Alistair J. Manning

Operational prediction of ash concentrations in the distal volcanic cloud from the 2010 Eyjafjallajökull eruption

[1] During the 2010 eruption of Eyjafjallajokull, improvements were made to the modeling procedure at the Met Office, UK, enabling peak ash concentrations within the volcanic cloud to be estimated. In this paper we describe the ash concentration forecasting method, its rationale and how it evolved over time in response to new information and user requirements. The change from solely forecasting regions of ash to also estimating peak ash concentrations required consideration of volcanic ash emission rates, the fraction of ash surviving near-source fall-out, and the relationship between predicted mean and local peak ash concentrations unresolved by the model. To validate the modeling procedure, predicted peak ash concentrations are compared against observations obtained by ground-based and research aircraft instrumentation. This comparison between modeled and observed peak concentrations highlights the many sources of error and the uncertainties involved. Despite the challenges of predicting ash concentrations, the ash forecasting method employed here is found to give useful guidance on likely ash concentrations. Predicted peak ash concentrations lie within about one and a half orders of magnitude of the observed peak concentrations. A significant improvement in the agreement between modeled and observed values is seen if a buffer zone, accounting for positional errors in the predicted ash cloud, is used. Sensitivity of the predicted ash concentrations to the source properties (e.g., the plume height and the vertical distribution of ash at the source) is assessed and in some cases, seemingly minor uncertainties in the source specification have a large effect on predicted ash concentrations.

Global trends, seasonal cycles and European emissions of dichloromethane, trichloroethene and tetrachloroethene from the AGAGE observations at Mace Head, Ireland and Cape Grim, Tasmania

[1] In situ observations (every 4 hours) of dichloromethane (CH 2 Cl 2 ) from April 1995 to December 2004 and trichloroethene (C 2 HCl 3 ) and tetrachloroethene (C 2 Cl 4 ) from September 2000 to December 2004 are reported for the Advanced Global Atmospheric Gases Experiment (AGAGE) station at Mace Head, Ireland. At a second AGAGE station at Cape Grim, Tasmania, CH 2 Cl 2 and C 2 Cl 4 data collection commenced in 1998 and 2000, respectively. C 2 HCl 3 is below the limit of detection at Cape Grim except during pollution episodes. At Mace Head CH 2 Cl 2 shows a downward trend from 1995 to 2004 of 0.7±0.2 ppt yr -1 (ppt: expressed as dry mole fractions in 10 12 ), although from 1998 to 2004 the decrease has been only 0.3 ± 0.1ppt yr -1 . Conversely, there has been a small but significant growth of 0.05 ± 0.01 ppt yr -1 in CH 2 Cl 2 at Cape Grim. The time series for C 2 HCl 3 and C 2 Cl 4 are relatively short for accurate trend analyses; however, we observe a small but significant decline in C 2 Cl 4 (0.18 ± 0.05 ppt yr -1 ) at Mace Head. European emissions inferred from AGAGE measurements are compared to recent estimates from industry data and show general agreement for C 2 HCl 3 . Emissions estimated from observations are lower than industry emission estimates for C 2 Cl 4 and much lower in the case of CH 2 Cl 2 . A study of wildfires in Tasmania, uncontaminated by urban emissions, suggests that the biomass burning source of CH 2 Cl 2 may have been previously overestimated. All three solvents have distinct annual cycles, with the phases and amplitudes reflecting their different chemical reactivity with OH as the primary sink.

Estimating source regions of European emissions of trace gases from observations at Mace Head

Abstract A technique is described for identifying probable source locations for a range of greenhouse and ozone-depleting trace gases from the long-term measurements made at Mace Head, Ireland. The Met. Offices dispersion model NAME is used to predict concentrations at Mace Head from all possible sources in Europe, then source regions identified as those which consistently lead to elevated concentrations at Mace Head. Estimates of European emissions and their distribution are presented for a number of trace gases for the period 1995–1998. Estimated emission patterns are realistic, given the nature and varied applications of the species considered. The results indicate that whilst there are limitations, useful information about source distribution can be extracted from continuous measurements at a remote site. It is probable that much improved estimates could be derived if observations were available from a number of sites. The ability to assess emissions has obvious implications in monitoring compliance with internationally agreed quota and protocols.

Low European methyl chloroform emissions inferred from long-term atmospheric measurements

Methyl chloroform (CH3CCl3, 1,1,1,-trichloroethane) was used widely as a solvent before it was recognized to be an ozone-depleting substance and its phase-out was introduced under the Montreal Protocol. Subsequently, its atmospheric concentration has declined steadily and recent European methyl chloroform consumption and emissions were estimated to be less than 0.1 gigagrams per year. However, data from a short-term tropospheric measurement campaign (EXPORT) indicated that European methyl chloroform emissions could have been over 20 gigagrams in 2000 (ref. 6), almost doubling previously estimated global emissions. Such enhanced emissions would significantly affect results from the CH3CC13 method of deriving global abundances of hydroxyl radicals (OH) (refs 7–12)—the dominant reactive atmospheric chemical for removing trace gases related to air pollution, ozone depletion and the greenhouse effect. Here we use long-term, high-frequency data from Mace Head, Ireland and Jungfraujoch, Switzerland, to infer European methyl chloroform emissions. We find that European emission estimates declined from about 60 gigagrams per year in the mid-1990s to 0.3–1.4 and 1.9–3.4 gigagrams per year in 2000–03, based on Mace Head and Jungfraujoch data, respectively. Our European methyl chloroform emission estimates are therefore higher than calculated from consumption data, but are considerably lower than those derived from the EXPORT campaign in 2000 (ref. 6).

The origin of high particulate concentrations over the United Kingdom, March 2000

Abstract An episode of exceptionally high PM10 and PM2.5 levels was observed during the night of the 2–3 March 2000 throughout England and Wales. The weather was characterised by strong westerly winds and widespread rainfall associated with a low pressure system to the north of Scotland, conditions usually associated with relatively clean, unpolluted air. Possible sources included volcanic ash from an eruption on 26 February 2000 in Iceland, or dust from large sandstorms over the Sahara. A combination of atmospheric transport modelling using the Lagrangian dispersion model NAME, an analyses of satellite imagery and observational data from Mace Head has shown that the most likely origin of the episode was long range transport of dust from the Sahara region of North Africa. Further modelling studies have revealed a number of previously unidentified dust episodes, and indicate that transport of dust from the Sahara can occur several times a year. Dust episodes are of interest for a number of reasons, particulate levels can be elevated over a wide area and in some instances can significantly exceeded current air quality standards. If a natural source is identified over which there can be no control, there are implications for the setting of air quality standards.

Role of atmospheric oxidation in recent methane growth

Significance Methane, the second most important greenhouse gas, has varied markedly in its atmospheric growth rate. The cause of these fluctuations remains poorly understood. Recent efforts to determine the drivers of the pause in growth in 1999 and renewed growth from 2007 onward have focused primarily on changes in sources alone. Here, we show that changes in the major methane sink, the hydroxyl radical, have likely played a substantial role in the global methane growth rate. This work has significant implications for our understanding of the methane budget, which is important if we are to better predict future changes in this potent greenhouse gas and effectively mitigate enhanced radiative forcing caused by anthropogenic emissions. The growth in global methane (CH4) concentration, which had been ongoing since the industrial revolution, stalled around the year 2000 before resuming globally in 2007. We evaluate the role of the hydroxyl radical (OH), the major CH4 sink, in the recent CH4 growth. We also examine the influence of systematic uncertainties in OH concentrations on CH4 emissions inferred from atmospheric observations. We use observations of 1,1,1-trichloroethane (CH3CCl3), which is lost primarily through reaction with OH, to estimate OH levels as well as CH3CC3 emissions, which have uncertainty that previously limited the accuracy of OH estimates. We find a 64–70% probability that a decline in OH has contributed to the post-2007 methane rise. Our median solution suggests that CH4 emissions increased relatively steadily during the late 1990s and early 2000s, after which growth was more modest. This solution obviates the need for a sudden statistically significant change in total CH4 emissions around the year 2007 to explain the atmospheric observations and can explain some of the decline in the atmospheric 13CH4/12CH4 ratio and the recent growth in C2H6. Our approach indicates that significant OH-related uncertainties in the CH4 budget remain, and we find that it is not possible to implicate, with a high degree of confidence, rapid global CH4 emissions changes as the primary driver of recent trends when our inferred OH trends and these uncertainties are considered.

UK emissions of the greenhouse gas nitrous oxide

Signatories of the Kyoto Protocol are obliged to submit annual accounts of their anthropogenic greenhouse gas emissions, which include nitrous oxide (N2O). Emissions from the sectors industry (3.8 Gg), energy (14.4 Gg), agriculture (86.8 Gg), wastewater (4.4 Gg), land use, land-use change and forestry (2.1 Gg) can be calculated by multiplying activity data (i.e. amount of fertilizer applied, animal numbers) with simple emission factors (Tier 1 approach), which are generally applied across wide geographical regions. The agricultural sector is the largest anthropogenic source of N2O in many countries and responsible for 75 per cent of UK N2O emissions. Microbial N2O production in nitrogen-fertilized soils (27.6 Gg), nitrogen-enriched waters (24.2 Gg) and manure storage systems (6.4 Gg) dominate agricultural emission budgets. For the agricultural sector, the Tier 1 emission factor approach is too simplistic to reflect local variations in climate, ecosystems and management, and is unable to take into account some of the mitigation strategies applied. This paper reviews deviations of observed emissions from those calculated using the simple emission factor approach for all anthropogenic sectors, briefly discusses the need to adopt specific emission factors that reflect regional variability in climate, soil type and management, and explains how bottom-up emission inventories can be verified by top-down modelling.

Global environmental impacts of the hydrogen economy

Hydrogen-based energy systems appear to be an attractive proposition in providing a future replacement for the current fossil-fuel based energy systems. Hydrogen is an important, though little studied, trace component of the atmosphere. It is present at the mixing ratio of about 510 ppb currently and has important man-made and natural sources. Because hydrogen reacts with tropospheric hydroxyl radicals, emissions of hydrogen to the atmosphere perturb the distributions of methane and ozone, the second and third most important greenhouse gases after carbon dioxide. Hydrogen is therefore an indirect greenhouse gas with a global warming potential GWP of 5.8 over a 100-year time horizon. A future hydrogen economy would therefore have greenhouse consequences and would not be free from climate perturbations. If a global hydrogen economy replaced the current fossil fuel-based energy system and exhibited a leakage rate of 1%, then it would produce a climate impact of 0.6% of the current fossil fuel based system. Careful attention must be given to reduce to a minimum the leakage of hydrogen from the synthesis, storage and use of hydrogen in a future global hydrogen economy if the full climate benefits are to be realised.

European emissions of halogenated greenhouse gases inferred from atmospheric measurements.

European emissions of nine representative halocarbons (CFC-11, CFC-12, Halon 1211, HCFC-141b, HCFC-142b, HCFC-22, HFC-125, HFC-134a, HFC-152a) are derived for the year 2009 by combining long-term observations in Switzerland, Italy, and Ireland with campaign measurements from Hungary. For the first time, halocarbon emissions over Eastern Europe are assessed by top-down methods, and these results are compared to Western European emissions. The employed inversion method builds on least-squares optimization linking atmospheric observations with calculations from the Lagrangian particle dispersion model FLEXPART. The aggregated halocarbon emissions over the study area are estimated at 125 (106-150) Tg of CO(2) equiv/y, of which the hydrofluorocarbons (HFCs) make up the most important fraction with 41% (31-52%). We find that chlorofluorocarbon (CFC) emissions from banks are still significant and account for 35% (27-43%) of total halocarbon emissions in Europe. The regional differences in per capita emissions are only small for the HFCs, while emissions of CFCs and hydrochlorofluorocarbons (HCFCs) tend to be higher in Western Europe compared to Eastern Europe. In total, the inferred per capita emissions are similar to estimates for China, but 3.5 (2.3-4.5) times lower than for the United States. Our study demonstrates the large benefits of adding a strategically well placed measurement site to the existing European observation network of halocarbons, as it extends the coverage of the inversion domain toward Eastern Europe and helps to better constrain the emissions over Central Europe.

Reconciling reported and unreported HFC emissions with atmospheric observations

Significance Hydrofluorocarbons (HFCs) are among the atmosphere’s fastest growing, and most potent, greenhouse gases. Proposals have been made to phase down their use over the coming decades. Such initiatives may largely be informed by existing emissions inventories, which, we show, are the subject of significant uncertainty. In this work, we use atmospheric models and measurements to examine the accuracy of these inventories for five major HFCs. We show that, when aggregated together, reported emissions of these HFCs from developed countries are consistent with the atmospheric measurements, and almost half of global emissions now originate from nonreporting countries. However, the agreement between our results and the inventory breaks down for individual HFC emissions, suggesting inaccuracies in the reporting methods for individual compounds. We infer global and regional emissions of five of the most abundant hydrofluorocarbons (HFCs) using atmospheric measurements from the Advanced Global Atmospheric Gases Experiment and the National Institute for Environmental Studies, Japan, networks. We find that the total CO2-equivalent emissions of the five HFCs from countries that are required to provide detailed, annual reports to the United Nations Framework Convention on Climate Change (UNFCCC) increased from 198 (175–221) Tg-CO2-eq⋅y–1 in 2007 to 275 (246–304) Tg-CO2-eq⋅y–1 in 2012. These global warming potential-weighted aggregated emissions agree well with those reported to the UNFCCC throughout this period and indicate that the gap between reported emissions and global HFC emissions derived from atmospheric trends is almost entirely due to emissions from nonreporting countries. However, our measurement-based estimates of individual HFC species suggest that emissions, from reporting countries, of the most abundant HFC, HFC-134a, were only 79% (63–95%) of the UNFCCC inventory total, while other HFC emissions were significantly greater than the reported values. These results suggest that there are inaccuracies in the reporting methods for individual HFCs, which appear to cancel when aggregated together.