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1. The response of the North Pacific jet and stratosphere-to-troposphere transport of ozone over western North America to RCP8.5 climate forcing

   https://doi.org/10.5194/acp-23-5101-2023  

   Elsbury, Dillon; Butler, Amy H.; Albers, John R.; Breeden, Melissa L.; Langford, Andrew O'Neil (January 2023, Atmospheric Chemistry and Physics)

   Abstract. Stratosphere-to-troposphere transport (STT) is an important sourceof ozone for the troposphere, particularly over western North America. STTin this region is predominantly controlled by a combination of thevariability and location of the Pacific jet stream and the amount of ozonein the lower stratosphere, two factors which are likely to change ifgreenhouse gas concentrations continue to increase. Here we use WholeAtmosphere Community Climate Model experiments with a tracer ofstratospheric ozone (O3S) to study how end-of-the-century RepresentativeConcentration Pathway (RCP) 8.5 sea surface temperatures (SSTs) andgreenhouse gases (GHGs), in isolation and in combination, influence STT ofozone over western North America relative to a preindustrial controlbackground state. We find that O3S increases by up to 37 % during late winter at 700 hPaover western North America in response to RCP8.5 forcing, with the increasestapering off somewhat during spring and summer. When this response to RCP8.5greenhouse gas forcing is decomposed into the contributions made by futureSSTs alone versus future GHGs alone, the latter are found to be primarilyresponsible for these O3S changes. Both the future SSTs alone and the futureGHGs alone accelerate the Brewer–Dobson circulation, which modifiesextratropical lower-stratospheric ozone mixing ratios. While the future GHGsalone promote a more zonally symmetric lower-stratospheric ozone change dueto enhanced ozone production and some transport, the future SSTs aloneincrease lower-stratospheric ozone predominantly over the North Pacific viatransport associated with a stationary planetary-scale wave. Ozoneaccumulates in the trough of this anomalous wave and is reduced over thewave's ridges, illustrating that the composition of the lower-stratosphericozone reservoir in the future is dependent on the phase and position of thestationary planetary-scale wave response to future SSTs alone, in additionto the poleward mass transport provided by the accelerated Brewer–Dobsoncirculation. Further, the future SSTs alone account for most changes to thelarge-scale circulation in the troposphere and stratosphere compared to theeffect of future GHGs alone. These changes include modifying the positionand speed of the future North Pacific jet, lifting the tropopause,accelerating both the Brewer–Dobson circulation's shallow and deep branches,and enhancing two-way isentropic mixing in the stratosphere. 

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2. Numerical impacts on tracer transport: Diagnosing the influence of dynamical core formulation and resolution on stratospheric transport

   https://doi.org/10.1175/JAS-D-21-0085.1  

   Gupta, Aman; Gerber, Edwin P.; Plumb, R. Alan; Lauritzen, Peter H. (September 2021, Journal of the Atmospheric Sciences)

   Abstract Accurate representation of stratospheric trace gas transport is important for ozone modeling and climate projection. Intermodel spread can arise from differences in the representation of transport by the diabatic (overturning) circulation vs. comparatively faster adiabatic mixing by breaking waves, or through numerical errors, primarily diffusion. This study investigates the impact of these processes on transport using an idealised tracer, the age-of-air. Transport is assessed in two state-of-the-art dynamical cores based on fundamentally different numerical formulations: finite volume and spectral element. Integrating the models in free-running and nudged tropical wind configurations reveals the crucial impact of tropical dynamics on stratospheric transport. Using age-budget theory, vertical and horizontal gradients of age allow comparison of the roles of the diabatic circulation, adiabatic mixing, and the numerical diffusive flux. Their respective contribution is quantified by connecting the full 3-d model to the tropical leaky pipe framework of Neu and Plumb (1999). Transport by the two cores varies significantly in the free-running integrations, with the age in the middle stratosphere differing by about 2 years primarily due to differences in adiabatic mixing. When winds in the tropics are constrained, the difference in age drops to about 0.5 years; in this configuration, more than half the difference is due to the representation of the diabatic circulation. Numerical diffusion is very sensitive to the resolution of the core, but does not play a significant role in differences between the cores when they are run at comparable resolution. It is concluded that fundamental differences rooted in dynamical core formulation can account for a substantial fraction of transport bias between climate models. 

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3. Global seasonal distribution of CH ₂ Br ₂ and CHBr ₃ in the upper troposphere and lower stratosphere

   https://doi.org/10.5194/acp-22-15049-2022  

   Jesswein, Markus; Fernandez, Rafael P.; Berná, Lucas; Saiz-Lopez, Alfonso; Grooß, Jens-Uwe; Hossaini, Ryan; Apel, Eric C.; Hornbrook, Rebecca S.; Atlas, Elliot L.; Blake, Donald R.; et al (January 2022, Atmospheric Chemistry and Physics)

   Abstract. Bromine released from the decomposition of short-lived brominated source gases contributes as a sink of ozone in the lower stratosphere.The two major contributors are CH2Br2 and CHBr3.In this study, we investigate the global seasonal distribution of these two substances, based on four High Altitude and Long Range Research Aircraft (HALO) missions, the HIAPER Pole-to-Pole Observations (HIPPO) mission, and the Atmospheric Tomography (ATom) mission.Observations of CH2Br2 in the free and upper troposphere indicate a pronounced seasonality in both hemispheres, with slightly larger mixing ratios in the Northern Hemisphere (NH).Compared to CH2Br2, CHBr3 in these regions shows larger variability and less clear seasonality, presenting larger mixing ratios in winter and autumn in NH midlatitudes to high latitudes.The lowermost stratosphere of SH and NH shows a very similar distribution of CH2Br2 in hemispheric spring with differences well below 0.1 ppt, while the differences in hemispheric autumn are much larger with substantially smaller values in the SH than in the NH.This suggests that transport processes may be different in both hemispheric autumn seasons, which implies that the influx of tropospheric air (“flushing”) into the NH lowermost stratosphere is more efficient than in the SH.The observations of CHBr3 support the suggestion, with a steeper vertical gradient in the upper troposphere and lower stratosphere in SH autumn than in NH autumn.However, the SH database is insufficient to quantify this difference.We further compare the observations to model estimates of TOMCAT (Toulouse Off-line Model of Chemistry And Transport) and CAM-Chem (Community Atmosphere Model with Chemistry, version 4), both using the same emission inventory of Ordóñez et al. (2012).The pronounced tropospheric seasonality of CH2Br2 in the SH is not reproduced by the models,presumably due to erroneous seasonal emissions or atmospheric photochemical decomposition efficiencies.In contrast, model simulations of CHBr3 show a pronounced seasonality in both hemispheres, which is not confirmed by observations.The distributions of both species in the lowermost stratosphere of the Northern and Southern hemispheres are overall well captured by the models with the exception of southern hemispheric autumn,where both models present a bias that maximizes in the lowest 40 K above the tropopause, with considerably lower mixing ratios in the observations.Thus, both models reproduce equivalent flushing in both hemispheres, which is not confirmed by the limited available observations.Our study emphasizes the need for more extensive observations in the SH to fully understand the impact of CH2Br2 and CHBr3 on lowermost-stratospheric ozone loss and to help constrain emissions. 

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4. The Spillover of Tropospheric Ozone Increases Has Hidden the Extent of Stratospheric Ozone Depletion by Halogens

   https://doi.org/10.1029/2023AV001154  

   Prather, Michael J (June 2024, AGU Advances)

   Abstract Stratospheric ozone depletion from halocarbons is partly countered by pollution‐driven increases in tropospheric ozone, with transport connecting the two. While recognizing this connection, the ozone assessment's evaluation of observations and processes have often split the chapters at the tropopause boundary. Using a chemistry‐transport model we find that air‐pollution ozone enhancements in the troposphere spill over into the stratosphere at significant rates, that is, 13%–34% of the excess tropospheric burden appears in the lowermost extra‐tropical stratosphere. As we track the anticipated recovery of the observed ozone depletion, we should recognize that two tenths of that recovery may come from the transport of increasing tropospheric ozone into the stratosphere. 

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5. On the atmospheric budget of 1,2-dichloroethane and its impact on stratospheric chlorine and ozone (2002–2020)

   https://doi.org/10.5194/acp-24-13457-2024  

   Hossaini, Ryan; Sherry, David; Wang, Zihao; Chipperfield, Martyn P; Feng, Wuhu; Oram, David E; Adcock, Karina E; Montzka, Stephen A; Simpson, Isobel J; Mazzeo, Andrea; et al (December 2024, Atmospheric Chemistry and Physics)

   Abstract. The chemical compound 1,2-dichloroethane (DCE), or ethylene dichloride, is an industrial very short-lived substance (VSLS) whose major use is as a feedstock in the production chain of polyvinyl chloride (PVC). Like other chlorinated VSLSs, transport of DCE (and/or its atmospheric oxidation products) to the stratosphere could contribute to ozone depletion there. However, despite annual production volumes greatly exceeding those of more prominent VSLSs (e.g. dichloromethane), global DCE observations are sparse; thus, the magnitude and distribution of DCE emissions and trends in its atmospheric abundance are poorly known. In this study, we performed an exploratory analysis of the global DCE budget between 2002 and 2020. Combining bottom-up data on annual production and assumptions around fugitive losses during production and feedstock use, we assessed the DCE source strength required to reproduce atmospheric DCE observations. We show that the TOMCAT/SLIMCAT 3-D chemical transport model (CTM) reproduces DCE measurements from various aircraft missions well, including HIPPO (2009–2011), ATom (2016–2018), and KORUS-AQ (2016), along with surface measurements from Southeast Asia, when assuming a regionally varying production emission factor in the range of 0.5 %–1.5 %. Our findings imply substantial fugitive losses of DCE and/or substantial emissive applications (e.g. solvent use) that are poorly reported. We estimate that DCE's global source increased by ∼ 45 % between 2002 (349 ± 61 Gg yr−1) and 2020 (505 ± 90 Gg yr−1), with its contribution to stratospheric chlorine increasing from 8.2 (± 1.5) to ∼ 12.9 (± 2.4) ppt Cl (where ppt denotes parts per trillion) over this period. DCE's relatively short overall tropospheric lifetime (∼ 83 d) limits, although does not preclude, its transport to the stratosphere, and we show that its impact on ozone is small at present. Annually averaged, DCE is estimated to have decreased ozone in the lower stratosphere by up to several parts per billion (< 1 %) in 2020, although a larger effect in the springtime Southern Hemisphere polar lower stratosphere is apparent (decreases of up to ∼ 1.3 %). Given strong potential for growth in DCE production tied to demand for PVC, ongoing measurements would be of benefit to monitor potential future increases in its atmospheric abundance and its contribution to ozone depletion. 

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