An unexpected and persistent increase in global emissions of ozone-depleting CFC-11.

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 atmosphere1-3. 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.

Deriving Global OH Abundance and Atmospheric Lifetimes for Long-Lived Gases: A Search for CH3CCl3 Alternatives.

An accurate estimate of global hydroxyl radical (OH) abundance is important for projections of air quality, climate, and stratospheric ozone recovery. As the atmospheric mixing ratios of methyl chloroform (CH3CCl3) (MCF), the commonly used OH reference gas, approaches zero, it is important to find alternative approaches to infer atmospheric OH abundance and variability. The lack of global bottom-up emission inventories is the primary obstacle in choosing a MCF alternative. We illustrate that global emissions of long-lived trace gases can be inferred from their observed mixing ratio differences between the Northern Hemisphere (NH) and Southern Hemisphere (SH), given realistic estimates of their NH-SH exchange time, the emission partitioning between the two hemispheres, and the NH versus SH OH abundance ratio. Using the observed long-term trend and emissions derived from the measured hemispheric gradient, the combination of HFC-32 (CH2F2), HFC-134a (CH2FCF3, HFC-152a (CH3CHF2), and HCFC-22 (CHClF2), instead of a single gas, will be useful as a MCF alternative to infer global and hemispheric OH abundance and trace gas lifetimes. The primary assumption on which this multispecies approach relies is that the OH lifetimes can be estimated by scaling the thermal reaction rates of a reference gas at 272 K on global and hemispheric scales. Thus, the derived hemispheric and global OH estimates are forced to reconcile the observed trends and gradient for all four compounds simultaneously. However, currently, observations of these gases from the surface networks do not provide more accurate OH abundance estimate than that from MCF.

A post-Kyoto partner: considering the stratospheric ozone regime as a tool to manage nitrous oxide.

Nitrous oxide (N2O) is the largest known remaining anthropogenic threat to the stratospheric ozone layer. However, it is currently only regulated under the 1997 Kyoto Protocol because of its simultaneous ability to warm the climate. The threat N2O poses to the stratospheric ozone layer, coupled with the uncertain future of the international climate regime, motivates our exploration of issues that could be relevant to the Parties to the ozone regime (the 1985 Vienna Convention and its 1987 Montreal Protocol) should they decide to take measures to manage N2O in the future. There are clear legal avenues to regulate N2O under the ozone regime as well as several ways to share authority with the existing and future international climate treaties. N2O mitigation strategies exist to address the most significant anthropogenic sources, including agriculture, where behavioral practices and new technologies could contribute significantly to reducing emissions. Existing policies managing N2O and other forms of reactive nitrogen could be harnessed and built on by the ozone regime to implement N2O controls. There are several challenges and potential cobenefits to N2O control which we discuss here: food security, equity, and implications of the nitrogen cascade. The possible inclusion of N2O in the ozone regime need not be viewed as a sign of failure of the United Nations Framework Convention on Climate Change to adequately deal with climate change. Rather, it could represent an additional valuable tool in sustainable development diplomacy.

Persistence of climate changes due to a range of greenhouse gases.

Emissions of a broad range of greenhouse gases of varying lifetimes contribute to global climate change. Carbon dioxide displays exceptional persistence that renders its warming nearly irreversible for more than 1,000 y. Here we show that the warming due to non-CO(2) greenhouse gases, although not irreversible, persists notably longer than the anthropogenic changes in the greenhouse gas concentrations themselves. We explore why the persistence of warming depends not just on the decay of a given greenhouse gas concentration but also on climate system behavior, particularly the timescales of heat transfer linked to the ocean. For carbon dioxide and methane, nonlinear optical absorption effects also play a smaller but significant role in prolonging the warming. In effect, dampening factors that slow temperature increase during periods of increasing concentration also slow the loss of energy from the Earth's climate system if radiative forcing is reduced. Approaches to climate change mitigation options through reduction of greenhouse gas or aerosol emissions therefore should not be expected to decrease climate change impacts as rapidly as the gas or aerosol lifetime, even for short-lived species; such actions can have their greatest effect if undertaken soon enough to avoid transfer of heat to the deep ocean.

Contributions of stratospheric water vapor to decadal changes in the rate of global warming.

Stratospheric water vapor concentrations decreased by about 10% after the year 2000. Here we show that this acted to slow the rate of increase in global surface temperature over 2000-2009 by about 25% compared to that which would have occurred due only to carbon dioxide and other greenhouse gases. More limited data suggest that stratospheric water vapor probably increased between 1980 and 2000, which would have enhanced the decadal rate of surface warming during the 1990s by about 30% as compared to estimates neglecting this change. These findings show that stratospheric water vapor is an important driver of decadal global surface climate change.

Nitrous oxide (N2O): the dominant ozone-depleting substance emitted in the 21st century.

By comparing the ozone depletion potential-weighted anthropogenic emissions of N2O with those of other ozone-depleting substances, we show that N2O emission currently is the single most important ozone-depleting emission and is expected to remain the largest throughout the 21st century. N2O is unregulated by the Montreal Protocol. Limiting future N2O emissions would enhance the recovery of the ozone layer from its depleted state and would also reduce the anthropogenic forcing of the climate system, representing a win-win for both ozone and climate.

The large contribution of projected HFC emissions to future climate forcing.

The consumption and emissions of hydrofluorocarbons (HFCs) are projected to increase substantially in the coming decades in response to regulation of ozone depleting gases under the Montreal Protocol. The projected increases result primarily from sustained growth in demand for refrigeration, air-conditioning (AC) and insulating foam products in developing countries assuming no new regulation of HFC consumption or emissions. New HFC scenarios are presented based on current hydrochlorofluorocarbon (HCFC) consumption in leading applications, patterns of replacements of HCFCs by HFCs in developed countries, and gross domestic product (GDP) growth. Global HFC emissions significantly exceed previous estimates after 2025 with developing country emissions as much as 800% greater than in developed countries in 2050. Global HFC emissions in 2050 are equivalent to 9-19% (CO(2)-eq. basis) of projected global CO(2) emissions in business-as-usual scenarios and contribute a radiative forcing equivalent to that from 6-13 years of CO(2) emissions near 2050. This percentage increases to 28-45% compared with projected CO(2) emissions in a 450-ppm CO(2) stabilization scenario. In a hypothetical scenario based on a global cap followed by 4% annual reductions in consumption, HFC radiative forcing is shown to peak and begin to decline before 2050.

The importance of the Montreal Protocol in protecting climate.

The 1987 Montreal Protocol on Substances that Deplete the Ozone Layer is a landmark agreement that has successfully reduced the global production, consumption, and emissions of ozone-depleting substances (ODSs). ODSs are also greenhouse gases that contribute to the radiative forcing of climate change. Using historical ODSs emissions and scenarios of potential emissions, we show that the ODS contribution to radiative forcing most likely would have been much larger if the ODS link to stratospheric ozone depletion had not been recognized in 1974 and followed by a series of regulations. The climate protection already achieved by the Montreal Protocol alone is far larger than the reduction target of the first commitment period of the Kyoto Protocol. Additional climate benefits that are significant compared with the Kyoto Protocol reduction target could be achieved by actions under the Montreal Protocol, by managing the emissions of substitute fluorocarbon gases and/or implementing alternative gases with lower global warming potentials.

Airborne observations of vegetation and implications for biogenic emission characterization.

Measuring hydrocarbons from aircraft represents one way to infer biogenic emissions at the surface. The focus of this paper is to show that complementary remote sensing information can be provided by optical measurements of a vegetation index, which is readily measured with high temporal coverage using reflectance data. We examine the similarities between the vegetation index and in situ measurements of the chemicals isoprene, methacrolein, and alpha-pinene to estimate whether the temporal behavior of the in situ measurements of these chemicals could be better understood by the addition of the vegetation index. Data were compared for flights conducted around Houston in August and September 2000. The three independent sets of chemical measurements examined correspond reasonably well with the vegetation index curves for the majority of flight days. While low values of the vegetation index always correspond to low values of the in situ chemical measurements, high values of the index correspond to both high and low values of the chemical measurements. In this sense it represents an upper limit when compared with in situ data (assuming the calibration constant is adequately chosen). This result suggests that while the vegetation index cannot represent a purely predictive quantity for the in situ measurements, it represents a complementary measurement that can be useful in understanding comparisons of various in situ observations, particularly when these observations occur with relatively low temporal frequency. In situ isoprene measurements and the vegetation index were also compared to an isoprene emission inventory to provide additional insight on broad issues relating to the use of vegetation indices in emission database development.