Arctic Ozone Depletion in 2019/20: Roles of Chemistry, Dynamics And the Montreal Protocol
No abstract provided
Chipperfield, Martyn P.↗
Engineering topics
Chipperfield, Martyn P.
Publications and source records attributed to Chipperfield, Martyn P..
Tropospheric Jet Response to Antarctic Ozone Depletion: An Update with Chemistry-Climate Model Initiative (CCMI) Models
The Southern Hemisphere (SH) zonal-mean circulation change in response to Antarctic ozone depletion is re-visited by examining a set of the latest model simulations archived for the Chemistry-Climate Model Initiative (CCMI) project. All models reasonably well reproduce Antarctic ozone depletion in the late 20th century. The related SH-summer circulation changes, such as a poleward intensification of westerly jet and a poleward expansion of the Hadley cell, are also well captured. All experiments exhibit quantitatively the same multi-model mean trend, irrespective of whether the ocean is coupled or prescribed. Results are also quantitatively similar to those derived from the Coupled Model Intercomparison Project phase 5 (CMIP5) high-top model simulations in which the stratospheric ozone is mostly prescribed with monthly- and zonally-averaged values. These results suggest that the ozone-hole-induced SH-summer circulation changes are robust across the models irrespective of the specific chemistry-atmosphere-ocean coupling.
chemistry-climate models↗
Ozone Sensitivity to Varying Greenhouse Gases and Ozone-Depleting Substances in CCMI-1 Simulations
Ozone fields simulated for the first phase of the Chemistry-Climate Model Initiative (CCMI-1) will be used as forcing data in the 6th Coupled Model Intercomparison Project. Here we assess, using reference and sensitivity simulations produced for CCMI-1, the suitability of CCMI-1 model results for this process, investigating the degree of consistency amongst models regarding their responses to variations in individual forcings. We consider the influences of methane, nitrous oxide, a combination of chlorinated or brominated ozone-depleting substances, and a combination of carbon dioxide and other greenhouse gases. We find varying degrees of consistency in the models' responses in ozone to these individual forcings, including some considerable disagreement. In particular, the response of total-column ozone to these forcings is less consistent across the multi-model ensemble than profile comparisons. We analyse how stratospheric age of air, a commonly used diagnostic of stratospheric transport, responds to the forcings. For this diagnostic we find some salient differences in model behaviour, which may explain some of the findings for ozone. The findings imply that the ozone fields derived from CCMI-1 are subject to considerable uncertainties regarding the impacts of these anthropogenic forcings. We offer some thoughts on how to best approach the problem of generating a consensus ozone database from a multi-model ensemble such as CCMI-1.
CCMI↗
Deriving Global OH Abundance and Atmospheric Lifetimes for Long-Lived Gases: A Search for CH3CCl3 Alternatives
An accurate estimate of global hydroxyl radical (OH) abundance is important for projections of air quality, climate, and stratospheric ozone recovery. As the atmospheric mixing ratios of methyl chloroform (CH3CCl3) (MCF), the commonly used OH reference gas, approaches zero, it is important to find alternative approaches to infer atmospheric OH abundance and variability. The lack of global bottom-up emission inventories is the primary obstacle in choosing a MCF alternative. We illustrate that global emissions of long-lived trace gases can be inferred from their observed mixing ratio differences between the Northern Hemisphere (NH) and Southern Hemisphere (SH), given realistic estimates of their NH-SH exchange time, the emission partitioning between the two hemispheres, and the NH versus SH OH abundance ratio. Using the observed long-term trend and emissions derived from the measured hemispheric gradient, the combination of HFC-32 (CH2F2), HFC-134a (CH2FCF3, HFC-152a (CH3CHF2), and HCFC-22 (CHClF2), instead of a single gas, will be useful as a MCF alternative to infer global and hemispheric OH abundance and trace gas lifetimes. The primary assumption on which this multispecies approach relies is that the OH lifetimes can be estimated by scaling the thermal reaction rates of a reference gas at 272 K on global and hemispheric scales. Thus, the derived hemispheric and global OH estimates are forced to reconcile the observed trends and gradient for all four compounds simultaneously. However, currently, observations of these gases from the surface networks do not provide more accurate OH abundance estimate than that from MCF.
Lifetime↗
Review of the Global Models Used Within Phase 1 of the Chemistry-Climate Model Initiative (CCMI)
We present an overview of state-of-the-art chemistry-climate and chemistry transport models that are used within phase 1 of the Chemistry-Climate Model Initiative (CCMI-1). The CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, tropospheric composition, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI-1 recommendations for simulations have been followed is necessary to understand model responses to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI-1 simulations with the aim of informing CCMI data users.
CCMI↗
Quantifying the Causes of Differences in Tropospheric OH Within Global Models
The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (Tau CH4) between these models. Annual average Tau CH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in Tau CH4 (Delta Tau CH4) result from variations in chemical mechanisms (Delta Tau CH4 = 0.46 years), the photolysis frequency (J) of O3 yields O(D-1) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The Delta Tau CH4 due to CTM differences in NO(x) (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NO(x). Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.
Surface Measurements and Models↗
Model Sensitivity Studies of the Decrease in Atmospheric Carbon Tetrachloride
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(exp -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(exp -1). Further progress in constraining the CCl4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the National Oceanic and Atmospheric Administration (NOAA) network are larger than from the Advanced Global Atmospheric Gases Experiment (AGAGE) network but have shown a steeper decreasing trend over the past 2 decades. These differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl4 sinks.
Carbon Trechloride↗
A Global Atmospheric Model of Meteoric Iron
The first global model of meteoric iron in the atmosphere (WACCM-Fe) has been developed by combining three components: the Whole Atmosphere Community Climate Model (WACCM), a description of the neutral and ion-molecule chemistry of iron in the mesosphere and lower thermosphere (MLT), and a treatment of the injection of meteoric constituents into the atmosphere. The iron chemistry treats seven neutral and four ionized iron containing species with 30 neutral and ion-molecule reactions. The meteoric input function (MIF), which describes the injection of Fe as a function of height, latitude, and day, is precalculated from an astronomical model coupled to a chemical meteoric ablation model (CABMOD). This newly developed WACCM-Fe model has been evaluated against a number of available ground-based lidar observations and performs well in simulating the mesospheric atomic Fe layer. The model reproduces the strong positive correlation of temperature and Fe density around the Fe layer peak and the large anticorrelation around 100 km. The diurnal tide has a significant effect in the middle of the layer, and the model also captures well the observed seasonal variations. However, the model overestimates the peak Fe+ concentration compared with the limited rocket-borne mass spectrometer data available, although good agreement on the ion layer underside can be obtained by adjusting the rate coefficients for dissociative recombination of Fe-molecular ions with electrons. Sensitivity experiments with the same chemistry in a 1-D model are used to highlight significant remaining uncertainties in reaction rate coefficients, and to explore the dependence of the total Fe abundance on the MIF and rate of vertical transport.
meteoric inputfunction↗
A Model Study of the Impact of Magnetic Field Reversal on Atmospheric Composition during Solar Proton Events
During a polarity transition of the Earth's magnetic field, the structure and strength of the field change significantly from their present values. This will alter the global pattern of charged particle precipitation into the atmosphere. Thus, particle precipitation is possible into regions that are at the moment effectively shielded by the Earth's magnetic field. A two-dimensional global fbHy coupled chemistry, radiation, and transport model of the atmosphere has been used to investigate how the increased particle precipitation affects the chemical composition of the middle and lower atmosphere. Ozone losses resulting from large energetic particle events are found to increase significantly, with resultant losses similar to those observed m the Antarctic ozone hole of the 1990s. This results in significant increases in surface UV-B radiation as well as changes in stratospheric temperature and circulation over a period of several months after large particle events.
Sinnhuber, Miaiam↗