F. M. O'Connor

Prolonged stratospheric ozone loss in the 1995–96 Arctic winter

It is well established that extensive depletion of ozone, initiated by heterogenous reactions on polar stratospheric clouds (PSCs) can occur in both the Arctic and Antarctic lower stratosphere. Moreover, it has been shown that ozone loss rates in the Arctic region in recent years reached values comparable to those over the Antarctic,. But until now the accumulated ozone losses over the Arctic have been the smaller, mainly because the period of Arctic ozone loss has not—unlike over the Antarctic—persisted well into springtime. Here we report the occurrence—during the unusually cold 1995–96 Arctic winter—of the highest recorded chemical ozone loss over the Arctic region. Two new kinds of behaviour were observed. First, ozone loss at some altitudes was observed long after the last exposure to PSCs. This continued loss appears to be due to a removal of the nitrogen species that slow down chemical ozone depletion. Second, in another altitude range ozone loss rates decreased while PSCs were still present, apparently because of an early transformation of the ozone-destroying chlorine species into less active chlorinenitrate. The balance between these two counteracting mechanisms is probably a fine one, determined by small differences in wintertime stratospheric temperatures. If the apparent cooling trend in the Arctic stratosphere is real, more dramatic ozone losses may occur in the future.

Possible role of wetlands, permafrost, and methane hydrates in the methane cycle under future climate change: A review

We have reviewed the available scientific literature on how natural sources and the atmospheric fate of methane may be affected by future climate change. We discuss how processes governing methane wetland emissions, permafrost thawing, and destabilization of marine hydrates may affect the climate system. It is likely that methane wetland emissions will increase over the next century. Uncertainties arise from the temperature dependence of emissions and changes in the geographical distribution of wetland areas. Another major concern is the possible degradation or thaw of terrestrial permafrost due to climate change. The amount of carbon stored in permafrost, the rate at which it will thaw, and the ratio of methane to carbon dioxide emissions upon decomposition form the main uncertainties. Large amounts of methane are also stored in marine hydrates, and they could be responsible for large emissions in the future. The time scales for destabilization of marine hydrates are not well understood and are likely to be very long for hydrates found in deep sediments but much shorter for hydrates below shallow waters, such as in the Arctic Ocean. Uncertainties are dominated by the sizes and locations of the methane hydrate inventories, the time scales associated with heat penetration in the ocean and sediments, and the fate of methane released in the seawater. Overall, uncertainties are large, and it is difficult to be conclusive about the time scales and magnitudes of methane feedbacks, but significant increases in methane emissions are likely, and catastrophic emissions cannot be ruled out. We also identify gaps in our scientific knowledge and make recommendations for future research and development in the context of Earth system modeling.

Arctic Ozone Loss in Threshold Conditions: Match Observations in 1997/1998 and 1998/1999

Chemical ozone loss rates inside the Arctic polar vortex were determined in early 1998 and early 1999 by using the Match technique based on coordinated ozonesonde measurements. These two winters provide the only opportunities in recent years to investigate chemical ozone loss in a warm Arctic vortex under threshold conditions, i.e., where the preconditions for chlorine activation, and hence ozone destruction, only occurred occasionally. In 1998, results were obtained in January and February between 410 and 520 K. The overall ozone loss was observed to be largely insignificant, with the exception of late February, when those air parcels exposed to temperatures below 195 K were affected by chemical ozone loss. In 1999, results are confined to the 475 K isentropic level, where no significant ozone loss was observed. Average temperatures were some 8°–10° higher than those in 1995, 1996, and 1997, when substantial chemical ozone loss occurred. The results underline the strong dependence of the chemical ozone loss on the stratospheric temperatures. This study shows that enhanced chlorine alone does not provide a sufficient condition for ozone loss. The evolution of stratospheric temperatures over the next decade will be the determining factor for the amount of wintertime chemical ozone loss in the Arctic stratosphere.

The World Avoided by the Montreal Protocol

[1] The impact of increased stratospheric chlorine, averted by controls imposed by the Montreal Protocol, is studied using the UKCA chemistry-climate model. We contrast an atmosphere with 9 ppbv Cly, which could have occurred by 2030, with the present-day loading (3.5 ppbv), and consider the response of climate to resulting ozone perturbations, disregarding the radiative impact of the additional CFCs. Ozone columns decline everywhere, with climate impacts in both polar regions. The additional chlorine leads to a strengthening of the Southern Annular Mode, versus the reference, and Antarctic surface temperature differences resemble observed changes. Over Eurasia, winter surface temperature changes project on the Northern Annular Mode. These high-latitude temperature perturbations (>1 K) are larger than the global mean temperature rises projected over the next few decades, and perhaps comparable with projected regional changes. The Montreal Protocol has not only averted further damage to the ozone layer but has helped prevent significant regional climate change. Citation: Morgenstern, O., P. Braesicke, M. M. Hurwitz, F. M. O’Connor, A. C. Bushell, C. E. Johnson, and J. A. Pyle (2008), The World Avoided by the Montreal Protocol, Geophys. Res. Lett., 35, L16811, doi:10.1029/2008GL034590.

Forest fire plumes over the North Atlantic: p‐TOMCAT model simulations with aircraft and satellite measurements from the ITOP/ICARTT campaign

[1] Intercontinental Transport of Ozone and Precursors (ITOP) (part of International Consortium for Atmospheric Research on Transport and Transformation (ICARTT)) was an intense research effort to measure long-range transport of pollution across the North Atlantic and its impact on O3 production. During the aircraft campaign plumes were encountered containing large concentrations of CO plus other tracers and aerosols from forest fires in Alaska and Canada. A chemical transport model, p-TOMCAT, and new biomass burning emissions inventories are used to study the emissions long-range transport and their impact on the troposphere O3 budget. The fire plume structure is modeled well over long distances until it encounters convection over Europe. The CO values within the simulated plumes closely match aircraft measurements near North America and over the Atlantic and have good agreement with MOPITT CO data. O3 and NOx values were initially too great in the model plumes. However, by including additional vertical mixing of O3 above the fires, and using a lower NO2/CO emission ratio (0.008) for boreal fires, O3 concentrations are reduced closer to aircraft measurements, with NO2 closer to SCIAMACHY data. Too little PAN is produced within the simulated plumes, and our VOC scheme’s simplicity may be another reason for O3 and NOx modeldata discrepancies. In the p-TOMCAT simulations the fire emissions lead to increased tropospheric O3 over North America, the north Atlantic and western Europe from photochemical production and transport. The increased O3 over the Northern Hemisphere in the simulations reaches a peak in July 2004 in the range 2.0 to 6.2 Tg over a baseline of about 150 Tg.

A review of recent developments in climate change science. Part I: Understanding of future change in the large-scale climate system:

This article reviews some of the major lines of recent scientific progress relevant to the choice of global climate policy targets, focusing on changes in understanding since publication of the Intergovernmental Panel on Climate Change Fourth Assessment Report (IPCC AR4). Developments are highlighted in the following major climate system components: ice sheets; sea ice; the Atlantic Meridional Overturning Circulation; tropical forests; and accelerated carbon release from permafrost and ocean hydrates. The most significant developments in each component are identified by synthesizing input from multiple experts from each field. Overall, while large uncertainties remain in all fields, some substantial progress in understanding is revealed.

Understanding the glacial methane cycle

Atmospheric methane (CH4) varied with climate during the Quaternary, rising from a concentration of 375 p.p.b.v. during the last glacial maximum (LGM) 21,000 years ago, to 680 p.p.b.v. at the beginning of the industrial revolution. However, the causes of this increase remain unclear; proposed hypotheses rely on fluctuations in either the magnitude of CH4 sources or CH4 atmospheric lifetime, or both. Here we use an Earth System model to provide a comprehensive assessment of these competing hypotheses, including estimates of uncertainty. We show that in this model, the global LGM CH4 source was reduced by 28–46%, and the lifetime increased by 2–8%, with a best-estimate LGM CH4 concentration of 463–480 p.p.b.v. Simulating the observed LGM concentration requires a 46–49% reduction in sources, indicating that we cannot reconcile the observed amplitude. This highlights the need for better understanding of the effects of low CO2 and cooler climate on wetlands and other natural CH4 sources.

Revisiting the Mystery of Recent Stratospheric Temperature Trends

Simulated stratospheric temperatures over the period 1979-2016 in models from the Chemistry-Climate Model Initiative (CCMI) are compared with recently updated and extended satellite observations. The multi-model mean global temperature trends over 1979- 2005 are -0.88 ± 0.23, -0.70 ± 0.16, and -0.50 ± 0.12 K decade-1 for the Stratospheric Sounding Unit (SSU) channels 3 (~40-50 km), 2 (~35-45 km), and 1 (~25-35 km), respectively. These are within the uncertainty bounds of the observed temperature trends from two reprocessed satellite datasets. In the lower stratosphere, the multi-model mean trend in global temperature for the Microwave Sounding Unit channel 4 (~13-22 km) is -0.25 ± 0.12 K decade-1 over 1979-2005, consistent with estimates from three versions of this satellite record. The simulated stratospheric temperature trends in CCMI models over 1979-2005 agree with the previous generation of chemistry-climate models. The models and an extended satellite dataset of SSU with the Advanced Microwave Sounding Unit-A show weaker global stratospheric cooling over 1998-2016 compared to the period of intensive ozone depletion (1979-1997). This is due to the reduction in ozone-induced cooling from the slow-down of ozone trends and the onset of ozone recovery since the late 1990s. In summary, the results show much better consistency between simulated and satellite observed stratospheric temperature trends than was reported by Thompson et al. (2012) for the previous versions of the SSU record and chemistry-climate models. The improved agreement mainly comes from updates to the satellite records; the range of simulated trends is comparable to the previous generation of models.

Fast sensitivity analysis methods for computationally expensive models with multidimensional output

Global sensitivity analysis (GSA) is a powerful approach in identifying which inputs or parameters most affect a model’s output. This determines which inputs to include when performing model calibration or uncertainty analysis. GSA allows quantification of the sensitivity index (SI) of a particular input – the percentage of the total variability in the output attributed to the changes in that input – by averaging over the other inputs rather than fixing them at specific values. Traditional methods of computing the SIs using the Sobol and extended Fourier Amplitude Sensitivity Test (eFAST) methods involve running a model thousands of times, but this may not be feasible for computationally expensive Earth system models. GSA methods that use a statistical emulator in place of the expensive model are popular, as they require far fewer model runs. We performed an eight-input GSA, using the Sobol and eFAST methods, on two computationally expensive atmospheric chemical transport models using emulators that were trained with 80 runs of the models. We considered two methods to further reduce the computational cost of GSA: (1) a dimension reduction approach and (2) an emulator-free approach. When the output of a model is multi-dimensional, it is common practice to build a separate emulator for each dimension of the output space. Here, we used principal component analysis (PCA) to reduce the output dimension, built an emulator for each of the transformed outputs, and then computed SIs of the reconstructed output using the Sobol method. We considered the global distribution of the annual column mean lifetime of atmospheric methane, which requires ∼ 2000 emulators without PCA but only 5–40 emulators with PCA. We also applied an emulator-free method using a generalised additive model (GAM) to estimate the SIs using only the training runs. Compared to the emulator-only methods, the emulator– PCA and GAM methods accurately estimated the SIs of the ∼ 2000 methane lifetime outputs but were on average 24 and 37 times faster, respectively.

Forest fire plumes over the North Atlantic: p-TOMCAT model simulations with aircraft and satellite measurements from the ITOP/ICARTT campaign

[1] Intercontinental Transport of Ozone and Precursors (ITOP) (part of International Consortium for Atmospheric Research on Transport and Transformation (ICARTT)) was an intense research effort to measure long-range transport of pollution across the North Atlantic and its impact on O3 production. During the aircraft campaign plumes were encountered containing large concentrations of CO plus other tracers and aerosols from forest fires in Alaska and Canada. A chemical transport model, p-TOMCAT, and new biomass burning emissions inventories are used to study the emissions long-range transport and their impact on the troposphere O3 budget. The fire plume structure is modeled well over long distances until it encounters convection over Europe. The CO values within the simulated plumes closely match aircraft measurements near North America and over the Atlantic and have good agreement with MOPITT CO data. O3 and NOx values were initially too great in the model plumes. However, by including additional vertical mixing of O3 above the fires, and using a lower NO2/CO emission ratio (0.008) for boreal fires, O3 concentrations are reduced closer to aircraft measurements, with NO2 closer to SCIAMACHY data. Too little PAN is produced within the simulated plumes, and our VOC scheme’s simplicity may be another reason for O3 and NOx modeldata discrepancies. In the p-TOMCAT simulations the fire emissions lead to increased tropospheric O3 over North America, the north Atlantic and western Europe from photochemical production and transport. The increased O3 over the Northern Hemisphere in the simulations reaches a peak in July 2004 in the range 2.0 to 6.2 Tg over a baseline of about 150 Tg.