investigated for the first time the heterogeneous hydrolysis of ClONO2 on TiO2 and SiO2 aerosol particles at room temperature and at different relative humidities (RHs), using an aerosol flow tube. The uptake coefficient, γ(ClONO2), on TiO2 was ∼ 1.2 × 10−3 at 7 % RH and remained unchanged at 33 % RH, and increased for SiO2 from ∼ 2 × 10−4 at 7 % RH to  ∼ 5 × 10−4 at 35 % RH, reaching a value of  ∼ 6 × 10−4 at 59 % RH. We have also examined the impacts of a hypothetical TiO2 injection on stratospheric chemistry using the UKCA (United Kingdom Chemistry and Aerosol) chemistry–climate model, in which heterogeneous hydrolysis of N2O5 and ClONO2 on TiO2 particles is considered. A TiO2 injection scenario with a solar-radiation scattering effect very similar to the eruption of Mt Pinatubo was constructed. It is found that, compared to the eruption of Mt Pinatubo, TiO2 injection causes less ClOx activation and less ozone destruction in the lowermost stratosphere, while reduced depletion of N2O5 and NOx in the middle stratosphere results in decreased ozone levels. Overall, no significant difference in the vertically integrated ozone abundances is found between TiO2 injection and the eruption of Mt Pinatubo. Future work required to further assess the impacts of TiO2 injection on stratospheric chemistry is also discussed.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
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  • 2
    In: Journal of Climate, American Meteorological Society, Vol. 28, No. 16 ( 2015-08-15), p. 6516-6535
    Abstract: A warm bias in tropical tropopause temperature is found in the Met Office Unified Model (MetUM), in common with most models from phase 5 of CMIP (CMIP5). Key dynamical, microphysical, and radiative processes influencing the tropical tropopause temperature and lower-stratospheric water vapor concentrations in climate models are investigated using the MetUM. A series of sensitivity experiments are run to separate the effects of vertical advection, ice optical and microphysical properties, convection, cirrus clouds, and atmospheric composition on simulated tropopause temperature and lower-stratospheric water vapor concentrations in the tropics. The numerical accuracy of the vertical advection, determined in the MetUM by the choice of interpolation and conservation schemes used, is found to be particularly important. Microphysical and radiative processes are found to influence stratospheric water vapor both through modifying the tropical tropopause temperature and through modifying upper-tropospheric water vapor concentrations, allowing more water vapor to be advected into the stratosphere. The representation of any of the processes discussed can act to significantly reduce biases in tropical tropopause temperature and stratospheric water vapor in a physical way, thereby improving climate simulations.
    Type of Medium: Online Resource
    ISSN: 0894-8755 , 1520-0442
    RVK:
    Language: English
    Publisher: American Meteorological Society
    Publication Date: 2015
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    detail.hit.zdb_id: 2021723-7
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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
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    SSG: 12
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 22 ( 2017-11-20), p. 13801-13818
    Abstract: Abstract. Chemical and dynamical drivers of trends in tropical total-column ozone (TCO3) for the recent past and future periods are explored using the UM-UKCA (Unified Model HadGEM3-A (Hewitt et al., 2011) coupled with the United Kingdom Chemistry and Aerosol scheme) chemistry–climate model. A transient 1960–2100 simulation is analysed which follows the representative concentration pathway 6.0 (RCP6.0) emissions scenario for the future. Tropical averaged (10° S–10° N) TCO3 values decrease from the 1970s, reach a minimum around 2000 and return to their 1980 values around 2040, consistent with the use and emission of halogenated ozone-depleting substances (ODSs), and their later controls under the Montreal Protocol. However, when the ozone column is subdivided into three partial columns (PCO3) that cover the upper stratosphere (PCO3US), lower stratosphere (PCO3LS) and troposphere (PCO3T), significant differences in the temporal behaviour of the partial columns are seen. Modelled PCO3T values under the RCP6.0 emissions scenario increase from 1960 to 2000 before remaining approximately constant throughout the 21st century. PCO3LS values decrease rapidly from 1960 to 2000 and remain constant from 2000 to 2050, before gradually decreasing further from 2050 to 2100 and never returning to their 1980s values. In contrast, PCO3US values decrease from 1960 to 2000, before increasing rapidly throughout the 21st century and returning to 1980s values by  ∼  2020, and reach significantly higher values by 2100. Using a series of idealised UM-UKCA time-slice simulations with concentrations of well-mixed greenhouse gases (GHGs) and halogenated ODS species set to either year 2000 or 2100 levels, we examine the main processes that drive the PCO3 responses in the three regions and assess how these processes change under different emission scenarios. Finally, we present a simple, linearised model to describe the future evolution of tropical stratospheric column ozone values based on terms representing time-dependent abundances of GHG and halogenated ODS.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 5
    Online Resource
    Online Resource
    Copernicus GmbH ; 2019
    In:  Geoscientific Model Development Vol. 12, No. 3 ( 2019-03-29), p. 1227-1239
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 12, No. 3 ( 2019-03-29), p. 1227-1239
    Abstract: Abstract. Improvements are made to two areas of the United Kingdom Chemistry and Aerosol (UKCA) module, which forms part of the Met Office Unified Model (UM) used for weather and climate applications. Firstly, a solar cycle is added to the photolysis scheme. The effect on total column ozone of this addition was found to be around 1 %–2 % in midlatitude and equatorial regions, in phase with the solar cycle. Secondly, reactions occurring on the surfaces of polar stratospheric clouds and sulfate aerosol are updated and extended by modification of the uptake coefficients of five existing reactions and the addition of a further eight reactions involving bromine species. These modifications are shown to reduce the overabundance of modelled total column ozone in the Arctic during October to February, southern midlatitudes during August and the Antarctic during September. Antarctic springtime ozone depletion is shown to be enhanced by 25 DU on average, which now causes the ozone hole to be somewhat too deep compared to observations. We show that this is in part due to a cold bias of the Antarctic polar vortex in the model.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2456725-5
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  • 6
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 127, No. 20 ( 2022-10-27)
    Abstract: Coupling in ozone chemistry causes an increase in persistence of low temperature anomalies over both poles In the Antarctic, coupling in chemistry amplifies pre‐existing stratospheric cold biases These effects can be masked by other dynamical differences present in some models
    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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  • 7
    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
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    SSG: 16,13
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  • 8
    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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  • 9
    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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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 2 ( 2021-01-29), p. 1211-1243
    Abstract: Abstract. Quantifying forcings from anthropogenic perturbations to the Earth system (ES) is important for understanding changes in climate since the pre-industrial (PI) period. Here, we quantify and analyse a wide range of present-day (PD) anthropogenic effective radiative forcings (ERFs) with the UK's Earth System Model (ESM), UKESM1, following the protocols defined by the Radiative Forcing Model Intercomparison Project (RFMIP) and the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP). In particular, quantifying ERFs that include rapid adjustments within a full ESM enables the role of various chemistry–aerosol–cloud interactions to be investigated. Global mean ERFs for the PD (year 2014) relative to the PI (year 1850) period for carbon dioxide (CO2), nitrous oxide (N2O), ozone-depleting substances (ODSs), and methane (CH4) are 1.89 ± 0.04, 0.25 ± 0.04, −0.18 ± 0.04, and 0.97 ±  0.04 W m−2, respectively. The total greenhouse gas (GHG) ERF is 2.92 ± 0.04 W m−2. UKESM1 has an aerosol ERF of −1.09 ± 0.04 W m−2. A relatively strong negative forcing from aerosol–cloud interactions (ACI) and a small negative instantaneous forcing from aerosol–radiation interactions (ARI) from sulfate and organic carbon (OC) are partially offset by a substantial forcing from black carbon (BC) absorption. Internal mixing and chemical interactions imply that neither the forcing from ARI nor ACI is linear, making the aerosol ERF less than the sum of the individual speciated aerosol ERFs. Ozone (O3) precursor gases consisting of volatile organic compounds (VOCs), carbon monoxide (CO), and nitrogen oxides (NOx), but excluding CH4, exert a positive radiative forcing due to increases in O3. However, they also lead to oxidant changes, which in turn cause an indirect aerosol ERF. The net effect is that the ERF from PD–PI changes in NOx emissions is negligible at 0.03 ± 0.04 W m−2, while the ERF from changes in VOC and CO emissions is 0.33 ± 0.04 W m−2. Together, aerosol and O3 precursors (called near-term climate forcers (NTCFs) in the context of AerChemMIP) exert an ERF of −1.03 ± 0.04 W m−2, mainly due to changes in the cloud radiative effect (CRE). There is also a negative ERF from land use change (−0.17 ± 0.04 W m−2). When adjusted from year 1850 to 1700, it is more negative than the range of previous estimates, and is most likely due to too strong an albedo response. In combination, the net anthropogenic ERF (1.76 ± 0.04 W m−2) is consistent with other estimates. By including interactions between GHGs, stratospheric and tropospheric O3, aerosols, and clouds, this work demonstrates the importance of ES interactions when quantifying ERFs. It also suggests that rapid adjustments need to include chemical as well as physical adjustments to fully account for complex ES interactions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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    detail.hit.zdb_id: 2069847-1
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