Fiona Tummon

Multimodel estimates of atmospheric lifetimes of long‐lived ozone‐depleting substances: Present and future

We have diagnosed the lifetimes of long-lived source gases emitted at the surface and removed in the stratosphere using six three-dimensional chemistry-climate models and a two-dimensional model. The models all used the same standard photochemical data. We investigate the effect of different definitions of lifetimes, including running the models with both mixing ratio (MBC) and flux (FBC) boundary conditions. Within the same model, the lifetimes diagnosed by different methods agree very well. Using FBCs versus MBCs leads to a different tracer burden as the implied lifetime contained in the MBC value does not necessarily match a models own calculated lifetime. In general, there are much larger differences in the lifetimes calculated by different models, the main causes of which are variations in the modeled rates of ascent and horizontal mixing in the tropical midlower stratosphere. The model runs have been used to compute instantaneous and steady state lifetimes. For chlorofluorocarbons (CFCs) their atmospheric distribution was far from steady state in their growth phase through to the 1980s, and the diagnosed instantaneous lifetime is accordingly much longer. Following the cessation of emissions, the resulting decay of CFCs is much closer to steady state. For 2100 conditions the model circulation speeds generally increase, but a thicker ozone layer due to recovery and climate change reduces photolysis rates. These effects compensate so the net impact on modeled lifetimes is small. For future assessments of stratospheric ozone, use of FBCs would allow a consistent balance between rate of CFC removal and model circulation rate.

High solar cycle spectral variations inconsistent with stratospheric ozone observations

Variability in solar UV radiation is uncertain, but it affects Earth’s climate. Simulations of the ozone response to various data sets of spectral solar irradiance show that high-amplitude solar variability is inconsistent with ozone observations.

Attribution of extreme weather to anthropogenic greenhouse gas emissions: Sensitivity to spatial and temporal scales

Recent studies have examined the anthropogenic contribution to specific extreme weather events, such as the European (2003) and Russian (2010) heat waves. While these targeted studies examine the attributable risk of an event occurring over a specified temporal and spatial domain, it is unclear how effectively their attribution statements can serve as a proxy for similar events occurring at different temporal and spatial scales. Here we test the sensitivity of attribution results to the temporal and spatial scales of extreme precipitation and temperature events by applying a probabilistic event attribution framework to the output of two global climate models, each run with and without anthropogenic greenhouse gas emissions. Attributable risk tends to be more sensitive to the temporal than spatial scale of the event, increasing as event duration increases. Globally, correlations between attribution statements at different spatial scales are very strong for temperature extremes and moderate for heavy precipitation extremes.

The changing ozone depletion potential of N2O in a future climate

Nitrous oxide (N2O), which decomposes in the stratosphere to form nitrogen oxides (NOx), is currently the dominant anthropogenic ozone-depleting substance emitted. Ozone depletion potentials (ODPs) of specific compounds, commonly evaluated for present-day conditions, were developed for long-lived halocarbons and are used by policymakers to inform decision-making around protection of the ozone layer. However, the effect of N2O on ozone will evolve in the future due to changes in stratospheric dynamics and chemistry induced by rising levels of greenhouse gases. Despite the fact that NOx-induced ozone loss slows with increasing concentrations of CO2 and CH4, we show that ODPN2O for year 2100 varies under different scenarios and is mostly larger than ODPN2O for year 2000. This occurs because the traditional ODP approach is tied to ozone depletion induced by CFC-11, which is also sensitive to CO2 and CH4. We therefore suggest that a single ODP for N2O is of limited use.

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.

Tropospheric ozone in CCMI models and Gaussian emulation to understand biases in the SOCOLv3 chemistry-climate model

Previous multi-model intercomparisons have shown that chemistry-climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC/IGAC (Stratosphere-troposphere Processes and their Role in Climate/International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40–50% in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb 5 Sounder (OMI/MLS), and a negative bias of up to ∼30% in the Southern Hemisphere. SOCOLv3.0 (version 3 of the SolarClimate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU – approximately 33% larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, “SO1 Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-615 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 26 June 2018 c