Delay in recovery of the Antarctic ozone hole from unexpected CFC-11 emissions.

The Antarctic ozone hole is decreasing in size but this recovery will be affected by atmospheric variability and any unexpected changes in chlorinated source gas emissions. Here, using model simulations, we show that the ozone hole will largely cease to occur by 2065 given compliance with the Montreal Protocol. If the unusual meteorology of 2002 is repeated, an ozone-hole-free-year could occur as soon as the early 2020s by some metrics. The recently discovered increase in CFC-11 emissions of ~ 13 Gg yr-1 may delay recovery. So far the impact on ozone is small, but if these emissions indicate production for foam use much more CFC-11 may be leaked in the future. Assuming such production over 10 years, disappearance of the ozone hole will be delayed by a few years, although there are significant uncertainties. Continued, substantial future CFC-11 emissions of 67 Gg yr-1 would delay Antarctic ozone recovery by well over a decade.

Large impacts, past and future, of ozone-depleting substances on Brewer-Dobson circulation trends: A multi-model assessment.

Substantial increases in the atmospheric concentration of well-mixed greenhouse gases (notably CO2), such as those projected to occur by the end of the 21st century under large radiative forcing scenarios, have long been known to cause an acceleration of the Brewer-Dobson circulation (BDC) in climate models. More recently, however, several single-model studies have proposed that ozone-depleting substances might also be important drivers of BDC trends. As these studies were conducted with different forcings over different periods, it is difficult to combine them to obtain a robust quantitative picture of the relative importance of ozone-depleting substances as drivers of BDC trends. To this end we here analyze - over identical past and future periods - the output from 20 similarly-forced models, gathered from two recent chemistry-climate modeling intercomparison projects. Our multi-model analysis reveals that ozone-depleting substances are responsible for more than half of the modeled BDC trends in the two decades 1980-2000. We also find that, as a consequence of the Montreal Protocol, decreasing concentrations of ozone-depleting substances in coming decades will strongly decelerate the BDC until the year 2080, reducing the age-of-air trends by more than half, and will thus substantially mitigate the impact of increasing CO2. As ozone-depleting substances impact BDC trends, primarily, via the depletion/recovery of stratospheric ozone over the South Pole, they impart seasonal and hemispheric asymmetries to the trends which may offer opportunities for detection in coming decades.

Impact on short-lived climate forcers increases projected warming due to deforestation.

The climate impact of deforestation depends on the relative strength of several biogeochemical and biogeophysical effects. In addition to affecting the exchange of carbon dioxide (CO2) and moisture with the atmosphere and surface albedo, vegetation emits biogenic volatile organic compounds (BVOCs) that alter the formation of short-lived climate forcers (SLCFs), which include aerosol, ozone and methane. Here we show that a scenario of complete global deforestation results in a net positive radiative forcing (RF; 0.12 W m-2) from SLCFs, with the negative RF from decreases in ozone and methane concentrations partially offsetting the positive aerosol RF. Combining RFs due to CO2, surface albedo and SLCFs suggests that global deforestation could cause 0.8 K warming after 100 years, with SLCFs contributing 8% of the effect. However, deforestation as projected by the RCP8.5 scenario leads to zero net RF from SLCF, primarily due to nonlinearities in the aerosol indirect effect.

Impact on short-lived climate forcers (SLCFs) from a realistic land-use change scenario via changes in biogenic emissions.

More than one quarter of natural forests have been cleared by humans to make way for other land-uses, with changes to forest cover projected to continue. The climate impact of land-use change (LUC) is dependent upon the relative strength of several biogeophysical and biogeochemical effects. In addition to affecting the surface albedo and exchanging carbon dioxide (CO2) and moisture with the atmosphere, vegetation emits biogenic volatile organic compounds (BVOCs), altering the formation of short-lived climate forcers (SLCFs) including aerosol, ozone (O3) and methane (CH4). Once emitted, BVOCs are rapidly oxidised by O3, and the hydroxyl (OH) and nitrate (NO3) radicals. These oxidation reactions yield secondary organic products which are implicated in the formation and growth of aerosol particles and are estimated to have a negative radiative effect on the climate (i.e. a cooling). These reactions also deplete OH, increasing the atmospheric lifetime of CH4, and directly affect concentrations of O3; the latter two being greenhouse gases which impose a positive radiative effect (i.e. a warming) on the climate. Our previous work assessing idealised deforestation scenarios found a positive radiative effect due to changes in SLCFs; however, since the radiative effects associated with changes to SLCFs result from a combination of non-linear processes it may not be appropriate to scale radiative effects from complete deforestation scenarios according to the deforestation extent. Here we combine a land-surface model, a chemical transport model, a global aerosol model, and a radiative transfer model to assess the net radiative effect of changes in SLCFs due to historical LUC between the years 1850 and 2000.

Solar cycle response and long-term trends in the mesospheric metal layers.

The meteoric metal layers (Na, Fe, and K)-which form as a result of the ablation of incoming meteors-act as unique tracers for chemical and dynamical processes that occur within the upper mesosphere/lower thermosphere region. In this work, we examine whether these metal layers are sensitive indicators of decadal long-term changes within the upper atmosphere. Output from a whole-atmosphere climate model is used to assess the response of the Na, K, and Fe layers across a 50 year period (1955-2005). At short timescales, the K layer has previously been shown to exhibit a very different seasonal behavior compared to the other metals. Here we show that this unusual behavior is also exhibited at longer timescales (both the ~11 year solar cycle and 50 year periods), where K displays a much more pronounced response to atmospheric temperature changes than either Na or Fe. The contrasting solar cycle behavior of the K and Na layers predicted by the model is confirmed using satellite and lidar observations for the period 2004-2013.

Quantifying the ozone and ultraviolet benefits already achieved by the Montreal Protocol.

Chlorine- and bromine-containing ozone-depleting substances (ODSs) are controlled by the 1987 Montreal Protocol. In consequence, atmospheric equivalent chlorine peaked in 1993 and has been declining slowly since then. Consistent with this, models project a gradual increase in stratospheric ozone with the Antarctic ozone hole expected to disappear by ∼2050. However, we show that by 2013 the Montreal Protocol had already achieved significant benefits for the ozone layer. Using a 3D atmospheric chemistry transport model, we demonstrate that much larger ozone depletion than observed has been avoided by the protocol, with beneficial impacts on surface ultraviolet. A deep Arctic ozone hole, with column values <120 DU, would have occurred given meteorological conditions in 2011. The Antarctic ozone hole would have grown in size by 40% by 2013, with enhanced loss at subpolar latitudes. The decline over northern hemisphere middle latitudes would have continued, more than doubling to ∼15% by 2013.

Diurnal variation of the potassium layer in the upper atmosphere.

Measurements of the diurnal cycle of potassium (K) atoms between 80 and 110 km have been made during October (for the years 2004-2011) using a Doppler lidar at Kühlungsborn, Germany (54.1°N, 11.7°E). A pronounced diurnal variation is observed in the K number density, which is explored by using a detailed description of the neutral and ionized chemistry of K in a three-dimensional chemistry climate model. The model captures both the amplitude and phase of the diurnal and semidiurnal variability of the layer, although the peak diurnal amplitude around 90 km is overestimated. The model shows that the total potassium density (≈ K + K+ + KHCO3) exhibits little diurnal variation at each altitude, and the diurnal variations are largely driven by photochemical conversion between these reservoir species. In contrast, tidally driven vertical transport has a small effect at this midlatitude location, and diurnal fluctuations in temperature are of little significance because they are small and the chemistry of K is relatively temperature independent.

The near-global mesospheric potassium layer: Observations and modeling.

The meteoric metal layers act as unique tracers of chemistry and dynamics in the upper atmosphere. Existing lidar studies from a few locations show that K exhibits a semiannual seasonality (winter and summer maxima), quite unlike the annual seasonality (winter maximum and summer minimum) seen with Na and Fe. This work uses spaceborne observations made with the Optical Spectrograph and InfraRed Imager System instrument on the Odin satellite to retrieve the near-global K layer for the first time. The satellite data (2004 to mid-2013) are used to validate the implementation of a recently proposed potassium chemistry scheme in a whole atmosphere chemistry climate model, which provides a chemical basis for this semiannual seasonal behavior. The satellite and model data show that this semiannual seasonality is near global in extent, with the strongest variation at middle and high latitudes. The column abundance, centroid layer height, and root-mean-square width of the K layer are consistent with the limited available lidar record. The K data set is then used to investigate the impact of polar mesospheric clouds on the metal layers at high latitudes during summer. Finally, the occurrence frequency of sporadic K layers and their possible link to sporadic E layers are examined.

Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol.

We have developed a chemical mechanism describing the tropospheric degradation of chlorine containing very short-lived substances (VSLS). The scheme was included in a global atmospheric model and used to quantify the stratospheric injection of chlorine from anthropogenic VSLS ( ClyVSLS) between 2005 and 2013. By constraining the model with surface measurements of chloroform (CHCl3), dichloromethane (CH2Cl2), tetrachloroethene (C2Cl4), trichloroethene (C2HCl3), and 1,2-dichloroethane (CH2ClCH2Cl), we infer a 2013 ClyVSLS mixing ratio of 123 parts per trillion (ppt). Stratospheric injection of source gases dominates this supply, accounting for ∼83% of the total. The remainder comes from VSLS-derived organic products, phosgene (COCl2, 7%) and formyl chloride (CHClO, 2%), and also hydrogen chloride (HCl, 8%). Stratospheric ClyVSLS increased by ∼52% between 2005 and 2013, with a mean growth rate of 3.7 ppt Cl/yr. This increase is due to recent and ongoing growth in anthropogenic CH2Cl2-the most abundant chlorinated VSLS not controlled by the Montreal Protocol.

Revisiting the hemispheric asymmetry in midlatitude ozone changes following the Mount Pinatubo eruption: A 3-D model study.

Following the eruption of Mount Pinatubo, satellite and in situ measurements showed a large enhancement in stratospheric aerosol in both hemispheres, but significant midlatitude column O3 depletion was observed only in the north. We use a three-dimensional chemical transport model to determine the mechanisms behind this hemispheric asymmetry. The model, forced by European Centre for Medium-Range Weather Forecasts ERA-Interim reanalyses and updated aerosol surface area density, successfully simulates observed large column NO2 decreases and the different extents of ozone depletion in the two hemispheres. The chemical ozone loss is similar in the Northern (NH) and Southern Hemispheres (SH), but the contrasting role of dynamics increases the depletion in the NH and decreases it in the SH. The relevant SH dynamics are not captured as well by earlier ERA-40 reanalyses. Overall, the smaller SH column O3 depletion can be attributed to dynamical variability and smaller SH background lower stratosphere O3 concentrations.

Recent Northern Hemisphere stratospheric HCl increase due to atmospheric circulation changes.

The abundance of chlorine in the Earth's atmosphere increased considerably during the 1970s to 1990s, following large emissions of anthropogenic long-lived chlorine-containing source gases, notably the chlorofluorocarbons. The chemical inertness of chlorofluorocarbons allows their transport and mixing throughout the troposphere on a global scale, before they reach the stratosphere where they release chlorine atoms that cause ozone depletion. The large ozone loss over Antarctica was the key observation that stimulated the definition and signing in 1987 of the Montreal Protocol, an international treaty establishing a schedule to reduce the production of the major chlorine- and bromine-containing halocarbons. Owing to its implementation, the near-surface total chlorine concentration showed a maximum in 1993, followed by a decrease of half a per cent to one per cent per year, in line with expectations. Remote-sensing data have revealed a peak in stratospheric chlorine after 1996, then a decrease of close to one per cent per year, in agreement with the surface observations of the chlorine source gases and model calculations. Here we present ground-based and satellite data that show a recent and significant increase, at the 2σ level, in hydrogen chloride (HCl), the main stratospheric chlorine reservoir, starting around 2007 in the lower stratosphere of the Northern Hemisphere, in contrast with the ongoing monotonic decrease of near-surface source gases. Using model simulations, we attribute this trend anomaly to a slowdown in the Northern Hemisphere atmospheric circulation, occurring over several consecutive years, transporting more aged air to the lower stratosphere, and characterized by a larger relative conversion of source gases to HCl. This short-term dynamical variability will also affect other stratospheric tracers and needs to be accounted for when studying the evolution of the stratospheric ozone layer.