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The Antarctic ozone “hole” was discovered in 1985, and man-made ozone- depleting substances (ODS) are its primary cause. Following reductions of ODSs under the Montreal Protocol, signs of ozone recovery have been reported, based largely on observations and broad yet compelling model-data comparisons. While such approaches are highly valuable, they don't provide rigorous statistical detection of the temporal and spatial structure of Antarctic ozone recovery in the presence of internal climate variability. Here, we apply pattern-based detection and attribution methods as employed in climate change studies to separate anthropogenically forced ozone responses from internal variability, relying on trend pattern information as a function of month and height. The analysis uses satellite observations together with single-model and multi-model ensemble simulations to identify and quantify the month-height Antarctic ozone recovery “fingerprint”. We demonstrate that the data and simulations show remarkable agreement in the fingerprint pattern of the ozone response to decreasing ODSs since 2005. We also show that ODS forcing has enhanced ozone internal variability during the austral spring, influencing detection of forced responses and their time of emergence. Our results provide robust statistical and physical evidence that actions taken under the Montreal Protocol to reduce ODSs are indeed resulting in the beginning of Antarctic ozone recovery, defined as increases in ozone consistent with expected month-height patterns. 

Abstract Volcanic eruptions and wildfires can impact stratospheric chemistry. We apply tracer‐tracer correlations to satellite data from Atmospheric Chemistry Experiment—Fourier Transform Spectrometer and the Halogen Occultation Experiment at 68 hPa to consistently compare the chemical impact on HCl after multiple wildfires and volcanic eruptions of different magnitudes. The 2020 Australian New Year (ANY) fire displayed an order of magnitude less stratospheric aerosol extinction than the 1991 Pinatubo eruption, but showed similar large changes in mid‐latitude lower stratosphere HCl. While the mid‐latitude aerosol loadings from the 2015 Calbuco and 2022 Hunga volcanic eruptions were similar to the ANY fire, little impact on HCl occurred. The 2009 Australian Black Saturday fire and 2021 smoke remaining from 2020 yield small HCl changes, at the edge of the detection method. These observed contrasts across events highlight greater reactivity for smoke versus volcanic aerosols at warm temperatures. 

Abstract Following the Hunga Tonga–Hunga Ha'apai (HTHH) eruption in January 2022, significant reductions in stratospheric hydrochloric acid (HCl) were observed in the Southern Hemisphere mid‐latitudes during the latter half of 2022, suggesting potential chlorine activation. The objective of this study is to comprehensively understand the loss of HCl in the aftermath of HTHH. Satellite measurements and a global chemistry‐climate model are employed for the analysis. We find strong agreement of 2022 anomalies between the modeled and the measured data. The observed tracer‐tracer relations between nitrous oxide (N₂O) and HCl indicate a significant role of chemical processing in the observed HCl reduction, especially during the austral winter of 2022. Further examining the roles of chlorine gas‐phase and heterogeneous chemistry, we find that heterogeneous chemistry emerges as the primary driver for the chemical loss of HCl, and the reaction between hypobromous acid (HOBr) and HCl on sulfate aerosols is the dominant loss process. 

Abstract North Atlantic sea surface temperatures (NASST), particularly in the subpolar region, are among the most predictable in the world's oceans. However, the relative importance of atmospheric and oceanic controls on their variability at multidecadal timescales remain uncertain. Neural networks (NNs) are trained to examine the relative importance of oceanic and atmospheric predictors in predicting the NASST state in the Community Earth System Model 1 (CESM1). In the presence of external forcings, oceanic predictors outperform atmospheric predictors, persistence, and random chance baselines out to 25‐year leadtimes. Layer‐wise relevance propagation is used to unveil the sources of predictability, and reveal that NNs consistently rely upon the Gulf Stream‐North Atlantic Current region for accurate predictions. Additionally, CESM1‐trained NNs successfully predict the phasing of multidecadal variability in an observational data set, suggesting consistency in physical processes driving NASST variability between CESM1 and observations. 

The 2019 to 2020 Australian summer wildfires injected an amount of organic gases and particles into the stratosphere unprecedented in the satellite record since 2002, causing large unexpected changes in HCl and ClONO 2 . These fires provided a novel opportunity to evaluate heterogeneous reactions on organic aerosols in the context of stratospheric chlorine and ozone depletion chemistry. It has long been known that heterogeneous chlorine (Cl) activation occurs on the polar stratospheric clouds (PSCs; liquid and solid particles containing water, sulfuric acid, and in some cases nitric acid) that are found in the stratosphere, but these are only effective for ozone depletion chemistry at temperatures below about 195 K (i.e., largely in the polar regions during winter). Here, we develop an approach to quantitatively assess atmospheric evidence for these reactions using satellite data for both the polar (65 to 90°S) and the midlatitude (40 to 55°S) regions. We show that heterogeneous reactions apparently even happened at temperatures at 220 K during austral autumn on the organic aerosols present in 2020 in both regions, in contrast to earlier years. Further, increased variability in HCl was also found after the wildfires, suggesting diverse chemical properties among the 2020 aerosols. We also confirm the expectation based upon laboratory studies that heterogeneous Cl activation has a strong dependence upon water vapor partial pressure and hence atmospheric altitude, becoming much faster close to the tropopause. Our analysis improves the understanding of heterogeneous reactions that are important for stratospheric ozone chemistry under both background and wildfire conditions. 

Abstract Subgrid processes in global climate models are represented by parameterizations which are a major source of uncertainties in simulations of climate. In recent years, it has been suggested that machine‐learning (ML) parameterizations based on high‐resolution model output data could be superior to traditional parameterizations. Currently, both traditional and ML parameterizations of subgrid processes in the atmosphere are based on a single‐column approach, which only use information from single atmospheric columns. However, single‐column parameterizations might not be ideal since certain atmospheric phenomena, such as organized convective systems, can cross multiple grid boxes and involve slantwise circulations that are not purely vertical. Here we train neural networks (NNs) using non‐local inputs spanning over 3 × 3 columns of inputs. We find that including the non‐local inputs improves the offline prediction of a range of subgrid processes. The improvement is especially notable for subgrid momentum transport and for atmospheric conditions associated with mid‐latitude fronts and convective instability. Using an interpretability method, we find that the NN improvements partly rely on using the horizontal wind divergence, and we further show that including the divergence or vertical velocity as a separate input substantially improves offline performance. However, non‐local winds continue to be useful inputs for parameterizating subgrid momentum transport even when the vertical velocity is included as an input. Overall, our results imply that the use of non‐local variables and the vertical velocity as inputs could improve the performance of ML parameterizations, and the use of these inputs should be tested in online simulations in future work. 

Abstract Hydrochlorofluorocarbons (HCFCs) and hydrofluorocarbons (HFCs) are potent greenhouse gases regulated under the Montreal Protocol and its amendments. Emission estimates generally use constant atmospheric lifetimes accounting for loss via hydroxyl radical (OH) reactions. However, chemistry‐climate models suggest OH increases after 1980, implying underestimated emissions. Further, HCFCs and HFCs are soluble in seawater and could be destroyed through in situ oceanic microbial activity. These ocean sinks are largely overlooked. Using a coupled atmosphere‐ocean model, we show that increases in modeled OH imply underestimated HCFC and HFC emissions by ∼10% near their respective peak emissions. Our model results also suggest that oceanic processes could lead to up to an additional 10% underestimation in these halocarbon emissions in the 2020s. Ensuring global compliance to the Protocol and accurate knowledge of contributions to global warming from these gases therefore requires understanding of these processes. 

The ocean is a reservoir for CFC-11, a major ozone-depleting chemical. Anthropogenic production of CFC-11 dramatically decreased in the 1990s under the Montreal Protocol, which stipulated a global phase out of production by 2010. However, studies raise questions about current overall emission levels and indicate unexpected increases of CFC-11 emissions of about 10 Gg ⋅ yr −1 after 2013 (based upon measured atmospheric concentrations and an assumed atmospheric lifetime). These findings heighten the need to understand processes that could affect the CFC-11 lifetime, including ocean fluxes. We evaluate how ocean uptake and release through 2300 affects CFC-11 lifetimes, emission estimates, and the long-term return of CFC-11 from the ocean reservoir. We show that ocean uptake yields a shorter total lifetime and larger inferred emission of atmospheric CFC-11 from 1930 to 2075 compared to estimates using only atmospheric processes. Ocean flux changes over time result in small but not completely negligible effects on the calculated unexpected emissions change (decreasing it by 0.4 ± 0.3 Gg ⋅ yr −1 ). Moreover, it is expected that the ocean will eventually become a source of CFC-11, increasing its total lifetime thereafter. Ocean outgassing should produce detectable increases in global atmospheric CFC-11 abundances by the mid-2100s, with emission of around 0.5 Gg ⋅ yr −1 ; this should not be confused with illicit production at that time. An illustrative model projection suggests that climate change is expected to make the ocean a weaker reservoir for CFC-11, advancing the detectable change in the global atmospheric mixing ratio by about 5 yr.