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The Montreal Protocol was designed to protect the stratospheric ozone layer by enabling reductions in the abundance of ozone-depleting substances such as chlorofluorocarbons (CFCs) in the atmosphere 1 – 3 . The reduction in the atmospheric concentration of trichlorofluoromethane (CFC-11) has made the second-largest contribution to the decline in the total atmospheric concentration of ozone-depleting chlorine since the 1990s 1 . However, CFC-11 still contributes one-quarter of all chlorine reaching the stratosphere, and a timely recovery of the stratospheric ozone layer depends on a sustained decline in CFC-11 concentrations 1 . Here we show that the rate of decline of atmospheric CFC-11 concentrations observed at remote measurement sites was constant from 2002 to 2012, and then slowed by about 50 per cent after 2012. The observed slowdown in the decline of CFC-11 concentration was concurrent with a 50 per cent increase in the mean concentration difference observed between the Northern and Southern Hemispheres, and also with the emergence of strong correlations at the Mauna Loa Observatory between concentrations of CFC-11 and other chemicals associated with anthropogenic emissions. A simple model analysis of our findings suggests an increase in CFC-11 emissions of 13 ± 5 gigagrams per year (25 ± 13 per cent) since 2012, despite reported production being close to zero 4 since 2006. Our three-dimensional model simulations confirm the increase in CFC-11 emissions, but indicate that this increase may have been as much as 50 per cent smaller as a result of changes in stratospheric processes or dynamics. The increase in emission of CFC-11 appears unrelated to past production; this suggests unreported new production, which is inconsistent with the Montreal Protocol agreement to phase out global CFC production by 2010. Atmospheric CFC-11 concentrations have been declining less rapidly since 2012; evidence suggests that this finding is explained by an increase in the emission of CFC-11during these years.

This overview paper highlights the successes of the Ozone Monitoring Instrument (OMI) on board the Aura satellite spanning a period of nearly 14 years. Data from OMI has been used in a wide range of applications and research resulting in many new findings. Due to its unprecedented spatial resolution, in combination with daily global coverage, OMI plays a unique role in measuring trace gases important for the ozone layer, air quality, and climate change. With the operational very fast delivery (VFD; direct readout) and near real-time (NRT) availability of the data, OMI also plays an important role in the development of operational services in the atmospheric chemistry domain.

As a result of the 1987 Montreal Protocol and its amendments, the atmospheric loading of anthropogenic ozone-depleting substances is decreasing. Accordingly, the stratospheric ozone layer is expected to recover. However, short data records and atmospheric variability confound the search for early signs of recovery, and climate change is masking ozone recovery from ozone-depleting substances in some regions and will increasingly affect the extent of recovery. Here we discuss the nature and timescales of ozone recovery, and explore the extent to which it can be currently detected in different atmospheric regions.

The recovery of the stratospheric ozone layer relies on the continued decline in the atmospheric concentrations of ozone-depleting gases such as chlorofluorocarbons 1 . The atmospheric concentration of trichlorofluoromethane (CFC-11), the second-most abundant chlorofluorocarbon, has declined substantially since the mid-1990s 2 . A recently reported slowdown in the decline of the atmospheric concentration of CFC-11 after 2012, however, suggests that global emissions have increased 3 , 4 . A concurrent increase in CFC-11 emissions from eastern Asia contributes to the global emission increase, but the location and magnitude of this regional source are unknown 3 . Here, using high-frequency atmospheric observations from Gosan, South Korea, and Hateruma, Japan, together with global monitoring data and atmospheric chemical transport model simulations, we investigate regional CFC-11 emissions from eastern Asia. We show that emissions from eastern mainland China are 7.0 ± 3.0 (±1 standard deviation) gigagrams per year higher in 2014–2017 than in 2008–2012, and that the increase in emissions arises primarily around the northeastern provinces of Shandong and Hebei. This increase accounts for a substantial fraction (at least 40 to 60 per cent) of the global rise in CFC-11 emissions. We find no evidence for a significant increase in CFC-11 emissions from any other eastern Asian countries or other regions of the world where there are available data for the detection of regional emissions. The attribution of any remaining fraction of the global CFC-11 emission rise to other regions is limited by the sparsity of long-term measurements of sufficient frequency near potentially emissive regions. Several considerations suggest that the increase in CFC-11 emissions from eastern mainland China is likely to be the result of new production and use, which is inconsistent with the Montreal Protocol agreement to phase out global chlorofluorocarbon production by 2010. Emissions from eastern China account for approximately 40 to 60 per cent of the global rise in emissions of trichlorofluoromethane (CFC-11), which may be a result of new production and use.

Chlorofluorocarbon (CFC) banks from uses such as air conditioners or foams can be emitted after global production stops. Recent reports of unexpected emissions of CFC-11 raise the need to better quantify releases from these banks, and associated impacts on ozone depletion and climate change. Here we develop a Bayesian probabilistic model for CFC-11, 12, and 113 banks and their emissions, incorporating the broadest range of constraints to date. We find that bank sizes of CFC-11 and CFC-12 are larger than recent international scientific assessments suggested, and can account for much of current estimated CFC-11 and 12 emissions (with the exception of increased CFC-11 emissions after 2012). Left unrecovered, these CFC banks could delay Antarctic ozone hole recovery by about six years and contribute 9 billion metric tonnes of equivalent CO 2 emission. Derived CFC-113 emissions are subject to uncertainty, but are much larger than expected, raising questions about its sources. Following international agreements, the use of chlorofluorocarbons in production is supposed to be phased out. Here, the authors present a new estimate of these products already in use and their emissions and show that they are larger than expected and that not recovering these banks leads to a substantial delay in the polar ozone hole recovery.

Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer-Dobson circulation (BDC), forming a protective \"ozone layer\" around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60degS and 60degN outside the polar regions (60-90deg). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60degS and 60degN has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60degS and 60degN. We find that total column ozone between 60degS and 60degN appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.