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Impacts of Stratospheric Sulfate Geoengineering on Tropospheric Ozone

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Impacts of Stratospheric Sulfate Geoengineering on Tropospheric Ozone Atmos. Chem. Phys., 17, 11913–11928, 2017 https://doi.org/10.5194/acp-17-11913-2017 © Author(s) 2017. This work is distributed under the Creative Commons Attribution 3.0 License. Impacts of stratospheric sulfate geoengineering on tropospheric ozone Lili Xia1, Peer J. Nowack2,a, Simone Tilmes3, and Alan Robock1 1Department of Environmental Sciences, Rutgers University, New Brunswick, New Jersey, USA 2Department of Chemistry, Centre for Atmospheric Science, University of Cambridge, Cambridge, UK 3Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, Colorado, USA anow at: Grantham Institute and Department of Physics, Faculty of Natural Sciences, Imperial College London, London, UK Correspondence to: Lili Xia ([email protected]) Received: 8 May 2017 – Discussion started: 19 May 2017 Revised: 22 August 2017 – Accepted: 25 August 2017 – Published: 9 October 2017 Abstract. A range of solar radiation management (SRM) spheric humidity. Under insolation reduction, this is the dom- techniques has been proposed to counter anthropogenic cli- inant factor giving rise to the global surface ozone increase. mate change. Here, we examine the potential effects of Regionally, both surface ozone increases and decreases are stratospheric sulfate aerosols and solar insolation reduction found for both scenarios; that is, SRM would affect regions on tropospheric ozone and ozone at Earth’s surface. Ozone of the world differently in terms of air pollution. In conclu- is a key air pollutant, which can produce respiratory diseases sion, surface ozone and tropospheric chemistry would likely and crop damage. Using a version of the Community Earth be affected by SRM, but the overall effect is strongly de- System Model from the National Center for Atmospheric Re- pendent on the SRM scheme. Due to the health and eco- search that includes comprehensive tropospheric and strato- nomic impacts of surface ozone, all these impacts should be spheric chemistry, we model both stratospheric sulfur injec- taken into account in evaluations of possible consequences tion and solar irradiance reduction schemes, with the aim of SRM. of achieving equal levels of surface cooling relative to the Representative Concentration Pathway 6.0 scenario. This al- lows us to compare the impacts of sulfate aerosols and so- 1 Introduction lar dimming on atmospheric ozone concentrations. Despite nearly identical global mean surface temperatures for the 1.1 Atmospheric ozone two SRM approaches, solar insolation reduction increases global average surface ozone concentrations, while sulfate It is well known that sulfate aerosols in the stratosphere injection decreases it. A fundamental difference between the enhance heterogeneous chemical reactions that lead to two geoengineering schemes is the importance of hetero- enhanced ozone depletion after larger volcanic eruptions geneous reactions in the photochemical ozone balance with (Solomon, 1999). With present-day anthropogenic halogen larger stratospheric sulfate abundance, resulting in increased loading, the aerosols provide additional surface area for het- ozone depletion in mid- and high latitudes. This reduces the erogeneous reactions that activate halogens and hence in- net transport of stratospheric ozone into the troposphere and crease catalytic ozone destruction, especially in high lati- thus is a key driver of the overall decrease in surface ozone. tudes (Tie and Brasseur, 1995). This has been modeled and At the same time, the change in stratospheric ozone alters the observed following the large 1982 El Chichón and 1991 tropospheric photochemical environment due to enhanced ul- Pinatubo volcanic eruptions (Tie and Brasseur, 1995; Port- traviolet radiation. A shared factor among both SRM scenar- man et al., 1996). ios is decreased chemical ozone loss due to reduced tropo- However, volcanic eruptions do not only affect strato- spheric ozone but also impact tropospheric composition, of- Published by Copernicus Publications on behalf of the European Geosciences Union. 11914 L. Xia et al.: Impacts of stratospheric sulfate geoengineering on tropospheric ozone ten due to stratosphere–troposphere coupled effects. The reduction, the stratosphere would be cooler due to reduced 1991 Pinatubo eruption, for example, has been linked to shortwave heating (Govindasamy and Caldeira, 2000), al- changes in the stratosphere–troposphere exchange (STE) of though simultaneous stratospheric ozone changes (if consid- ozone (Aquila et al., 2012, 2013; Pitari et al., 2016). In addi- ered) may buffer this effect (Nowack et al., 2016). tion, the stratospheric ozone decrease led to an invigorated One of the most important differences between the two photochemical environment in the troposphere due to en- scenarios is that if a permanently enhanced stratospheric hanced downward chemically active ultraviolet (UV) radi- aerosol layer is artificially created in an attempt to reduce ation (Tang et al., 2013). anthropogenic global warming, the resulting strong ozone This study focuses on tropospheric ozone, in particular depletion, in particular in mid- and high latitudes, would surface ozone concentration changes. Surface ozone is of have serious impacts on the biosphere, similar to the ef- central importance to Earth’s environment, and as an air fects observed after large volcanic eruptions described above pollutant it adversely impacts human health (e.g., Kampa (Crutzen, 2006; Rasch et al., 2008a, b; Tilmes et al., 2008, and Castanas, 2008) and the ecosystem (e.g., Mauzeral and 2009, 2012). This effect would have to be expected as long as Wang, 2001; Ashmore, 2005; Ainsworth et al., 2012). There there is anthropogenic halogen in the stratosphere. In the re- have been numerous studies of the observed surface ozone mote future, the decreasing burden of anthropogenic halogen trend (e.g., Cooper et al., 2014), identifying ozone sources will eventually result in the recovery of the ozone layer. Un- and sinks (e.g., Wild, 2007), predicting future changes (e.g., der such conditions additional stratospheric aerosols could Young et al., 2013), and understanding the impacts of such actually have the opposite effect by deactivating ozone- changes (e.g., Silva et al., 2013). Global surface ozone con- depleting nitrogen oxides, thus leading to an increase in centrations are estimated to have doubled since the prein- ozone in the stratosphere (Tie and Brasseur, 1995; Pitari et dustrial period (Vingarzan, 2004), mainly due to increased al., 2014). Overall, such changes to the stratosphere would emissions of ozone precursors associated with industrializa- also have important implications for tropospheric composi- tion (e.g., Forster et al., 2007). Differences in future tro- tion. Decreasing stratospheric ozone leads to more UV prop- pospheric ozone concentrations will be strongly dependent agating through, with increasing ozone having the opposite on the emission pathway followed (Stevenson et al., 2006), effect, which would thus alter the photochemical environ- which will determine both in situ tropospheric chemical pro- ment of the troposphere in different ways (Tilmes et al., duction of ozone and transport from the ozone-rich strato- 2012; Nowack et al., 2016). sphere (Collins et al., 2003; Wild et al., 2012; Neu et al., In the following sections, we describe the experimental 2014). set-up of the two geoengineering schemes and discuss some general climate impacts, followed by a detailed discussion of 1.2 Differences between sulfate and solar tropospheric and surface ozone changes. We also show that geoengineering sulfate and solar geoengineering would impact the strato- sphere differently, which implies further key differences in The progression of global warming, slow mitigation efforts, their potential influences on tropospheric composition. In and our relatively limited adaptive capacity force considera- this study, we examine the impacts of stratospheric sulfate tion of solar radiation management (SRM) geoengineering as geoengineering on tropospheric ozone for the first time. one possible strategy to avoid many of the most undesirable consequences of global warming (Crutzen, 2006; Wigley, 2006; Tilmes et al., 2016a). The above discussed factors con- 2 Model and experiment design trolling tropospheric ozone concentrations could be affected by SRM schemes (Nowack et al., 2016). Here we compare We simulated both types of SRM schemes using the full a proposed geoengineering scheme, stratospheric sulfur in- tropospheric and stratospheric chemistry version of the jection, to solar irradiance reduction. Both schemes would Community Earth System Model–Community Atmospheric cool Earth’s surface by reducing sunlight reaching the sur- Model 4 (CESM CAM4-chem) with a horizontal resolution face, either by aerosols reflecting sunlight or by artificially of 0.9◦ × 1.25◦ (lat × long) and 26 levels from the surface to reducing the solar constant in a climate model, but sulfate about 40 km (3.5 mb). The model has been shown to give a geoengineering would strongly heat the stratosphere and pro- good representation of present-day atmospheric composition vide aerosol surfaces for chemical reactions. Previous stud- in the troposphere (Tilmes et al., 2016b) and stratosphere ies have shown that injected sulfur chemically forms sulfate at 2◦ resolution (Fernandez et al., 2017). Similar to the 2◦ aerosols within a couple of weeks. The aerosol layer absorbs model version, the 1◦ horizontal resolution version of the near infrared solar radiation
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