That speculation is due to increased CFC-11 emissions, a big issue that could delay ozone restoration efforts and contribute to a warming planet.
"This is the most surprising and unexpected thing that I've observed in 27 years of making these measurements", said Steve Montzka, a research chemist at NOAA and lead author of the paper. "In fact, I was amazed by this".
It's a distressing result for what's widely seen as a global environmental success story, in which nations - alarmed by a growing "ozone hole" - collectively took action to phase out chlorofluorocarbons. The discovery is likely to encourage the worldwide investigation of a mysterious source.
The 1987 Montreal Protocol phased out ozone-damaging chemicals like CFC-11 worldwide.
The scientists said the deviation coincided with a rise in amounts of two other chemicals, chlorodifluoromethane and dichloromethane, suggesting they were all coming from the same source, though it was not clear exactly where they were being produced. However, that decrease is significantly slower than it would be without the new CFC emissions.
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Thought the ozone layer was safe?
Under the Montreal Protocol, the world agreed to begin phasing out CFC-11, ending its production altogether by 2010.
Precise measurements of global atmospheric concentrations of CFC-11 made by NOAA and CIRES scientists at 12 remote sites around the globe show that CFC-11 concentrations declined at an accelerating rate prior to 2002 as expected.
Plus, it isn't just CFC-11 that was found to be increasing.
"In the end, we concluded that it's most likely that someone may be producing the CFC-11 that's escaping to the atmosphere", he said.
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Keith Weller, a spokesman for the United Nations Environment Program, which administers the Montreal Protocol, said the findings will have to be verified by the scientific panel to the Protocol, and then would be put before the treaty's member countries.
"It is therefore imperative that this finding be discussed at the next Ministerial meeting of Governments given recovery of the ozone layer is dependent on all countries complying with the Montreal Protocol (and its adjustments and amendments) with emissions globally dropping to zero".
"A timely recovery of the stratospheric ozone layer depends on a sustained decline of CFC-11 concentrations", the wrote. "They should tell the industries that's not going to work". This insults everybody who's worked on this for the last 30 years. But if the problem is allowed to persist, it could jeopardize ozone layer recovery and worsen climate change. In 2012, however, the rate of decline suddenly reduced by about 50% - indicating that new source of production had started up.
However, it took many decades for scientists to discover that when CFCs break down in the atmosphere, they release chlorine atoms that are able to rapidly destroy ozone molecules.
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