scholarly journals Linkages between ozone-depleting substances, tropospheric oxidation and aerosols

2013 ◽  
Vol 13 (9) ◽  
pp. 4907-4916 ◽  
Author(s):  
A. Voulgarakis ◽  
D. T. Shindell ◽  
G. Faluvegi
Keyword(s):  
Radiative Forcing ◽  
Scale Effects ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Tropospheric Chemistry ◽  
Atmospheric Composition ◽  
N2o Emissions ◽  
Sulfate Aerosols ◽  
Comparable Amount ◽  
Ozone Depleting Substances

Abstract. Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric ozone depleting substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The individual historical radiative forcings of CFCs and N2O through their indirect effects on methane (−22.6 mW m−2 for CFCs and −6.7 mW m−2 for N2O) and sulfate aerosols (−3.0 mW m−2 for CFCs and +6.5 mW m−2 for N2O when considering the direct aerosol effect) discussed here are non-negligible when compared to known historical ODS forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.

scholarly journals Linkages between ozone depleting substances, tropospheric oxidation and aerosols

2012 ◽  
Vol 12 (9) ◽  
pp. 25551-25572 ◽  
Author(s):  
A. Voulgarakis ◽  
D. T. Shindell ◽  
G. Faluvegi
Keyword(s):  
Radiative Forcing ◽  
Scale Effects ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Tropospheric Chemistry ◽  
Atmospheric Composition ◽  
N2o Emissions ◽  
Sulfate Aerosols ◽  
Comparable Amount ◽  
Ozone Depleting Substances

Abstract. Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric Ozone Depleting Substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The historical radiative forcing of CFCs through their indirect effects on methane (−22.6 mW m−2) and sulfate aerosols (−3.0 mW m−2) discussed here is non-negligible when compared to known historical CFC forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.

scholarly journals Options to accelerate ozone recovery: ozone and climate benefits

2010 ◽  
Vol 10 (16) ◽  
pp. 7697-7707 ◽  
Author(s):  
J. S. Daniel ◽  
E. L. Fleming ◽  
R. W. Portmann ◽  
G. J. M. Velders ◽  
C. H. Jackman ◽  
...  
Keyword(s):  
Ozone Depletion ◽  
Radiative Forcing ◽  
Montreal Protocol ◽  
N2o Emissions ◽  
Total Column Ozone ◽  
Potential Impact ◽  
Ozone Depleting Substances ◽  
Column Ozone ◽  
The Impact ◽  
Total Column

Abstract. Hypothetical reductions in future emissions of ozone-depleting substances (ODSs) and N2O are evaluated in terms of effects on equivalent effective stratospheric chlorine (EESC), globally-averaged total column ozone, and radiative forcing through 2100. Due to the established success of the Montreal Protocol, these actions can have only a fraction of the impact on ozone depletion that regulations already in force have had. If all anthropogenic ODS and N2O emissions were halted beginning in 2011, ozone is calculated to be higher by about 1–2% during the period 2030–2100 compared to a case of no additional restrictions. Direct radiative forcing by 2100 would be about 0.23 W/m2 lower from the elimination of anthropogenic N2O emissions and about 0.005 W/m2 lower from the destruction of the chlorofluorocarbon (CFC) bank. Due to the potential impact of N2O on future ozone levels, we provide an approach to incorporate it into the EESC formulation, which is used extensively in ozone depletion analyses. The ability of EESC to describe total ozone changes arising from additional ODS and N2O controls is also quantified.

scholarly journals Key drivers of ozone change and its radiative forcing over the 21st century

2017 ◽  
Author(s):  
Fernando Iglesias-Suarez ◽  
Douglas E. Kinnison ◽  
Alexandru Rap ◽  
Oliver Wild ◽  
Paul J. Young
Keyword(s):  
Climate Change ◽  
21St Century ◽  
Radiative Forcing ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Atmospheric Composition ◽  
Radiative Balance ◽  
Uncertainty Range ◽  
Ozone Depleting Substances ◽  
Year 2000

Abstract. Over the 21st century changes in both tropospheric and stratospheric ozone are likely to have important consequences for the Earth's radiative balance. In this study we investigated the radiative effects of future ozone changes, using the Community Earth System Model (CESM1), with the Whole Atmosphere Community Climate Model (WACCM), and including fully coupled radiation and chemistry schemes. Using year 2100 conditions from the Representative Concentration Pathways 8.5 (RCP8.5) scenario, we quantified the individual contributions to ozone radiative forcing of (1) climate change (with and without lightning feedback), (2) reduced concentrations of ozone depleting substances (ODSs), and (3) methane increases. We calculated future ozone radiative forcing relative to year 2000 of (1) 63 ± 76 m Wm−2, (2) 129 ± 81 m Wm−2, and (3) 225 ± 85 m Wm−2, due to climate change, ODSs and methane respectively. Our best estimate of net ozone forcing in this set of simulations is 420 ± 120 m Wm−2 relative to year 2000, and 750 ± 230 m Wm−2 relative to year 1750, with uncertainty range given by approximately ±30 %. We find that the overall long-term tropospheric ozone forcing from methane chemistry-climate feedbacks related to OH and methane lifetime is small (46 m Wm−2). Ozone forcings associated with climate change and stratospheric ozone recovery are robust with regard to background conditions, even though the ozone response is sensitive to both changes in atmospheric composition and climate. Changes in stratospheric-produced ozone account for ~ 47 % of the overall radiative forcing in this set of simulations, highlighting the key role of the stratosphere in determining future radiative forcing.

scholarly journals Effects of stratospheric ozone recovery on tropospheric chemistry and air quality

2013 ◽  
Vol 13 (8) ◽  
pp. 21427-21453
Author(s):  
H. Zhang ◽  
S. Wu ◽  
Y. Wang
Keyword(s):  
Air Quality ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Surface Ozone ◽  
Montreal Protocol ◽  
Tropospheric Chemistry ◽  
Chemical Transport Model ◽  
Photolysis Rates ◽  
Global Chemical Transport Model ◽  
Ozone Depleting Substances

Abstract. The stratospheric ozone has decreased greatly since 1980 due to ozone depleting substances (ODSs). As a result of the implementation of the Montreal Protocol and its amendments and adjustments, stratospheric ozone is expected to recover towards its pre-1980 level in the coming decades. We examine the implications of stratospheric ozone recovery for the tropospheric chemistry and ozone air quality with a global chemical transport model (GEOS-Chem). Significant decreases in surface ozone photolysis rates due to stratospheric ozone recovery are simulated. Increases in ozone lifetime by up to 7% are calculated in the troposphere. The global average OH decreases by 1.74% and the global burden of tropospheric ozone increases by 0.78%. The perturbations to tropospheirc ozone and surface ozone show large seasonal and spatial variations. General increases in surface ozone are calculated for each season, with increases by up to 5% for some regions.

scholarly journals The Importance of the Montreal Protocol in Protecting Earth’s Hydroclimate

2013 ◽  
Vol 26 (12) ◽  
pp. 4049-4068 ◽  
Author(s):  
Yutian Wu ◽  
Lorenzo M. Polvani ◽  
Richard Seager
Keyword(s):  
Ozone Depletion ◽  
Radiative Forcing ◽  
Hydrological Cycle ◽  
Stratospheric Ozone ◽  
Atmospheric Model ◽  
Ultraviolet B ◽  
Montreal Protocol ◽  
Mixed Layer Ocean ◽  
The World ◽  
Ozone Depleting Substances

Abstract The 1987 Montreal Protocol regulating emissions of chlorofluorocarbons (CFCs) and other ozone-depleting substances (ODSs) was motivated primarily by the harm to human health and ecosystems arising from increased exposure to ultraviolet-B (UV-B) radiation associated with depletion of the ozone layer. It is now known that the Montreal Protocol has helped reduce radiative forcing of the climate system since CFCs are greenhouse gases (GHGs), and that ozone depletion (which is now on the verge of reversing) has been the dominant driver of atmospheric circulation changes in the Southern Hemisphere in the last half century. This paper demonstrates that the Montreal Protocol also significantly protects Earth’s hydroclimate. Using the Community Atmospheric Model, version 3 (CAM3), coupled to a simple mixed layer ocean, it is shown that in the “world avoided” (i.e., with CFC emissions not regulated), the subtropical dry zones would be substantially drier, and the middle- and high-latitude regions considerably wetter in the coming decade (2020–29) than in a world without ozone depletion. Surprisingly, these changes are very similar, in both pattern and magnitude, to those caused by projected increases in GHG concentrations over the same period. It is further shown that, by dynamical and thermodynamical mechanisms, both the stratospheric ozone depletion and increased CFCs contribute to these changes. The results herein imply that, as a consequence of the Montreal Protocol, changes in the hydrological cycle in the coming decade will be only half as strong as what they otherwise would be.

scholarly journals Options to accelerate ozone recovery:ozone and climate benefits

2010 ◽  
Vol 10 (4) ◽  
pp. 10839-10863
Author(s):  
J. S. Daniel ◽  
E. L. Fleming ◽  
R. W. Portmann ◽  
G. J. M. Velders ◽  
C. H. Jackman ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Total Ozone ◽  
Montreal Protocol ◽  
N2o Emissions ◽  
Total Column Ozone ◽  
Ozone Depleting Substances ◽  
Column Ozone ◽  
The Impact ◽  
Total Column ◽  
Future Emissions

Abstract. Hypothetical reductions in future emissions of ozone-depleting substances (ODSs), including N2O, are evaluated in terms of effects on equivalent effective stratospheric chlorine (EESC), globally-averaged total column ozone, and radiative forcing through 2100. Due to the established success of the Montreal Protocol, these actions can have only a fraction of the impact that regulations already in force have had. If all anthropogenic ODS emissions were halted beginning in 2011, ozone is calculated to be higher by about 1–2{%} during the period 2030–2100 compared to a case of no additional ODS restrictions. Radiative forcing by 2100 would be about 0.23 W/m2 lower due to the elimination of N2O emissions and about 0.005 W/m2 lower due to destruction of the chlorofluorocarbon (CFC) bank. The ability of EESC to be a suitable metric for total ozone is also quantified. Responding to the recent suggestion that N2O should be considered an ODS, we provide an approach to incorporate N2O into the EESC formulation.

scholarly journals Chemical and climatic drivers of radiative forcing due to changes in stratospheric and tropospheric ozone over the 21<sup>st</sup> century

2017 ◽  
Author(s):  
Antara Banerjee ◽  
Amanda C. Maycock ◽  
John A. Pyle
Keyword(s):  
Greenhouse Gas ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Radiative Forcings ◽  
Climatic Drivers ◽  
Ozone Precursor ◽  
Ozone Depleting Substances ◽  
Projected Changes

Abstract. The ozone radiative forcings (RFs) resulting from projected changes in climate, ozone-depleting substances (ODSs), non-methane ozone precursor emissions and methane between the years 2000 and 2100 are calculated using simulations from the UM-UKCA chemistry-climate model. Projected measures to improve air-quality through reductions in tropospheric ozone precursor emissions present a co-benefit for climate, with a net global mean ozone RF of −0.09 Wm−2. This is opposed by a positive ozone RF of 0.07 Wm−2 due to future decreases in ODSs, which is mainly driven by an increase in tropospheric ozone through stratosphere-to-troposphere exchange. An increase in methane abundance by more than a factor of two (as projected by the RCP8.5 scenario) is found to drive an ozone RF of 0.19 Wm−2, which would greatly outweigh the climate benefits of tropospheric non-methane ozone precursor reductions. A third of the ozone RF due to the projected increase in methane results from increases in stratospheric ozone. The sign of the ozone RF due to future changes in climate (including the radiative effects of greenhouse gas concentrations, sea surface temperatures and sea ice changes) is shown to be dependent on the greenhouse gas emissions pathway, with a positive RF (0.06 Wm−2) for RCP4.5 and a negative RF (−0.07 Wm−2) for the RCP8.5 scenario. This dependence arises from differences in the contribution to RF from stratospheric ozone changes.

scholarly journals Key drivers of ozone change and its radiative forcing over the 21st century

2018 ◽  
Vol 18 (9) ◽  
pp. 6121-6139 ◽  
Author(s):  
Fernando Iglesias-Suarez ◽  
Douglas E. Kinnison ◽  
Alexandru Rap ◽  
Amanda C. Maycock ◽  
Oliver Wild ◽  
...  
Keyword(s):  
Climate Change ◽  
21St Century ◽  
Radiative Forcing ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Atmospheric Composition ◽  
Climate Conditions ◽  
Radiative Balance ◽  
Radiative Forcings ◽  
Year 2000

Abstract. Over the 21st century changes in both tropospheric and stratospheric ozone are likely to have important consequences for the Earth's radiative balance. In this study, we investigate the radiative forcing from future ozone changes using the Community Earth System Model (CESM1), with the Whole Atmosphere Community Climate Model (WACCM), and including fully coupled radiation and chemistry schemes. Using year 2100 conditions from the Representative Concentration Pathway 8.5 (RCP8.5) scenario, we quantify the individual contributions to ozone radiative forcing of (1) climate change, (2) reduced concentrations of ozone depleting substances (ODSs), and (3) methane increases. We calculate future ozone radiative forcings and their standard error (SE; associated with inter-annual variability of ozone) relative to year 2000 of (1) 33 ± 104 m Wm−2, (2) 163 ± 109 m Wm−2, and (3) 238 ± 113 m Wm−2 due to climate change, ODSs, and methane, respectively. Our best estimate of net ozone forcing in this set of simulations is 430 ± 130 m Wm−2 relative to year 2000 and 760 ± 230 m Wm−2 relative to year 1750, with the 95 % confidence interval given by ±30 %. We find that the overall long-term tropospheric ozone forcing from methane chemistry–climate feedbacks related to OH and methane lifetime is relatively small (46 m Wm−2). Ozone radiative forcing associated with climate change and stratospheric ozone recovery are robust with regard to background climate conditions, even though the ozone response is sensitive to both changes in atmospheric composition and climate. Changes in stratospheric-produced ozone account for ∼ 50 % of the overall radiative forcing for the 2000–2100 period in this set of simulations, highlighting the key role of the stratosphere in determining future ozone radiative forcing.

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

2021 ◽  
Author(s):  
Ewa Bednarz ◽  
Ryan Hossaini ◽  
Luke Abraham ◽  
Peter Braesicke ◽  
Martyn Chipperfield
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Lower Boundary ◽  
Montreal Protocol ◽  
Recent Past ◽  
Substantial Impact ◽  
Ozone Depleting Substances ◽  
The Impact

&lt;p&gt;The emissions of most long-lived halogenated ozone-depleting substances (ODSs) are now decreasing, owing to controls on their production introduced by Montreal Protocol and its amendments. However, short-lived halogenated compounds can also have substantial impact on atmospheric chemistry, including stratospheric ozone, particularly if emitted near climatological uplift regions. It has recently become evident that emissions of some chlorinated very short-lived species (VSLSs), such as chloroform (CHCl&lt;sub&gt;3&lt;/sub&gt;) and dichloromethane (CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;), could be larger than previously believed and increasing, particularly in Asia. While these may exert a significant influence on atmospheric chemistry and climate, their impacts remain poorly characterised.&amp;#160;&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;We address this issue using the UM-UKCA chemistry-climate model (CCM). While not only the first, to our knowledge, model study addressing this problem using a CCM, it is also the first such study employing a whole atmosphere model, thereby simulating the tropospheric Cl-VSLSs emissions and the resulting stratospheric impacts in a fully consistent manner. We use a newly developed Double-Extended Stratospheric-Tropospheric (DEST) chemistry scheme, which includes emissions of all major chlorinated and brominated VSLSs alongside an extended treatment of long-lived ODSs.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;We examine the impacts of rising Cl-VSLSs emissions on atmospheric chlorine tracers and ozone, including their long-term trends. We pay particular attention to the role of &amp;#8216;nudging&amp;#8217;, as opposed to the free-running model set up, for the simulated Cl-VSLSs impacts, thereby demostrating the role of atmospheric dynamics in modulating the atmospheric responses to Cl-VSLSs. In addition, we employ novel estimates of Cl-VSLS emissions over the recent past and compare the results with the simulations that prescribe Cl-VSLSs using simple lower boundary conditions. This allows us to demonstrate the impact such choice has on the dominant location and seasonality of the Cl-VSLSs transport into the stratosphere.&lt;/p&gt;

scholarly journals Attribution of N<sub>2</sub>O sources in a grassland soil with laser spectroscopy based isotopocule analysis

2019 ◽  
Vol 16 (16) ◽  
pp. 3247-3266 ◽  
Author(s):  
Erkan Ibraim ◽  
Benjamin Wolf ◽  
Eliza Harris ◽  
Rainer Gasche ◽  
Jing Wei ◽  
...  
Keyword(s):  
Isotopic Composition ◽  
Radiative Forcing ◽  
Dispersion Model ◽  
Stratospheric Ozone ◽  
Particle Dispersion ◽  
N2o Emissions ◽  
Specific Information ◽  
N2o Reduction ◽  
Night Time ◽  
Nitrifier Denitrification

Abstract. Nitrous oxide (N2O) is the primary atmospheric constituent involved in stratospheric ozone depletion and contributes strongly to changes in the climate system through a positive radiative forcing mechanism. The atmospheric abundance of N2O has increased from 270 ppb (parts per billion, 10−9 mole mole−1) during the pre-industrial era to approx. 330 ppb in 2018. Even though it is well known that microbial processes in agricultural and natural soils are the major N2O source, the contribution of specific soil processes is still uncertain. The relative abundance of N2O isotopocules (14N14N16N, 14N15N16O, 15N14N16O, and 14N14N18O) carries process-specific information and thus can be used to trace production and consumption pathways. While isotope ratio mass spectroscopy (IRMS) was traditionally used for high-precision measurement of the isotopic composition of N2O, quantum cascade laser absorption spectroscopy (QCLAS) has been put forward as a complementary technique with the potential for on-site analysis. In recent years, pre-concentration combined with QCLAS has been presented as a technique to resolve subtle changes in ambient N2O isotopic composition. From the end of May until the beginning of August 2016, we investigated N2O emissions from an intensively managed grassland at the study site Fendt in southern Germany. In total, 612 measurements of ambient N2O were taken by combining pre-concentration with QCLAS analyses, yielding δ15Nα, δ15Nβ, δ18O, and N2O concentration with a temporal resolution of approximately 1 h and precisions of 0.46 ‰, 0.36 ‰, 0.59 ‰, and 1.24 ppb, respectively. Soil δ15N-NO3- values and concentrations of NO3- and NH4+ were measured to further constrain possible N2O-emitting source processes. Furthermore, the concentration footprint area of measured N2O was determined with a Lagrangian particle dispersion model (FLEXPART-COSMO) using local wind and turbulence observations. These simulations indicated that night-time concentration observations were largely sensitive to local fluxes. While bacterial denitrification and nitrifier denitrification were identified as the primary N2O-emitting processes, N2O reduction to N2 largely dictated the isotopic composition of measured N2O. Fungal denitrification and nitrification-derived N2O accounted for 34 %–42 % of total N2O emissions and had a clear effect on the measured isotopic source signatures. This study presents the suitability of on-site N2O isotopocule analysis for disentangling source and sink processes in situ and found that at the Fendt site bacterial denitrification or nitrifier denitrification is the major source for N2O, while N2O reduction acted as a major sink for soil-produced N2O.

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