Challenges for the recovery of the ozone layer

The recovery of stratospheric ozone from past depletion is underway owing to the 1987 Montreal Protocol and its subsequent amendments, which have been effective in phasing out the production and consumption of the major ozone-depleting substances (ODSs). However, there is uncertainty about the future rate of recovery. This uncertainty relates partly to unexpected emissions of controlled anthropogenic ODSs such as CCl₃F and slower-than-expected declines in atmospheric CCl₄. A further uncertainty surrounds emissions of uncontrolled short-lived anthropogenic ODSs (such as CH₂Cl₂ and CHCl₃), which observations show have been increasing in the atmosphere through 2017, as well as potential emission increases in natural ODSs (such as CH₃Cl and CH₃Br) induced by climate change, changes in atmospheric concentrations of greenhouse gases N₂O and CH₄, and stratospheric geoengineering. These challenges could delay the return of stratospheric ozone levels to historical values, (for example, the abundance in 1980), by up to decades, depending on the future evolution of the emissions and other influencing factors. To mitigate the threats to future ozone recovery, it is crucial to ensure that the Montreal Protocol and its amendments continue to be implemented effectively in order to have firm control on future levels of ODSs. This action needs to be supported by an expansion of the geographic coverage of atmospheric observations of ODSs, by enhancing the ability of source attribution modelling, and by improving understanding of the interactions between climate change and ozone recovery

Atmospheric science: the self-cleansing ability of prehistoric air

Isotopic data from an ice core have been used to estimate atmospheric oxidant levels during past climate transitions — pointing to relatively unexplored climate feedbacks as drivers of atmospheric composition

Ozone-depleting substances (ODSs) and related chemicals

The amended and adjusted Montreal Protocol continues to be successful at reducing emissions and atmospheric abundances of most controlled ozone-depleting substances (ODSs).Global Ozone Research and Monitoring Projec

Can the envisaged reductions of fossil fuel CO2 emissions be detected by atmospheric observations?

The lower troposphere is an excellent receptacle, which integrates anthropogenic greenhouse gases emissions over large areas. Therefore, atmospheric concentration observations over populated regions would provide the ultimate proof if sustained emissions changes have occurred. The most important anthropogenic greenhouse gas, carbon dioxide (CO2), also shows large natural concentration variations, which need to be disentangled from anthropogenic signals to assess changes in associated emissions. This is in principle possible for the fossil fuel CO2 component (FFCO2) by high-precision radiocarbon (14C) analyses because FFCO2 is free of radiocarbon. Long-term observations of 14CO2 conducted at two sites in south-western Germany do not yet reveal any significant trends in the regional fossil fuel CO2 component. We rather observe strong inter-annual variations, which are largely imprinted by changes of atmospheric transport as supported by dedicated transport model simulations of fossil fuel CO2. In this paper, we show that, depending on the remoteness of the site, changes of about 7–26% in fossil fuel emissions in respective catchment areas could be detected with confidence by high-precision atmospheric 14CO2 measurements when comparing 5-year averages if these inter-annual variations were taken into account. This perspective constitutes the urgently needed tool for validation of fossil fuel CO2 emissions changes in the framework of the Kyoto protocol and successive climate initiatives

Photolysis of sulphuric acid as the source of sulphur oxides in the mesosphere of Venus

The sulphur cycle plays fundamental roles in the chemistry and climate of Venus. Thermodynamic equilibrium chemistry at the surface of Venus favours the production of carbonyl sulphide and to a lesser extent sulphur dioxide. These gases are transported to the middle atmosphere by the Hadley circulation cell. Above the cloud top, a sulphur oxidation cycle involves conversion of carbonyl sulphide into sulphur dioxide, which is then transported further upwards. A significant fraction of this sulphur dioxide is subsequently oxidized to sulphur trioxide and eventually reacts with water to form sulphuric acid. Because the vapour pressure of sulphuric acid is low, it readily condenses and forms an upper cloud layer at altitudes of 60–70 km, and an upper haze layer above 70 km (ref. 9), which effectively sequesters sulphur oxides from photochemical reactions. Here we present simulations of the fate of sulphuric acid in the Venusian mesosphere based on the Caltech/JPL kinetics model, but including the photolysis of sulphuric acid. Our model suggests that the mixing ratios of sulphur oxides are at least five times higher above 90 km when the photolysis of sulphuric acid is included. Our results are inconsistent with the previous model results but in agreement with the recent observations using ground-based microwave spectroscopy and by Venus Express

Historical greenhouse gas concentrations for climate modelling (CMIP6)

Atmospheric greenhouse gas (GHG) concentrations are at unprecedented, record-high levels compared to the last 800 000 years. Those elevated GHG concentrations warm the planet and – partially offset by net cooling effects by aerosols – are largely responsible for the observed warming over the past 150 years. An accurate representation of GHG concentrations is hence important to understand and model recent climate change. So far, community efforts to create composite datasets of GHG concentrations with seasonal and latitudinal information have focused on marine boundary layer conditions and recent trends since the 1980s. Here, we provide consolidated datasets of historical atmospheric concentrations (mole fractions) of 43 GHGs to be used in the Climate Model Intercomparison Project – Phase 6 (CMIP6) experiments. The presented datasets are based on AGAGE and NOAA networks, firn and ice core data, and archived air data, and a large set of published studies. In contrast to previous intercomparisons, the new datasets are latitudinally resolved and include seasonality. We focus on the period 1850–2014 for historical CMIP6 runs, but data are also provided for the last 2000 years. We provide consolidated datasets in various spatiotemporal resolutions for carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O), as well as 40 other GHGs, namely 17 ozone-depleting substances, 11 hydrofluorocarbons (HFCs), 9 perfluorocarbons (PFCs), sulfur hexafluoride (SF6), nitrogen trifluoride (NF3) and sulfuryl fluoride (SO2F2). In addition, we provide three equivalence species that aggregate concentrations of GHGs other than CO2, CH4 and N2O, weighted by their radiative forcing efficiencies. For the year 1850, which is used for pre-industrial control runs, we estimate annual global-mean surface concentrations of CO2 at 284.3 ppm, CH4 at 808.2 ppb and N2O at 273.0 ppb. The data are available at https://esgfnode.llnl.gov/search/input4mips/ and http://www.climatecollege.unimelb.edu.au/cmip6. While the minimum CMIP6 recommendation is to use the global- and annual-mean time series, modelling groups can also choose our monthly and latitudinally resolved concentrations, which imply a stronger radiative forcing in the Northern Hemisphere winter (due to the latitudinal gradient and seasonality)

Reductions in ozone at high concentrations of stratospheric halogens

An increase in the concentration of inorganic chlorine to levels comparable to that of oxidized reactive nitrogen could cause a significant change in the chemistry of the lower stratosphere leading to a reduction potentially larger than 15% in the column density of ozone. This could occur, for example by the middle of the next century, if emissions of man-made chlorocarbons were to grow at a rate of 3% per year. Ozone could be further depressed by release of industrial bromocarbon