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Nitrous oxide (N2O) is the third most important long-lived GHG and an important stratospheric ozone depleting substance. Agricultural practices and the use of N-fertilizers have greatly enhanced emissions of N2O. Here, we present estimates of N2O emissions determined from three global atmospheric inversion frameworks during the period 1998–2016. We find that global N2O emissions increased substantially from 2009 and at a faster rate than estimated by the IPCC emission factor approach. The regions of East Asia and South America made the largest contributions to the global increase. From the inversion-based emissions, we estimate a global emission factor of 2.3 ± 0.6%, which is significantly larger than the IPCC Tier-1 default for combined direct and indirect emissions of 1.375%. The larger emission factor and accelerating emission increase found from the inversions suggest that N2O emission may have a nonlinear response at global and regional scales with high levels of N-input.

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 (CO 2 ) 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 CO 2 , 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. The climate impacts of deforestation due to changes in biogenic volatile organic compound emissions, which act as short-lived climate forcers (SLCFs), are poorly understood. Here the authors show that including the impact SLCFs increases the projected warming associated with idealised deforestation scenarios.

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. The Antarctic ozone hole is decreasing in size due to policies implemented following the Montreal Protocol. Here, model simulations show that if recently discovered increase in unreported CFC-11 emissions continue, they could delay the recovery of the ozone hole by well over a decade.

Short-lived halogens are produced naturally and anthropogenically, and are not governed by the Montreal Protocol. Like halocarbons, short-lived halogens destroy lower-stratospheric ozone, resulting in a net cooling effect since pre-industrial times. Halogens released from long-lived anthropogenic substances, such as chlorofluorocarbons, are the principal cause of recent depletion of stratospheric ozone, a greenhouse gas 1 , 2 , 3 . Recent observations show that very short-lived substances, with lifetimes generally under six months, are also an important source of stratospheric halogens 4 , 5 . Short-lived bromine substances are produced naturally by seaweed and phytoplankton, whereas short-lived chlorine substances are primarily anthropogenic. Here we used a chemical transport model to quantify the depletion of ozone in the lower stratosphere from short-lived halogen substances, and a radiative transfer model to quantify the radiative effects of that ozone depletion. According to our simulations, ozone loss from short-lived substances had a radiative effect nearly half that from long-lived halocarbons in 2011 and, since pre-industrial times, has contributed a total of about −0.02 W m −2 to global radiative forcing. We find natural short-lived bromine substances exert a 3.6 times larger ozone radiative effect than long-lived halocarbons, normalized by halogen content, and show atmospheric levels of dichloromethane, a short-lived chlorine substance not controlled by the Montreal Protocol, are rapidly increasing. We conclude that potential further significant increases in the atmospheric abundance of short-lived halogen substances, through changing natural processes 6 , 7 , 8 or continued anthropogenic emissions 9 , could be important for future climate.

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. Ozone-depleting substances have been controlled by the 1987 Montreal Protocol, ensuring atmospheric concentrations are now in decline. Here, the authors use a 3D model and suggest that these controls have already had significant benefits, with much larger ozone depletion than previously thought avoided by the protocol.

A chemistry-transport model (CTM) intercomparison experiment (TransCom-CH4 ) has been designed to investigate the roles of surface emissions, transport and chemical loss in simulating the global methane distribution. Model simulations were conducted using twelve models and four model variants and results were archived for the period of 1990-2007. All but one model transports were driven by reanalysis products from 3 different meteorological agencies. The transport and removal of CH4 in six different emission scenarios were simulated, with net global emissions of 513 ± 9 and 514 ± 14 Tg CH4 yr-1 for the 1990s and 2000s, respectively. Additionally, sulfur hexafluoride (SF6 ) was simulated to check the interhemispheric transport, radon (222 Rn) to check the subgrid scale transport, and methyl chloroform (CH3 CCl3 ) to check the chemical removal by the tropospheric hydroxyl radical (OH). The results are compared to monthly or annual mean time series of CH4 , SF6 and CH3 CCl3 measurements from 8 selected background sites, and to satellite observations of CH4 in the upper troposphere and stratosphere. Most models adequately capture the vertical gradients in the stratosphere, the average long-term trends, seasonal cycles, interannual variations (IAVs) and interhemispheric (IH) gradients at the surface sites for SF6 , CH3 CCl3 and CH4 . The vertical gradients of all tracers between the surface and the upper troposphere are consistent within the models, revealing vertical transport differences between models. An average IH exchange time of 1.39 ± 0.18 yr is derived from SF6 time series. Sensitivity simulations suggest that the estimated trends in exchange time, over the period of 1996-2007, are caused by a change of SF6 emissions towards the tropics. Using six sets of emission scenarios, we show that the decadal average CH4 growth rate likely reached equilibrium in the early 2000s due to the flattening of anthropogenic emission growth since the late 1990s. Up to 60% of the IAVs in the observed CH4 concentrations can be explained by accounting for the IAVs in emissions, from biomass burning and wetlands, as well as meteorology in the forward models. The modeled CH4 budget is shown to depend strongly on the troposphere-stratosphere exchange rate and thus on the model's vertical grid structure and circulation in the lower stratosphere. The 15-model median CH4 and CH3 CCl3 atmospheric lifetimes are estimated to be 9.99 ± 0.08 and 4.61 ± 0.13 yr, respectively, with little IAV due to transport and temperature.

Air pollutants, such as ozone, have adverse impacts on human health and cause, for example, respiratory and cardiovascular problems. In the United Kingdom (UK), peak surface ozone concentrations typically occur in the spring and summer and are controlled by emission of precursor gases, tropospheric chemistry and local meteorology which can be influenced by large-scale synoptic weather regimes. In this study we composite surface and satellite observations of summer-time (April to September) ozone under different UK atmospheric circulation patterns, as defined by the Lamb weather types. Anticyclonic conditions and easterly flows are shown to significantly enhance ozone concentrations over the UK relative to summer-time average values. Anticyclonic stability and light winds aid the trapping of ozone and its precursor gases near the surface. Easterly flows (NE, E, SE) transport ozone and precursor gases from polluted regions in continental Europe (e.g. the Benelux region) to the UK. Cyclonic conditions and westerly flows, associated with unstable weather, transport ozone from the UK mainland, replacing it with clean maritime (North Atlantic) air masses. Increased cloud cover also likely decrease ozone production rates. We show that the UK Met Office regional air quality model successfully reproduces UK summer-time ozone concentrations and ozone enhancements under anticyclonic and south-easterly conditions for the summer of 2006. By using established ozone exposure-health burden metrics, anticyclonic and easterly condition enhanced surface ozone concentrations pose the greatest public health risk.

Policies have been in place since 1987 to reduce the release of chlorine atoms in the stratosphere, where they deplete ozone; here observations show that since 2007 hydrogen chloride has been increasing in the lower stratosphere of the Northern Hemisphere, an increase that is attributed to a slowdown in atmospheric circulation. Stratospheric chlorine reservoir rising The Montreal Protocol, the 1987 UN treaty that restricted the use of the major chlorine- and bromine-containing halocarbons that were damaging the stratospheric ozone layer, has led to a decrease in the main stratospheric chlorine reservoir, hydrogen chloride. This paper reports a recent increase in hydrogen chloride in the Northern Hemisphere. With the help of a model study, the authors attribute the phenomenon to a short-term slowdown in the Northern Hemisphere atmospheric circulation that transports aged air, with a larger relative conversion of chlorine source gases to hydrogen chloride in the lower stratosphere. The increase in hydrogen chloride is not the result of unaccounted emissions from chlorine-containing source gases and the Montreal treaty continues to lead to an overall long-term reduction in stratospheric halogens. 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 1 , before they reach the stratosphere where they release chlorine atoms that cause ozone depletion 2 . The large ozone loss over Antarctica 3 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 4 , in line with expectations. Remote-sensing data have revealed a peak in stratospheric chlorine after 1996 5 , then a decrease of close to one per cent per year 6 , 7 , in agreement with the surface observations of the chlorine source gases and model calculations 7 . Here we present ground-based and satellite data that show a recent and significant increase, at the 2 σ 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.

The Mediterranean troposphere exhibits a marked and localised summertime ozone maximum, which has the potential to strongly impact regional air quality and radiative forcing. The Mediterranean region can be perturbed by long-range pollution import from Northern Europe, North America and Asia, in addition to local emissions, which may all contribute to regional ozone enhancements. We exploit ozone profile observations from the Tropospheric Emission Spectrometer (TES) and the Global Ozone Monitoring Experiment-2 (GOME-2) satellite instruments, and an offline 3-D global chemical transport model (TOMCAT) to investigate the geographical and vertical structure of the summertime tropospheric ozone maximum over the Mediterranean region. We show that both TES and GOME-2 are able to detect enhanced levels of ozone in the lower troposphere over the region during the summer. These observations, together with surface measurements, are used to evaluate the TOMCAT model's ability to capture the observed ozone enhancement. The model is used to quantify sensitivities of the ozone maximum to anthropogenic and natural volatile organic compound (VOC) emissions, anthropogenic NOx emissions, wildfire emissions and long-range import of ozone and precursors. Our results show a dominant sensitivity to natural VOC emissions in the Mediterranean basin over anthropogenic VOC emissions. However, local anthropogenic NOx emissions are result in the overall largest sensitivity in near-surface ozone. We also show that in the lower troposphere, global VOC emissions account for 40% of the ozone sensitivity to VOC emissions in the region, whereas, for NOx the ozone sensitivity to local sources is 9 times greater than that for global emissions at these altitudes. However, in the mid and upper troposphere ozone is most sensitive to non-local emission sources. In terms of radiative effects on regional climate, ozone contributions from non-local emission sources are more important, as these have a larger impact on ozone in the upper troposphere where its radiative effects are larger, with Asian monsoon outflow having the greatest impact. Our results allow improved understanding of the large-scale processes controlling air quality and climate in the region of the Mediterranean basin.

A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment pseudo-modal aerosol dynamics approach rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulfate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulfuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulfate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.