Halocarbon ozone depletion and global warming potentials

Concern over the global environmental consequences of fully halogenated chlorofluorocarbons (CFCs) has created a need to determine the potential impacts of other halogenated organic compounds on stratospheric ozone and climate. The CFCs, which do not contain an H atom, are not oxidized or photolyzed in the troposphere. These compounds are transported into the stratosphere where they decompose and can lead to chlorine catalyzed ozone depletion. The hydrochlorofluorocarbons (HCFCs or HFCs), in particular those proposed as substitutes for CFCs, contain at least one hydrogen atom in the molecule, which confers on these compounds a much greater sensitivity toward oxidation by hydroxyl radicals in the troposphere, resulting in much shorter atmospheric lifetimes than CFCs, and consequently lower potential for depleting ozone. The available information is reviewed which relates to the lifetime of these compounds (HCFCs and HFCs) in the troposphere, and up-to-date assessments are reported of the potential relative effects of CFCs, HCFCs, HFCs, and halons on stratospheric ozone and global climate (through 'greenhouse' global warming)

Radiative forcing from modelled and observed stratospheric ozone changes due to the 11-year solar cycle

International audienceThree analyses of satellite observations and two sets of model studies are used to estimate changes in the stratospheric ozone distribution from solar minimum to solar maximum and are presented for three different latitudinal bands: Poleward of 30° north, between 30° north and 30° south and poleward of 30° south. In the model studies the solar cycle impact is limited to changes in UV fluxes. There is a general agreement between satellite observation and model studies, particular at middle and high northern latitudes. Ozone increases at solar maximum with peak values around 40 km. The profiles are used to calculate the radiative forcing (RF) from solar minimum to solar maximum. The ozone RF, calculated with two different radiative transfer schemes is found to be negligible (a magnitude of 0.01 Wm?2 or less), compared to the direct RF due to changes in solar irradiance, since contributions from the longwave and shortwave nearly cancel each other. The largest uncertainties in the estimates come from the lower stratosphere, where there is significant disagreement between the different ozone profiles

Multi-model simulations of the impact of international shipping on Atmospheric Chemistry and Climate in 2000 and 2030

The global impact of shipping on atmospheric chemistry and radiative forcing, as well as the associated uncertainties, have been quantified using an ensemble of ten state-of-the-art atmospheric chemistry models and a predefined set of emission data. The analysis is performed for present-day conditions ( year 2000) and for two future ship emission scenarios. In one scenario ship emissions stabilize at 2000 levels; in the other ship emissions increase with a constant annual growth rate of 2.2% up to 2030 ( termed the "Constant Growth Scenario" (CGS)). Most other anthropogenic emissions follow the IPCC ( Intergovernmental Panel on Climate Change) SRES ( Special Report on Emission Scenarios) A2 scenario, while biomass burning and natural emissions remain at year 2000 levels. An intercomparison of the model results with observations over the Northern Hemisphere (25 degrees - 60 degrees N) oceanic regions in the lower troposphere showed that the models are capable to reproduce ozone (O-3) and nitrogen oxides (NOx= NO+ NO2) reasonably well, whereas sulphur dioxide (SO2) in the marine boundary layer is significantly underestimated. The most pronounced changes in annual mean tropospheric NO2 and sulphate columns are simulated over the Baltic and North Seas. Other significant changes occur over the North Atlantic, the Gulf of Mexico and along the main shipping lane from Europe to Asia, across the Red and Arabian Seas. Maximum contributions from shipping to annual mean near-surface O-3 are found over the North Atlantic ( 5 - 6 ppbv in 2000; up to 8 ppbv in 2030). Ship contributions to tropospheric O3 columns over the North Atlantic and Indian Oceans reach 1 DU in 2000 and up to 1.8 DU in 2030. Tropospheric O-3 forcings due to shipping are 9.8 +/- 2.0 mW/m(2) in 2000 and 13.6 +/- 2.3 mW/m(2) in 2030. Whilst increasing O-3, ship NOx simultaneously enhances hydroxyl radicals over the remote ocean, reducing the global methane lifetime by 0.13 yr in 2000, and by up to 0.17 yr in 2030, introducing a negative radiative forcing. The models show future increases in NOx and O-3 burden which scale almost linearly with increases in NOx emission totals. Increasing emissions from shipping would significantly counteract the benefits derived from reducing SO2 emissions from all other anthropogenic sources under the A2 scenario over the continents, for example in Europe. Globally, shipping contributes 3% to increases in O-3 burden between 2000 and 2030, and 4.5% to increases in sulphate under A2/CGS. However, if future ground based emissions follow a more stringent scenario, the relative importance of ship emissions will increase. Inter-model differences in the simulated O-3 contributions from ships are significantly smaller than estimated uncertainties stemming from the ship emission inventory, mainly the ship emission totals, the distribution of the emissions over the globe, and the neglect of ship plume dispersion

The use of QBO, ENSO, and NAO perturbations in the evaluation of GOME-2 MetOp A total ozone measurements

In this work we present evidence that quasi-cyclical perturbations in total ozone (quasi-biennial oscillation – QBO, El Niño–Southern Oscillation – ENSO, and North Atlantic Oscillation – NAO) can be used as independent proxies in evaluating Global Ozone Monitoring Experiment (GOME) 2 aboard MetOp A (GOME-2A) satellite total ozone data, using ground-based (GB) measurements, other satellite data, and chemical transport model calculations. The analysis is performed in the frame of the validation strategy on longer time scales within the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT) Satellite Application Facility on Atmospheric Composition Monitoring (AC SAF) project, covering the period 2007–2016. Comparison of GOME-2A total ozone with ground observations shows mean differences of about -0.7±1.4&thinsp;% in the tropics (0–30∘), about +0.1±2.1&thinsp;% in the mid-latitudes (30–60∘), and about +2.5±3.2&thinsp;% and 0.0±4.3&thinsp;% over the northern and southern high latitudes (60–80∘), respectively. In general, we find that GOME-2A total ozone data depict the QBO–ENSO–NAO natural fluctuations in concurrence with the co-located solar backscatter ultraviolet radiometer (SBUV), GOME-type Total Ozone Essential Climate Variable (GTO-ECV; composed of total ozone observations from GOME, SCIAMACHY – SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY, GOME-2A, and OMI – ozone monitoring instrument, combined into one homogeneous time series), and ground-based observations. Total ozone from GOME-2A is well correlated with the QBO (highest correlation in the tropics of +0.8) in agreement with SBUV, GTO-ECV, and GB data which also give the highest correlation in the tropics. The differences between deseazonalized GOME-2A and GB total ozone in the tropics are within ±1&thinsp;%. These differences were tested further as to their correlations with the QBO. The differences had practically no QBO signal, providing an independent test of the stability of the long-term variability of the satellite data. Correlations between GOME-2A total ozone and the Southern Oscillation Index (SOI) were studied over the tropical Pacific Ocean after removing seasonal, QBO, and solar-cycle-related variability. Correlations between ozone and the SOI are on the order of +0.5, consistent with SBUV and GB observations. Differences between GOME-2A and GB measurements at the station of Samoa (American Samoa; 14.25∘&thinsp;S, 170.6∘&thinsp;W) are within ±1.9&thinsp;%. We also studied the impact of the NAO on total ozone in the northern mid-latitudes in winter. We find very good agreement between GOME-2A and GB observations over Canada and Europe as to their NAO-related variability, with mean differences reaching the ±1&thinsp;% levels. The agreement and small differences which were found between the independently produced total ozone datasets as to the influence of the QBO, ENSO, and NAO show the importance of these climatological proxies as additional tool for monitoring the long-term stability of satellite–ground-truth biases.</p

Analysis and quantification of the diversities of aerosol life cycles within AeroCom

Simulation results of global aerosol models have been assembled in the framework of the AeroCom intercomparison exercise. In this paper, we analyze the life cycles of dust, sea salt, sulfate, black carbon and particulate organic matter as simulated by sixteen global aerosol models. The diversities among the models for the sources and sinks, burdens, particle sizes, water uptakes, and spatial dispersals have been established. These diversities have large consequences for the calculated radiative forcing and the aerosol concentrations at the surface. The AeroCom all-models-average emissions are dominated by the mass of sea salt (SS), followed by dust (DU), sulfate (SO_4), particulate organic matter (POM), and finally black carbon (BC). Interactive parameterizations of the emissions and contrasting particles sizes of SS and DU lead generally to higher diversities of these species, and for total aerosol. The lower diversity of the emissions of the fine aerosols, BC, POM, and SO_4, is due to the use of similar emission inventories, and does therefore not necessarily indicate a better understanding of their sources. The diversity of SO_4-sources is mainly caused by the disagreement on depositional loss of precursor gases and on chemical production. The diversities of the emissions are passed on to the burdens, but the latter are also strongly affected by the model-specific treatments of transport and aerosol processes. The burdens of dry masses decrease from largest to smallest: DU, SS, SO_4, POM, and BC. The all-models-average residence time is shortest for SS with about half a day, followed by S_O4 and DU with four days, and POM and BC with six and seven days, respectively. The wet deposition rate is controlled by the solubility and increases from DU, BC, POM to SO_4 and SS. It is the dominant sink for SO_4, BC, and POM, and contributes about one third to the total removal rate coefficients of SS and DU species. For SS and DU we find high diversities for the removal rate coefficients and deposition pathways. Models do neither agree on the split between wet and dry deposition, nor on that between sedimentation and turbulent dry Deposition. We diagnose an extremely high diversity for the uptake of ambient water vapor that influences the particle size and thus the sink rate coefficients. Furthermore, we find little agreement among the model results for the partitioning of wet removal into scavenging by convective and stratiform rain. Large differences exist for aerosol dispersal both in the vertical and in the horizontal direction. In some models, a minimum of total aerosol concentration is simulated at the surface. Aerosol dispersal is most pronounced for SO4 and BC and lowest for SS. Diversities are higher for meridional than for vertical dispersal, they are similar for a given species and highest for SS and DU. For these two components we do not find a correlation between vertical and meridional aerosol dispersal. In addition the degree of dispersals of SS and DU is not related to their residence times. SO_4, BC, and POM, however, show increased meridional dispersal in models with larger vertical dispersal, and dispersal is larger for longer simulated residence times

The effect of harmonized emissions on aerosol properties in global models – an AeroCom experiment

The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA) and one with unified emissions, injection heights, and particle sizes at the source (ExpB). Surprisingly, harmonization of aerosol sources has only a small impact on the simulated diversity for aerosol burden, and consequently optical properties, as the results are largely controlled by model-specific transport, removal, chemistry (leading to the formation of secondary aerosols) and parameterizations of aerosol microphysics (e.g. the split between deposition pathways) and to a lesser extent on the spatial and temporal distributions of the (precursor) emissions. The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversity for these two species was caused by few outliers. The experiment also indicated that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences. These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters) in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies

An AeroCom initial assessment – optical properties in aerosol component modules of global models

The AeroCom exercise diagnoses multi-component aerosol modules in global modeling. In an initial assessment simulated global distributions for mass and mid-visible aerosol optical thickness (aot) were compared among 20 different modules. Model diversity was also explored in the context of previous comparisons. For the component combined aot general agreement has improved for the annual global mean. At 0.11 to 0.14, simulated aot values are at the lower end of global averages suggested by remote sensing from ground (AERONET ca. 0.135) and space (satellite composite ca. 0.15). More detailed comparisons, however, reveal that larger differences in regional distribution and significant differences in compositional mixture remain. Of particular concern are large model diversities for contributions by dust and carbonaceous aerosol, because they lead to significant uncertainty in aerosol absorption (aab). Since aot and aab, both, influence the aerosol impact on the radiative energy-balance, the aerosol (direct) forcing uncertainty in modeling is larger than differences in aot might suggest. New diagnostic approaches are proposed to trace model differences in terms of aerosol processing and transport: These include the prescription of common input (e.g. amount, size and injection of aerosol component emissions) and the use of observational capabilities from ground (e.g. measurements networks) or space (e.g. correlations between aerosol and clouds)