Sources and source variations for aerosol at Mace Head,Ireland

The sources and source variations for aerosol at Mace Head, Ireland, were studied by applying positive matrix factorization (PMF), a variant of factor analysis, to a 5-yr data set for bulk aerosol. Signals for the following six sources were evident year round: (1) mineral dust, (2) sea salt, (3) general pollution, (4) a secondary SO₄²⁻–Se signal that is composed of both natural (marine) and pollution (coal) components, (5) ferrous industries, (6) and a second marine (possibly biogenic) source. Analyses of seasonally stratified data suggested additional sources for iodine and oil emissions but these were present only in certain seasons, respectively. The marine signal is particularly strong in winter. The main pollution transport from Europe to Mace Head occurs in May, but the influence of continental European emissions is evident throughout the year. Mineral aerosol evidently follows a transport pathway similar to that of pollution aerosol, i.e., recirculation via the westerlies brings pollutants mixed with dust to the site from nearby land, i.e., Ireland, the United Kingdom, and the Belgium, Netherlands, and Luxemburg (Benelux) region, with some inputs from Scandinavia, Western Europe, Eastern Europe, and even the Mediterranean region. Compared with Bermuda, aerosol at Mace Head has stronger marine sources (especially marine-derived secondary SO₄²⁻ and Se) but weaker crustal and oil signals. Transport across the North Atlantic, especially in winter, cannot be ruled out.     

International field intercomparison measurements of atmospheric mercury species at Mace Head,Ireland

Eleven laboratories from North America and Europe met at Mace Head, Ireland for the period 11–15 September 1995 for the first international field intercomparison of measurement techniques for atmospheric mercury species in ambient air and precipitation at a marine background location. Different manual methods for the sampling and analysis of total gaseous mercury (TGM) on gold and silver traps were compared with each other and with new automated analyzers. Additionally, particulate-phase mercury (Hg_part) in ambient air, total mercury, reactive mercury and methylmercury in precipitation were analyzed by some of the participating laboratories. Whereas measured concentrations of TGM and of total mercury in precipitation show good agreement between the participating laboratories, results for airborne particulate-phase mercury show much higher differences. Two laboratories measured inorganic oxidized gaseous mercury species (IOGM), and obtained levels in the low picogram m^-3 range.     

Continuous observations of carbon dioxide at Mace Head,Ireland from 1995 to 1999 and its net European ecosystem exchange

A 5-yr record of continuous high-frequency carbon dioxide CO₂ observations over the 1995–1999 period for the Mace Head Atmospheric Research Station has been examined to reveal a complex interplay between local- and regional-scale sources and sinks. During the winter months, an additional CO₂ source, over and above fossil fuel combustion, is required to support the observed concentrations of CO₂ in European regionally polluted air masses. During the summer months, an additional CO₂ sink is required. Over the entire study period, the additional net European ecosystem exchange source–sink required is –0.36±0.4 Gtonne C yr⁻¹.     

Trends over a 20-year period from 1987 to 2007 in surface ozone at the atmospheric research station,Mace Head,Ireland

Hourly measurements of baseline ozone at the Mace Head Atmospheric Research Station on the Atlantic Ocean coast of Ireland are observed when unpolluted air masses are advected to the station from across the North Atlantic Ocean. Monthly mean ozone mixing ratios in baseline air masses have risen steadily during the 1980s and 1990s reaching unprecedented levels during the early months of 1999. During the 2000s, baseline ozone mixing ratios have shown evidence of decline and stabilisation. Over the entire 20-year 1987–2007 period, the trend in annual baseline ozone has been +0.31±0.12(2−σ) ppb year⁻¹ and is highly statistically significant. Trends have been highest in the spring months and lowest in the summer months, producing a significant increase in the amplitude of the seasonal cycle. Over the shorter 1995–2007 period, we demonstrate how the growth to peak in 1999 and the subsequent decline have been driven by boreal biomass burning events during 1998/1999 and 2002/2003. The 2000s have been characterised by relatively constant baseline ozone and CH₄ levels and these may be a reasonable guide to future prospects, at least in the short term.     

Black carbon aerosol and carbon monoxide in European regionally polluted air masses at Mace Head, Ireland during 1995–1998

Continuous measurements of black carbon aerosol (BCA) at the Mace Head Atmospheric Research Station on the Atlantic Ocean coast of Ireland show the occurrence of dramatically elevated concentrations when regionally polluted air masses are advected to the station. These occurrences correlate well with similar elevations in carbon monoxide and a wide range of other trace gases monitored near-simultaneously with the BCA. Using daily sector allocation and a sophisticated Lagrangian dispersion model, two independent estimates of the European emission source strength of BCA that are required to explain the Mace Head observations have been made. The best estimates of the UK and European emission source strengths of BCA are 46±14 and [(482–511)±140]×10³ tonnes yr⁻¹, respectively, and these estimates compare favourably with published inventories, at least to within ±25%, though they are considerably smaller than the emissions employed in some early global climate model studies.     

Natural chloroform emissions from the blanket peat bogs in the vicinity of Mace Head,Ireland over a 14-year period

Simultaneous chloroform (CHCl₃) emission and ozone (O₃) deposition are regularly observed under nocturnal inversions during the summer months from and to the peat bogs in the vicinity of the Mace Head Atmospheric Research Station, Connemara, Co Galway, Ireland. Emissions were estimated using the nocturnal box model applied to routine atmospheric observations collected over a 14-year period from 1995 to 2008. Strict criteria were applied in the selection of events of low wind speed, under a stable night-time inversion layer in baseline air conditions, with no transport from Europe. The mean peatland CHCl₃ flux was 2.91 μg m^?2 h^?1 with highly variable fluxes ranging from 0.44 to 12.94 μg m^?2 h^?1. These fluxes are generally larger than those reported previously for similar biomes and if representative would make a significant contribution to the global estimated source of CHCl₃. Fluxes were not strongly correlated with either atmospheric temperature or the level of precipitation. Over the 14-year period there appears to have been a small increase in overall CHCl₃ emissions, although we stress that the nocturnal box model has a number of limitations and assumptions which should be taken into account.     

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

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. Office's 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.     

Quantitative trace analysis of polyfluorinated alkyl substances (PFAS) in ambient air samples from Mace Head (Ireland): A method intercomparison

A method intercomparison study of analytical methods for the determination of neutral, volatile polyfluorinated alkyl substances (PFAS) was carried out in March, 2006. Environmental air samples were collected in triplicate at the European background site Mace Head on the west coast of Ireland, a site dominated by ‘clean’ westerly winds coming across the Atlantic. Extraction and analysis were performed at two laboratories active in PFAS research using their in-house methods. Airborne polyfluorinated telomer alcohols (FTOHs), fluorooctane sulfonamides and sulfonamidoethanols (FOSAs/FOSEs) as well as additional polyfluorinated compounds were investigated. Different native and isotope-labelled internal standards (IS) were applied at various steps in the analytical procedure to evaluate the different quantification strategies. Field blanks revealed no major blank problems. European background concentrations observed at Mace Head were found to be in a similar range to Arctic data reported in the literature. Due to trace-levels at the remote site, only FTOH data sets were complete and could therefore be compared between the laboratories. Additionally, FOSEs could partly be included. Data comparison revealed that despite the challenges inherent in analysis of airborne PFAS and the low concentrations, all methods applied in this study obtained similar results. However, application of isotope-labelled IS early in the analytical procedure leads to more precise results and is therefore recommended.     

Statistical analysis of condensation nuclei measurements in northwestern Spain

Measurements of condensation nuclei (CN) were taken daily at Villanubla, Spain, 845 m above sea level, in the months of March and April, 1980. The results are analyzed considering the fit to different statistical distributions using various stratifications based on meteorological parameters.     

The phase-in and phase-out of European emissions of HCFC-141b and HCFC-142b under the Montreal Protocol: Evidence from observations at Mace Head,Ireland and Jungfraujoch,Switzerland from 1994 to 2004

The mixing ratios of HCFC-141b (1,1-dichlorofluoroethane) and HCFC-142b (1-chloro-1,1-difluoroethane) have been rising steadily in baseline air at Mace Head, Ireland over the 10-year period from 1994 to 2004. These HCFCs are widely used replacements for the chlorofluorocarbons phased out under the Montreal Protocol and its subsequent amendments. Analysis of the HCFC content of regionally-polluted air arriving at Mace Head from the European continent shows that European emissions reached a peak during 2000–2001 and have declined subsequently, following the phase-out in their usage. European emissions of HCFC-141b have been further constrained by observations at the High-Alpine Jungfraujoch site. The reductions are consistent with the phase-out of HCFC production and use from the year 2001 onwards mandated by European regulations designed to exceed the requirements of the Montreal Protocol.     

Particle size dependence of a condensation nuclei counter

The influence of the particle size on the concentration indicated by a condensation nuclei counter (Model Rich 100, Environment One Corp.) was determined experimentally. The particle size dependence of this device was measured using fairly monodisperse silver particles and an absolute photographic condensation nuclei counter. The absolute calibration factor of the condensation nuclei counter also changed when the particle size of an aerosol containing atmospheric and Bunsen nuclei was changed.     

A preliminary study of the chemical modification of cloud condensation nuclei in stratiform clouds at Whiteface Mountain,New York

Results are presented for pH, nitrate and sulfate ion content of cloud water collected at Whiteface Mountain in northern New York. Evidence exists for the production of sulfate in possibly one of the case studies and for nitrate production in all three of the case studies examined. The results are not entirely consistent with the hypothesis that chemical modification of cloud condensation nuclei (CCN) takes place in stratiform clouds. For only one case is CCN production evident and total aerosol number concentration is enhanced.The measured nitrate production cannot be accounted for by the soluble fraction of the CCN aerosol and may result from the absorption of interstitial HNO₃(g). This might account for the change in cloud condensation nuclei, indicated by the results, when sulfate production was not evident. The CCN spectrum can also be altered by agglomeration of captured particles upon cloud droplet evaporation. It is not possible to separate the two mechanisms (chemical vs physical) at this time.     

On the operation of the TSI-3020 condensation nuclei counter at altitudes up to 10 km

A TSI-3020 condensation nuclei counter has been modified for airborne use up to 10 km altitude. The single particle count mode of the instrument was calibrated with laboratory aerosols at pressures down to 180 Torr. Negligible pressure dependence was observed above 350 Torr. During a recent Arctic field experiment, the instrument was flown at altitudes up to 101cm.     

Modification of a commercial condensation nuclei counter for steady flow

By replacing two valves and adding an external reservoir, the input flow oscillations of the Model Rich 100 Condensation Nuclei Monitor (Environment/One Corp.) were eliminated. This increased the instrument's usefulness for analyzing aerosols.     

An analysis of the SO2 concentration levels in Athens,Greece

In this paper, an analysis of the meteorological parameters that affect SO₂ pollution in Athens, a problem of both local and international concern, is presented. The influence of these meteorological parameters on the SO₂ concentrations has been investigated by a statistical analysis of the daily average SO₂ values measured at six locations in the Athens basin for the six years from 1974 to 1979. Wind speed, minimum temperature and amount of rain has been found to control SO₂ concentrations during the cold season while wind speed, wind direction and relative humidity are central in the warm season. Based on this, multiple regression models, both linear and non-linear, for the prediction of the next day's SO₂ concentration have been derived that explain more than 50% of the data variance. Further improvements on the modelling are contingent on the availability of boundary layer structure data and on details of the local wind field. The meteorology of high concentration episodes has also been examined and the synoptic characteristics for the onset and end of such episodes have been identified. Finally, discriminant analysis classification functions, utilizing forecast meteorological variables have been obtained which are capable of predicting accurately the occurrence of high pollution concentrations.     

Methane emissions from peat bogs in the vicinity of the Mace Head Atmospheric Research Station over a 12-year period

Methane emissions from the peat bogs in Connemara, Ireland have been inferred from the trace gas observations at the Mace Head Atmospheric Research Station using the nocturnal box method. A total of 237 local events, during April to September, over a 12-year period have been studied. Simultaneous emissions of methane, carbon dioxide and chloroform are routinely observed under nocturnal inversions with low wind speeds from the peat bogs proximal to Mace Head. Night-time deposition of ozone and hydrogen occurs concurrently with these emissions. Using the temporally correlated methane and ozone data we estimate methane emissions from each event. Simultaneous methane and chloroform emissions, together with ozone and hydrogen deposition have been characterised, leading to the estimation of methane emission rates for each event. The mean methane emission flux was found to be 400 ± 90 ng m^?2 s^?1. A strong seasonal cycle was found in the methane emission fluxes but there was little evidence of a long-term trend in the emissions from the peat bogs in the vicinity of the Mace Head station.     

Long-term study of cloud condensation nuclei (CCN) activation of the atmospheric aerosol in Vienna

During a total of 11 months, cloud condensation nuclei (CCN at super-saturation S 0.5%) and condensation nuclei (CN) concentrations were measured in the urban background aerosol of Vienna, Austria. For several months, number size distributions between 13.22?nm and 929?nm were also measured with a scanning mobility particle spectrometer (SMPS). Activation ratios (i.e. CCN/CN ratios) were calculated and apparent activation diameters obtained by integrating the SMPS size distributions. Variations in all CCN parameters (concentration, activation ratio, apparent activation diameter) are quite large on timescales of days to weeks. Passages of fronts influenced CCN parameters. Concentrations decreased with the passage of a front. No significant differences were found for fronts from different sectors (for Vienna mainly north to west and south to east). CCN concentrations at 0.5% S ranged from 160?cm(-3) to 3600?cm(-3) with a campaign average of 820?cm(-3). Activation ratios were quite low (0.02-0.47, average: 0.13) and comparable to activation ratios found in other polluted regions (e.g. Cubison et?al., 2008). Apparent activation diameters were found to be much larger (campaign average: 169?nm, range: (69-370) nm) than activation diameters for single-salt particles (around 50?nm depending on the salt). Contrary to CN concentrations, which are influenced by source patterns, CCN concentrations did not exhibit distinct diurnal patterns. Activation ratios showed diurnal variations counter-current to the variations of CN concentrations.     

Composition analysis of PM2.5 at multiple sites in Zhengzhou,China: implications for characterization and source apportionment at different pollution levels

Environmental Science and Pollution Research - Zhengzhou is one of the most heavily polluted cities in China. This study collected samples of PM2.5 (atmospheric fine particulate matter with...