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Until now our understanding of the 11-year solar cycle signal (SCS) in stratospheric ozone has been largely based on high-quality but sparse ozone profiles from the Stratospheric Aerosol and Gas Experiment (SAGE) II or coarsely resolved ozone profiles from the nadir-viewing Solar Backscatter Ultraviolet Radiometer (SBUV) satellite instruments. Here, we analyse 16 years (2005–2020) of ozone profile measurements from the Microwave Limb Sounder (MLS) instrument on the Aura satellite to estimate the 11-year SCS in stratospheric ozone. Our analysis of Aura-MLS data suggests a single-peak-structured SCS profile (about 3 % near 4 hPa or 40 km) in tropical stratospheric ozone, which is significantly different to the SAGE II and SBUV-based double-peak-structured SCS. We also find that MLS-observed ozone variations are more consistent with ozone from our control model simulation that uses Naval Research Laboratory (NRL) v2 solar fluxes. However, in the lowermost stratosphere modelled ozone shows a negligible SCS compared to about 1 % in Aura-MLS data. An ensemble of ordinary least squares (OLS) and three regularised (lasso, ridge and elastic net) linear regression models confirms the robustness of the estimated SCS. In addition, our analysis of MLS and model simulations shows a large SCS in the Antarctic lower stratosphere that was not seen in earlier studies. We also analyse chemical transport model simulations with alternative solar flux data. We find that in the upper (and middle) stratosphere the model simulation with Solar Radiation and Climate Experiment (SORCE) satellite solar fluxes is also consistent with the MLS-derived SCS and agrees well with the control simulation and one which uses Spectral and Total Irradiance Reconstructions (SATIRE) solar fluxes. Hence, our model simulation suggests that with recent adjustments and corrections, SORCE data can be used to analyse effects of solar flux variations. Furthermore, analysis of a simulation with fixed solar fluxes and

Using multidecadal time series of ground-based and satellite Fourier transform infrared measurements of inorganic fluorine (i.e., total fluorine resident in stratospheric fluorine reservoirs), we investigate stratospheric circulation changes over the past 20 years. The representation of these changes in five modern reanalyses is further analyzed through chemical-transport model (CTM) simulations. From the observations but also from all reanalyses, we show that the inorganic fluorine is accumulating less rapidly in the Southern Hemisphere than in the Northern Hemisphere during the 21st century. Comparisons with a study evaluating the age-of-air of these reanalyses using the same CTM allow us to link this hemispheric asymmetry to changes in the Brewer-Dobson circulation (BDC), with the age-of-air of the Southern Hemisphere getting younger relative to that of the Northern Hemisphere. Large differences in simulated total columns and absolute trend values are, nevertheless, depicted between our simulations driven by the five reanalyses. Superimposed on this multidecadal change, we, furthermore, confirm a 5–7-year variability of the BDC that was first described in a recent study analyzing long-term time series of hydrogen chloride (HCl) and nitric acid (HNO3). It is important to stress that our results, based on observations and meteorological reanalyses, are in contrast with the projections of chemistry-climate models in response to the coupled increase of greenhouse gases and decrease of ozone-depleting substances, calling for further investigations and the continuation of long-term observations.

Atraccion de Talento de la Comunidad de Madrid (2016-T2/AMB-1405) Project STEADY (CGL2017-83198-R) Artículo firmado por 15 autores., Substantial increases in the atmospheric concentration of well-mixed greenhouse gases (notably CO_(2)), 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 multimodel 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 CO_(2). 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., Fudan University, National Natural Science Foundation of China (NSFC), Comunidad de Madrid, Ministerio de Economía, Industria y Competitividad (España), Met Office Hadley Centre Programme - BEIS, Met Office Hadley Centre Programme - Defra, European Commission, NZ Governments Strategic Science Investment Fund (SSIF), Royal Society of New Zealand, Depto. de Física de la Tierra y Astrofísica, Fac. de Ciencias Físicas, TRUE, pub, Pagado por el autor

We quantify the stratospheric injection of brominated very short-lived substances (VSLS) based on aircraft observations acquired in winter 2014 above the Tropical Western Pacific during the CONvective TRansport of Active Species in the Tropics (CONTRAST) and the Airborne Tropical TRopopause EXperiment (ATTREX) campaigns. The overall contribution of VSLS to stratospheric bromine was determined to be 5.0 ± 2.1 ppt, in agreement with the 5 ± 3 ppt estimate provided in the 2014 World Meteorological Organization (WMO) Ozone Assessment report (WMO 2014), but with lower uncertainty. Measurements of organic bromine compounds, including VSLS, were analyzed using CFC-11 as a reference stratospheric tracer. From this analysis, 2.9 ± 0.6 ppt of bromine enters the stratosphere via organic source gas injection of VSLS. This value is two times the mean bromine content of VSLS measured at the tropical tropopause, for regions outside of the Tropical Western Pacific, summarized in WMO 2014. A photochemical box model, constrained to CONTRAST observations, was used to estimate inorganic bromine from measurements of BrO collected by two instruments. The analysis indicates that 2.1 ± 2.1 ppt of bromine enters the stratosphere via inorganic product gas injection. We also examine the representation of brominated VSLS within 14 global models that participated in the Chemistry-Climate Model Initiative. The representation of stratospheric bromine in these models generally lies within the range of our empirical estimate. Models that include explicit representations of VSLS compare better with bromine observations in the lower stratosphere than models that utilize longer-lived chemicals as a surrogate for VSLS.

We describe the motivation, design, and execution of the Greenhouse gAs Uk and Global Emissions (GAUGE) project. The overarching scientific objective of GAUGE was to use atmospheric data to estimate the magnitude, distribution, and uncertainty of the UK greenhouse gas (GHG, defined here as CO2, CH4, and N2O) budget, 2013-2015. To address this objective, we established a multi-year and interlinked measurement and data analysis programme, building on an established tall-tower GHG measurement network. The calibrated measurement network comprises ground-based, airborne, ship-borne, balloon-borne, and space-borne GHG sensors. Our choice of measurement technologies and measurement locations reflects the heterogeneity of UK GHG sources, which range from small point sources such as landfills to large, diffuse sources such as agriculture. Atmospheric mole fraction data collected at the tall towers and on the ships provide information on sub-continental fluxes, representing the backbone to the GAUGE network. Additional spatial and temporal details of GHG fluxes over East Anglia were inferred from data collected by a regional network. Data collected during aircraft flights were used to study the transport of GHGs on local and regional scales. We purposely integrated new sensor and platform technologies into the GAUGE network, allowing us to lay the foundations of a strengthened UK capability to verify national GHG emissions beyond the project lifetime. For example, current satellites provide sparse and seasonally uneven sampling over the UK mainly because of its geographical size and cloud cover. This situation will improve with new and future satellite instruments, e.g. measurements of CH4 from the TROPOspheric Monitoring Instrument (TROPOMI) aboard Sentinel-5P. We use global, nested, and regional atmospheric transport models and inverse methods to infer geographically resolved CO2 and CH4 fluxes. This multi-model approach allows us to study model spread in a posteriori flux

It is well established that anthropogenic chlorine-containing chemicals contribute to ozone layer depletion. The successful implementation of the Montreal Protocol has led to reductions in the atmospheric concentration of many ozone-depleting gases, such as chlorofluorocarbons. As a consequence, stratospheric chlorine levels are declining and ozone is projected to return to levels observed pre-1980 later this century. However, recent observations show the atmospheric concentration of dichloromethane—an ozone-depleting gas not controlled by the Montreal Protocol—is increasing rapidly. Using atmospheric model simulations, we show that although currently modest, the impact of dichloromethane on ozone has increased markedly in recent years and if these increases continue into the future, the return of Antarctic ozone to pre-1980 levels could be substantially delayed. Sustained growth in dichloromethane would therefore offset some of the gains achieved by the Montreal Protocol, further delaying recovery of Earth’s ozone layer.

Up to now our understanding of the 11year ozone solar cycle signal (SCS) in the upper stratosphere has been largely based on the Stratospheric Aerosol and Gas Experiment (SAGE) II (v6.2) data record, which indicated a large positive signal which could not be reproduced by models, calling into question our understanding of the chemistry of the upper stratosphere. Here we present an analysis of new v7.0 SAGE II data which shows a smaller upper stratosphere ozone SCS, due to a more realistic ozone-temperature anticorrelation. New simulations from a state-of-art 3-D chemical transport model show a small SCS in the upper stratosphere, which is in agreement with SAGE v7.0 data and the shorter Halogen Occultation Experiment and Microwave Limb Sounder records. However, despite these improvements in the SAGE II data, there are still large uncertainties in current observational and meteorological reanalysis data sets, so accurate quantification of the influence of solar flux variability on the climate system remains an open scientific question.

The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated (nine chemical transport models and two chemistry–climate models) by simulating the major natural bromine VSLS, bromoform (CHBr3) and dibromomethane (CH2Br2), over a 20-year period (1993–2012). Except for three model simulations, all others were driven offline by (or nudged to) reanalysed meteorology. The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes. Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA's long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements – including high-altitude observations from the NASA Global Hawk platform. The models generally capture the observed seasonal cycle of surface CHBr3 and CH2Br2 well, with a strong model–measurement correlation (r ≥ 0.7) at most sites. In a given model, the absolute model–measurement agreement at the surface is highly sensitive to the choice of emissions. Large inter-model differences are apparent when using the same emission inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve best agreement to surface CHBr3 observations usin

Carbon tetrachloride (CCl4) is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. However, the current observed rate of this decrease is known to be slower than expected based on reported CCl4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (74 % of total), but a reported 10 % uncertainty in its combined photolysis cross section and quantum yield has only a modest impact on the modelled rate of CCl4 decay. This is partly due to the limiting effect of the rate of transport of CCl4 from the main tropospheric reservoir to the stratosphere, where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9 % of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (17 % of total) has the largest impact on modelled CCl4 decay due to its sizeable contribution to CCl4 loss and large lifetime uncertainty range (147 to 241 years). With an assumed CCl4 emission rate of 39 Gg year−1, the reference simulation with the best estimate of loss processes still underestimates the observed CCl4 (overestimates the decay) over the past 2 decades but to a smaller extent than previous studies. Changes to the rate of CCl4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 47 Gg year−1. Further progress in constraining the CCl4 budget is partly limited by systematic biases between observational dat

The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated, simulating the major natural bromine VSLS, bromoform (CHBr3) and dibromomethane (CH2Br2), over a 20-year period (1993-2012). The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes.Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA’s long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements - including high altitude observations from the NASA Global Hawk platform. The models generally capture the seasonal cycle of surface CHBr3 and CH2Br2 well, with a strong model-measurement correlation (r ≥ 0.7) and a low sensitivity to the choice of emission inventory, at most sites. In a given model, the absolute model-measurement agreement is highly sensitive to the choice of emissions and inter-model differences are also apparent, even when using the same inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve optimal agreement to surface CHBr3 observations using the lowest of the three CHBr3 emission inventories tested (similarly, 8 out of 11 models for CH2 Br2). In general, the models are able to rep

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.

Halogens released from long-lived anthropogenic substances, such as chlorofluorocarbons, are the principal cause of recent depletion of stratospheric ozone, a greenhouse gas(1-3). 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(6-8) or continued anthropogenic emissions(9), could be important for future climate.

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 ( inline image) 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 inline image 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 inline image 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.