Db Ryall

Validation of the UK Met. Office’s name model against the ETEX dataset

Abstract The ETEX 1 data set has been used to assess the performance of the UK Met Office’s long-range dispersion model NAME. In terms of emergency response modelling the model performed well, successfully predicting the overall spread and timing of the plume across Europe. However, in common with most other models, NAME overpredicted the observed concentrations. This is in contrast with other NAME validation studies which indicate either no significant bias or a tendency to underpredict concentrations. This suggests the reasons for overpredicting are specific to the ETEX situation. Explanations include inadequate vertical diffusion or transport, possible venting by convective activity, and experimental errors. An assessment of a range of advection schemes of varying complexity indicated no clear advantage, at present, in using more sophisticated random walk techniques at long range, a simple diffusion coefficient based scheme providing some of the best results. A brief look is also taken at a simulation of the more problematical ETEX 2 release.

In situ chloroform measurements at Advanced Global Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998

Measurements of atmospheric chloroform (CHCl3) by in situ gas chromatography using electron capture detection are reported from the Advanced Global Atmospheric Gases Experiment (AGAGE) network of atmospheric research stations. They are some of the most comprehensive in situ, high-frequency measurements to be reported for CHCl3 and provide valuable information not only on clean “baseline” mixing ratios but also on local and regional sources. Emissions from these sources cause substantial periodic increases in CHCl3 concentrations above their baseline levels, which can be used to identify source strengths. This is particularly the case for measurements made at Mace Head, Ireland. Furthermore, these local sources of CHCl3 emissions are significant in relation to current estimates of global emissions and illustrate that the understanding of competing sources and sinks of CHCl3 is still fragmentary. These observations also show that CHCl3 has a very pronounced seasonal cycle with a summer minimum and winter maximum presumably resulting from enhanced destruction by OH in the summer. The amplitude of the cycle is dependent on sampling location. Over the 57 months of in situ measurements a global average baseline concentration of 8.9±0.1 ppt was determined with no appreciable trend in the baseline detected.

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.

Continuous high-frequency observations of hydrogen at the Mace Head baseline atmospheric monitoring station over the 1994–1998 period

Continuous high-frequency (every 40-min) automatic measurements of hydrogen have been made at the Mace Head atmospheric research station on the Atlantic Ocean coast of Ireland throughout 1994–1998. These observations represent one the most comprehensive in situ records of a trace gas that has received comparatively little attention. Individual measurements have been sorted by four independent methods to separate clean, maritime air masses from regionally polluted European air masses. Hydrogen concentrations in midlatitude Northern Hemisphere baseline air show a distinct seasonal cycle with highest concentrations during spring and lowest concentrations during late autumn, with a peak-to-trough amplitude of 38±6 ppb, averaged over the observed seasonal cycles from 1994 to 1998. The mean hydrogen concentration in midlatitude Northern Hemisphere baseline air on January 1, 1995, was estimated as 496.5 ppb with an upward trend of 1.2±0.8 ppb yr−1. Evidence has also been obtained for European pollution sources with source strength of about 0.8 Tg yr−1 and for deposition of hydrogen to soils. The observation of slightly elevated hydrogen concentrations relative to baseline levels in tropical maritime air masses points to a latitudinal gradient in hydrogen with higher concentrations in lower latitudes of the Northern Hemisphere and in the Southern Hemisphere. This is confirmed by comparable hydrogen observations at Cape Grim, Tasmania, which are consistently higher than measurements recorded at Mace Head. Mean hemispheric concentrations of 504 and 520 ppb have been estimated for the Northern and Southern Hemispheres, respectively, for January 1, 1996, corresponding to a total atmospheric hydrogen burden of 182 Tg.

The impact of the Montreal protocol on halocarbon concentrations in northern hemisphere baseline and European air masses at Mace Head, Ireland over a ten year period from 1987-1996

Abstract The international concern following the discovery of Antarctic stratospheric ozone depletion has prompted unprecedented international action by governments to control the production, sales and usage of a range of ozone-depleting chemicals. These international treaty obligations include the Montreal Protocol and its London and Copenhagen Amendments. They address, amongst many halocarbon species, the chlorofluorocarbons: CFC-11, -12 and -113 and the chlorocarbons: carbon tetrachloride and methyl chloroform. These chemicals have been routinely monitored at the remote, baseline monitoring station at Mace Head on the Atlantic Ocean coast of Ireland as part of the GAGE/AGAGE programme. The available monitoring data for the period 1987–1996 are presented here with a view to confirming the extent of compliance with the above Protocols on a global and European basis. Daily wind direction sectors provided by EMEP are used to sort the halocarbon data into northern hemisphere baseline air and European polluted air masses and trends have been determined for each wind direction sector. Evidence of the European phase-out of halocarbon usage is clearly apparent in the sorted halocarbon concentrations. A simple climatological long-range transport and a sophisticated Lagrangian air parcel dispersion model have been used to interpret the Mace Head halocarbon measurements and to derive estimates of European emission source strengths for each year. These emission source strengths confirm that the phase-out of halocarbon manufacture and sales is being followed in Europe.

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.

Calculated trends and the atmospheric abundance of 1,1,1,2‐tetrafluoroethane, 1,1‐dichloro‐1‐fluoroethane, and 1‐chloro‐1,1‐difluoroethane using automated in‐situ gas chromatography‐mass spectrometry measurements recorded at Mace Head, Ireland, from October 1994 to March 1997

The first in-situ measurements by automated gas chromatograph-mass spectrometer are reported for 1,1,1,2-tetrafluoroethane (HFC-134a), 1,1-dichloro-1-fluoroethane, (HCFC-141b), and 1-chloro-1,1-difluoroethane, (HCFC-142b). These compounds are steadily replacing the chlorofluorocarbons (CFCs) as refrigerants, foam-blowing agents, and solvents. The concentrations of all three compounds are shown to be rapidly increasing in the atmosphere, with 134a increasing at a rate of 2.05±0.02 ppt yr−1 over the 30 months of observations. Similarly, 141b and 142b increased at rates of 2.49±0.03 and 1.24±0.02 ppt yr−1, respectively, over the same period. The concentrations recorded at the atmospheric research station at Mace Head, Ireland, on January 1, 1996, the midpoint of the time series, were 3.67 ppt (134a), 7.38 ppt (141b), and 8.78 ppt (142b). From these observations we optimally estimate the HCFC and HFC emissions using a 12-box global model and OH concentrations derived from global 1,1,1-trichloroethane (CCl3CH3) measurements. Comparing two methods of estimating emissions with independent industry estimates shows satisfactory agreement for 134a and 141b, while for 142b, industry estimates are less than half those required to explain our observations.