"The precise cause of the trend is unknown but could be related to changes to the stratospheric circulation, which has a large influence on how ozone is distributed," said Ryan Hossaini, an ozone expert at the University of Lancaster in Britain, who was not involved in the study. Those, in turn, could be tied to climate change.
There's also a possibility that a new class of chlorine-containing chemicals not limited by the Montreal Protocol, dubbed "very short-lived substances", could be contributing to the problem. The most prominent of these substances is dichloromethane, which has a range of industrial uses, including as a paint stripper.
Concentrations of the substance have been increasing in the atmosphere and, because of the compound's relatively short lifetime, it is not regulated under the Montreal Protocol.
At the same time, though, it's not clear that there's enough of it in the atmosphere to be causing what scientists are now observing.
It all amounts to a mystery, but a troubling one because ozone protects life at the surface from incoming ultraviolet radiation, and any thinning of total ozone in the stratosphere is cause for concern.
"We're raising the alarm that we need to very rapidly investigate whether it's the short-lived compounds, whether it's a climate change response, whether our models aren't quite doing the right job, or whether there's something wrong with the data," Ball said.
The political implications of the new research are not clear, but Ball said it does not mean the Montreal Protocol isn't working.