This section contains conference presentations or proceedings that have some connection either with the Mace Head Research Station or with members, both present and past, of the Atmospheric Physics Research Cluster at NUI, Galway.
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T.C. O'Connor, L.W. Pollak, T.Murphy, The Uncertainties in measurement of concentratikons of Condensation Nuclei with photoelectric counters and the decay of nuclei in large vessels
Jennings, S.G. (1981)- The effect of particle size distribution and complex index of refraction of atmospheric aerosols in the visual range. Proc. of the Ninth International Conference in Atmospheric Aerosol, Condensation and Ice Nuclei, Galway University Press, 415 - 420.
Relationship between IR Extinction, Absorption, backscatter and liquid water content of the major cloud types
O'Doherty, S., et al. (2004), Rapid growth of hydrofluorocarbon 134a and hydrochlorofluorocarbons 141b, 142b, and 22 from Advanced Global Atmospheric Gases Experiment (AGAGE) observations at Cape Grim, Tasmania, and Mace Head, Ireland, J. Geophys. Res., 109, D06310, doi:10.1029/2003JD004277.
An update of in situ Advanced Global Atmospheric Gases Experiment (AGAGE) hydrofluorocarbon (HFC)/hydrochlorofluorocarbon (HCFC) measurements made at Mace Head, Ireland, and Cape Grim, Tasmania, from 1998 to 2002 are reported. HCFC-142b, HCFC-141b, HCFC-22 and HFC-134a show continued rapid growth in the atmosphere at mean rates of 1.1, 1.6, 6.0, and 3.4 ppt/year, respectively. Emissions inferred from measurements are compared to recent estimates from consumption data. Minor updates to the industry estimates of emissions are reported together with a discussion of how to best determine OH concentrations from these trace gas measurements. In addition, AGAGE measurements and derived emissions are compared to those deduced from NOAA-Climate Monitoring and Diagnostics Laboratory flask measurements (which are mostly made at different locations). European emission estimates obtained from Mace Head pollution events using the Nuclear Accident Model (NAME) dispersion model and the best fit algorithm (known as simulated annealing) are presented as 3-year rolling average emissions over Europe for the period 1999–2001. Finally, the measurements of HCFC-141b, HCFC-142b, and HCFC-22 discussed in this paper have been combined with the Atmospheric Lifetime Experiment (ALE)/Global Atmospheric Gases Experiment (GAGE)/AGAGE measurements of CFC-11, CFC-12, CFC-113, CCl4, and CH3CCl3 to produce the evolution of tropospheric chlorine loading.
Optimal estimation of the soil uptake rate of molecular hydrogen from the Advanced Global Atmospheric Gases Experiment and other measurements
Xiao, X., et al. (2007), Optimal estimation of the soil uptake rate of molecular hydrogen from the Advanced Global Atmospheric Gases Experiment and other measurements, J. Geophys. Res., 112, D07303, doi:10.1029/2006JD007241.
Hydrogen (H2), a proposed clean energy alternative, warrants detailed investigation of its global budget and future environmental impacts. The magnitudes and seasonal cycles of the major (presumably microbial) soil sink of hydrogen have been estimated from high-frequency in situ AGAGE H2 observations and also from more geographically extensive but low-frequency flask measurements from CSIRO and NOAA-GMD using the Kalman filter in a two-dimensional (2-D) global transport model. Hydrogen mole fractions exhibit well-defined seasonal cycles in each hemisphere with their phase difference being only about 3 months. The global production rate of H2 is estimated to be 103 ± 10 Tg yr−1 with only a small estimated interannual variation. Soil uptake (84 ± 8 Tg yr−1) represents the major loss process for H2 and accounts for 81% of the total destruction. Strong seasonal cycles are deduced for the soil uptake of H2. The soil sink is a maximum over the northern extratropics in summer and peaks only 2 to 3 months earlier in the Northern Hemisphere than in the Southern Hemisphere. Oxidation by tropospheric OH (18 ± 3 Tg yr−1) accounts for 17% of the destruction, with the remainder due to destruction in the stratosphere. The calculated global burden is 191 ± 29 Tg, indicating an overall atmospheric lifetime of 1.8 ± 0.3 years. Hydrogen in the troposphere (149 ± 23 Tg burden) has a lifetime of 1.4 ± 0.2 years.
Observations of 1,1-difluoroethane (HFC-152a) at AGAGE and SOGE monitoring stations in 1994–2004 and derived global and regional emission estimates
Greally, B. R., et al. (2007), Observations of 1,1-difluoroethane (HFC-152a) at AGAGE and SOGE monitoring stations in 1994–2004 and derived global and regional emission estimates, J. Geophys. Res., 112, D06308, doi:10.1029/2006JD007527.
Ground-based in situ measurements of 1,1-difluoroethane (HFC-152a, CH3CHF2) which is regulated under the Kyoto Protocol are reported under the auspices of the AGAGE (Advanced Global Atmospheric Gases Experiment) and SOGE (System of Observation of halogenated Greenhouse gases in Europe) programs. Observations of HFC-152a at five locations (four European and one Australian) over a 10 year period were recorded. The annual average growth rate of HFC-152a in the midlatitude Northern Hemisphere has risen from 0.11 ppt/yr to 0.6 ppt/yr from 1994 to 2004. The Southern Hemisphere annual average growth rate has risen from 0.09 ppt/yr to 0.4 ppt/yr from 1998 to 2004. The 2004 average mixing ratio for HFC-152a was 5.0 ppt and 1.8 ppt in the Northern and Southern hemispheres, respectively. The annual cycle observed for this species in both hemispheres is approximately consistent with measured annual cycles at the same locations in other gases which are destroyed by OH. Yearly global emissions of HFC-152a from 1994 to 2004 are derived using the global mean HFC-152a observations and a 12-box 2-D model. The global emission of HFC-152a has risen from 7 Kt/yr to 28 Kt/yr from 1995 to 2004. On the basis of observations of above-baseline elevations in the HFC-152a record and a consumption model, regional emission estimates for Europe and Australia are calculated, indicating accelerating emissions from Europe since 2000. The overall European emission in 2004 ranges from 1.5 to 4.0 Kt/year, 5–15% of global emissions for 1,1-difluoroethane, while the Australian contribution is negligible at 5–10 tonnes/year, <0.05% of global emissions.
S. Reimann, A.J. Manning, P.G. Simmonds, D.M. Cunnold, R.H.J. Wang, J. Li, A. McCulloch, R.G. Prinn, J. Huang, R.F. Weiss, P.F. Fraser, S. O'Doherty, B.R. Greally, K. Stemmler, M. Hill, and D. Folini, (2005), Low European methyl chloroform emissions inferred from long-term atmospheric measurements, Nature, 433, 506-508.
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 steadily2-4 and recent European methyl chloroform consumption and emissions were estimated to be less than 0.1 gigagrams per year1,5. 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 emissions1,4. Such enhanced emissions would significantly affect results from the CH3CCl3 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 data1,5, but are considerably lower than those derived from the EXPORT campaign in 2000
Lifetime and emission estimates of 1,1,2-trichlorotrifluorethane (CFC-113) from daily global background observations June 1982–June 1994
Fraser, P., D. Cunnold, F. Alyea, R. Weiss, R. Prinn, P. Simmonds, B. Miller, and R. Langenfelds (1996), Lifetime and emission estimates of 1,1,2-trichlorotrifluorethane (CFC-113) from daily global background observations June 1982–June 1994, J. Geophys. Res., 101(D7), 12,585–12,599.
Observations every two hours of CCl2FCClF2 at Mace Head, Ireland (February 1987–June 1994); Cape Meares, Oregon (April 1984–June 1989); Ragged Point, Barbados (October 1985–June 1994); Cape Matatula, Samoa (October 1985–June 1989 and January 1992–June 1994); and Cape Grim, Tasmania (June 1982–June 1994) are reported. The observations from Cape Grim have been extended back to 1978 using archived air samples. The global atmospheric abundance of CCl2FCClF2 is indicated to have been growing exponentially between 1978 and 1987 with an e-folding time of approximately 7.6 years; it has been growing less rapidly since that time. On January 1, 1994, the mean inferred northern hemispheric mixing ratio in the lower troposphere was 84.4 ± 0.4 ppt and the southern hemispheric value was 80.6 ± 0.4 ppt; the global growth rate in 1991–1993 is estimated to have averaged approximately 3.1 ± 0.1 ppt/year. The differences between the northern and southern hemispheric concentrations are calculated to be consistent with the almost entirely northern hemispheric release of this gas. The annual release estimates of CCl2FCClF2 by industry, which include estimates of eastern European emissions, fairly consistently exceed those deduced from the measurements by approximately 10% from 1980 to 1993. The uncertainties in each estimate is approximately 5%. This difference suggests that up to 10% of past production might not yet have been released. The measurements indicate that atmospheric releases of CCl2FCClF2 have been decreasing rapidly since 1989 and in 1993 amounted to 78 ± 27 × 106 kg or 42 ± 15% of the 1985–1987 emissions.
In situ measurements of atmospheric methane at GAGE AGAGE sites during 1985–2000 and resulting source inferences
Cunnold, D. M., et al. (2002), In situ measurements of atmospheric methane at GAGE/AGAGE sites during 1985–2000 and resulting source inferences, J. Geophys. Res., 107(D14), 4225, doi:10.1029/2001JD001226.
Continuous measurements of methane since 1986 at the Global Atmospherics Gases Experiment/Advanced Global Atmospherics Gases Experiment (GAGE/AGAGE) surface sites are described. The precisions range from approximately 10 ppb at Mace Head, Ireland, during GAGE to better than 2 ppb at Cape Grim, Tasmania, during AGAGE (i.e., since 1993). The measurements exhibit good agreement with coincident measurements of air samples from the same locations analyzed by Climate Monitoring and Diagnostics Laboratory (CMDL) except for differences of approximately 5 ppb before 1989 (GAGE lower) and about 4 ppb from 1991 to 1995 (GAGE higher). These results are obtained before applying a factor of 1.0119 to the GAGE/AGAGE values to place them on the Tohoku University scale. The measurements combined with a 12-box atmospheric model and an assumed atmospheric lifetime of 9.1 years indicates net annual emissions (emissions minus soil sinks) of 545 Tg CH4 with a variability of only ±20 Tg from 1985 to 1997 but an increase in the emissions in 1998 of 37 ± 10 Tg. The effect of OH changes inferred by Prinn et al.  is to increase the estimated methane emissions by approximately 20 Tg in the mid-1980s and to reduce them by 20 Tg in 1997 and by more thereafter. Using a two-dimensional (2-D), 12-box model with transport constrained by the GAGE/AGAGE chlorofluorocarbon measurements, we calculate that the proportion of the emissions coming from the Northern Hemisphere is between 73 and 81%, depending on the OH distribution used. However, this result includes an adjustment of 5% derived from a simulation of the 2-D estimation procedure using the 3-D MOZART model. This adjustment is needed because of the very different spatial emission distributions of the chlorofluorocarbons and methane which makes chlorofluorocarbons derived transport rates inaccurate for the 2-D simulation of methane. The 2-D model combined with the annual cycle in OH from Spivakovsky et al.  provide an acceptable fit to the observed 12-month cycles in methane. The trend in the amplitude of the annual cycle of methane at Cape Grim is used to infer a trend in OH in 30°–90°S of 0 ± 5% per decade from 1985 to 2000, in qualitative agreement with Prinn et al.  for the Southern Hemisphere.
In situ chloroform measurements at Advanced Global Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998
O'Doherty, S., et al. (2001), In situ chloroform measurements at Advanced Global Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998, J. Geophys. Res., 106(D17), 20,429–20,444.
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.
Simmonds, P. G., et al. (2006), Global trends, seasonal cycles, and European emissions of dichloromethane, trichloroethene, and tetrachloroethene from the AGAGE observations at Mace Head, Ireland, and Cape Grim, Tasmania, J. Geophys. Res., 111, D18304, doi:10.1029/2006JD007082.
In situ observations (every 4 hours) of dichloromethane (CH2Cl2) from April 1995 to December 2004 and trichloroethene (C2HCl3) and tetrachloroethene (C2Cl4) 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, CH2Cl2 and C2Cl4 data collection commenced in 1998 and 2000, respectively. C2HCl3 is below the limit of detection at Cape Grim except during pollution episodes. At Mace Head CH2Cl2 shows a downward trend from 1995 to 2004 of 0.7 ± 0.2 ppt yr−1 (ppt: expressed as dry mole fractions in 1012), 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 CH2Cl2 at Cape Grim. The time series for C2HCl3 and C2Cl4 are relatively short for accurate trend analyses; however, we observe a small but significant decline in C2Cl4 (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 C2HCl3. Emissions estimated from observations are lower than industry emission estimates for C2Cl4 and much lower in the case of CH2Cl2. A study of wildfires in Tasmania, uncontaminated by urban emissions, suggests that the biomass burning source of CH2Cl2 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.
Global trends and emission estimates of CCl4 from in situ background observations from July 1978 to June 1996
Simmonds, P. G., D. M. Cunnold, R. F. Weiss, R. G. Prinn, P. J. Fraser, A. McCulloch, F. N. Alyea, and S. O'Doherty (1998), Global trends and emission estimates of CCl4 from in situ background observations from July 1978 to June 1996, J. Geophys. Res., 103(D13), 16,017–16,027
Atmospheric Lifetime Experiment/Global Atmospheric Gases Experiment/Advanced Global Atmospheric Gases Experiment (ALE/GAGE/AGAGE) measurements of CCl4 at five remote surface locations from 1978 to 1996 are reported. The Scripps Institution of Oceanography (SIO) 1993 absolute calibration scale is used, reducing the concentrations by a factor of 0.77 compared to previous ALE/GAGE reports. Atmospheric concentrations of CCl4 reached a peak in 1989-1990 of 104.4 ± 3.1 parts per trillion (ppt) and have since been decreasing 0.7 ± 0.1 ppt yr-1. Assuming an atmospheric lifetime of 42 ± 12 years, the emissions averaged 94-11+22 × 106 kg from 1979 to 1988 and 49-13+26 × 106 kg from 1991 to 1995. The reduction in the emissions in 1989-1990 coincided with a substantial decrease in the global production of the chlorofluorocarbons (CFCs). The total emission of CCl4 from countries that report annual production is estimated to have declined from 11% in 1972 to 4% in 1995 of the CCl4 needed to produce the CFC amounts reported. This implies that nonreporting countries released substantial amounts of CCl4 into the atmosphere in the 1980s and that their releases have exceeded those from the reporting countries since 1991.
Cunnold, D. M., R. F. Weiss, R. G. Prinn, D. Hartley, P. G. Simmonds, P. J. Fraser, B. Miller, F. N. Alyea, and L. Porter (1997), GAGE/AGAGE measurements indicating reductions in global emissions of CCl3F and CCl2F2 in 1992–1994, J. Geophys. Res., 102(D1), 1259–1269.
Global Atmospheric Gases Experiment/Advanced GAGE (GAGE/AGAGE) observations of CCl3F indicate that global concentrations of this compound reached a maximum in 1993 and decayed slightly in 1994; CCl2F2 concentrations increased approximately 7 ppt in both 1993 and 1994. The observations suggest that world emissions in these two years were smaller than industry production figures would suggest and have decreased faster than expected under the Montreal Protocol and its amendments. An analysis of regional pollution events at the Mace Head site suggest that industry may be underestimating the decline of emissions in Europe. It is argued, however, that the decline in European emissions is not biasing the background Mace Head measurements (or the GAGE global averages). Combining the chlorofluorocarbon measurements, including CCl2FCClF2, with GAGE/AGAGE measured global decreases in CH3CCl3 and CCl4 after 1992 and with Cape Grim archived air measurements of CHClF2, the measurements suggest that anthropogenic atmospheric chlorine loading from these six gases maximized in 1992 at 2.95 ± 0.04 ppb and that it had decreased by 0.02 ± 0.01 ppb by the beginning of 1995.
Vollmer, M. K., S. Reimann, D. Folini, L. W. Porter, and L. P. Steele (2006), First appearance and rapid growth of anthropogenic HFC-245fa (CHF2CH2CF3) in the atmosphere, Geophys. Res. Lett., 33, L20806, doi:10.1029/2006GL026763.
We capture the first atmospheric appearance of HFC-245fa (CHF2CH2CF3), a new foam blowing agent. Our results from the high-altitude observatory at Jungfraujoch, Switzerland, show a rapid growth of this substance in the northern hemispheric troposphere from 0.28 ppt in July 2004 to 0.68 ppt at the end of 2005, which corresponds to an overall increase of >90% per year. By combining our observations with an atmospheric 3-box model we estimate a southern hemispheric trend for this trace gas which we compare to observations at southern hemisphere mid-latitudes. We also estimate a global HFC-245fa emissions increase from 2100–2400 tonnes in 2003 to 5100–5900 tonnes in 2005. Pollution episodes are relatively rare at Jungfraujoch compared to other hydrofluorocarbons thereby confirming the limited use of HFC-245fa in Europe. Back trajectory analysis reveals the largest potential European sources of HFC-245fa in northern Italy and northeastern Spain.
Experimental verification of a linear relation between IR Extinction and liquid water content of fogs
Pinnick, R.G., Jennings, S.G., and Chylek, P. (1978)-Experimental verification of a linear relation between IR extinction and liquid water content of fogs. American Meteorological Society Third Conference on Atmospheric Radiation, Davis, California, 140-143.
Droplet size spectra and water-vapor concentration of laboratory water clouds: inversion of Fourier transform infrared �500–5000 cm �1 � optical-depth measurement
Prinn, R. G., et al. (2005), Evidence for variability of atmospheric hydroxyl radicals over the past quarter century, Geophys. Res. Lett., 32, L07809, doi:10.1029/2004GL022228.
The hydroxyl free radical (OH) is the major oxidizing chemical in the atmosphere, destroying about 3.7 petagrams (Pg) of trace gases each year, including many gases involved in ozone depletion, the greenhouse effect and urban air pollution. Measurements of 1,1,1-trichloroethane (methyl chloroform, CH3CCl3), which reacts with OH, provide the most accurate method currently utilized for determining the global behavior of OH. We report that CH3CCl3 levels rose steadily from 1978 to reach a maximum in 1992 and have since decreased rapidly to levels in 2004 about 30% of the levels when measurements began in 1978. Analysis of these observations shows that global average OH levels had a small maximum around 1989 and a larger minimum around 1998, with OH concentrations in 2003 being comparable to those in 1979. This post-1998 recovery of OH reported here contrasts with the situation 4 years ago when reported OH was decreasing. The 1997–1999 OH minimum coincides with, and is likely caused by, major global wildfires and an intense El Nino event at this time.
Prinn, R. G.; Huang, J.; Weiss, R. F.; Cunnold, D. M.; Fraser, P. J.; Simmonds, P. G.; McCulloch, A.; Harth, C.; Salameh, P.; O'Doherty, S.; Wang, R. H. J.; Porter, L.; Miller, B. R.,Evidence for Substantial Variations of Atmospheric Hydroxyl Radicals in the Past Two Decades, Science, Volume 292, Issue 5523, pp. 1882-1888 (2001).
European Emissions of HFC-365mfc, a Chlorine-Free Substitute for the Foam Blowing Agents HCFC-141b and CFC-11
European Emissions of HFC-365mfc, a Chlorine-Free Substitute for the Foam Blowing Agents HCFC-141b and CFC-11
HFC-365mfc (1,1,1,3,3-pentafluorobutane) is an industrial chemical used for polyurethane foam blowing. From early 2003, HFC-365mfc has been commercially produced as a substitute for HCFC-141b, whose use in Europe has been banned since January 2004. We describe the first detection of HFC-365mfc in the atmosphere and report on a 2 year long record at the high Alpine station of Jungfraujoch (Switzerland) and the Atlantic coast station of Mace Head (Ireland). The measurements at Jungfraujoch are used to estimate the central European emissions of HFC-365mfc, HCFC-141b, and CFC-11. For HFC-365mfc, we estimate the central European emissions (Germany, France, Italy, Switzerland, The Netherlands, Belgium, and Luxembourg) in 2003 and 2004 as 400-500 tonnes year-1. These emissions are about one-third lower on a per capita basis than what we estimate from the Mace Head measurements for the total of Europe. The estimated emissions of HCFC-141b for central Europe are higher (i.e., 7.2-3.5 ktonnes year-1) with a decreasing trend in the period from 2000 to 2004. Residual emissions of CFC-11 are estimated at 2.4-4.7 ktonnes year-1 in the same time period. The Po Valley (northern Italy) appears to be a main source region for HFC-365mfc and for the former blowing agents HCFC-141b and CFC-11. In 2004, the emissions of HFC-365mfc arose from a wider region of Europe, which we attribute to an increased penetration of HFC-365mfc into the European market.
Jennings, S.G., and O'Connor, T.C (1969)-
Diffusion coefficients of charged aerosol particles. Proc. 7th International Conference: Condensation and Ice Nuclei, Prague, Vienna, 146-149.
Continuous Measurements of the natural aerosol size distribution at rural mountain and maritime sites
Jennings, S.G. (1976)- Continuous measurements of the natural aerosol size distribution at rural, mountain and maritime sites. Conference on the Atmospheric Aerosols: Their Optical Properties and Effects. NASA Conference Publication CP-2004, MB 4-1 to 4-4.
Continuous high-frequency observations of hydrogen at the Mace Head baseline atmospheric monitoring station over the 1994–1998 period
Simmonds, P. G., R. G. Derwent, S. O'Doherty, D. B. Ryall, L. P. Steele, R. L. Langenfelds, P. Salameh, H. J. Wang, C. H. Dimmer, and L. E. Hudson (2000), Continuous high-frequency observations of hydrogen at the Mace Head baseline atmospheric monitoring station over the 1994–1998 period, J. Geophys. Res., 105(D10), 12,105–12,121
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.
O'Reilly S.; Kleefeld C.; Jennings S.G.; Aalto P.; Becker E.; O'Dowd C.D., Comparison of measured and calculated aerosol optical properties at mace head, Journal of Aerosol Science, Volume 31, Supplement 1, September 2000 , pp. 274-275(2)
There are large uncertainties associated with the estimation of the direct radiative forcing of the earth's climate by tropospheric aerosol particles (IPCC, 1996). The radiative effects of the tropospheric aerosol depend on the chemical, physical and optical properties of the aerosol. Because of their short atmospheric residence times, the distribution of tropospheric aerosols about the globe varies significantly, both spatially and temporally. Therefore, investigation of radiative forcing due to these aerosols requires analysis on a regional scale and the characterisation of the properties of the local aerosol.
Uncertainties associated with the calculation of direct radiative forcing by tropospheric aerosols can be identified and quantified using closure studies (Quinn et al., 1996). In a closure study a measured aerosol property is compared with values calculated from a model using other independently measured properties. Closure is achieved if there is agreement between the measured and calculated values within an accepted level of uncertainty. Such agreement indicates that the model may be a suitable representation of the observed system.
Black carbon aerosol and carbon monoxide in European regionally polluted air masses at Mace Head, Ireland during 1995–1998
Derwent, R.G., Ryall, D.B., Jennings, S.G., Spain, T.G., and Simmonds, P.G. (2001). Black carbon aerosol and carbon monoxide in European regionally polluted air masses at Mace Head, Ireland during 1995-1998. Atmos. Environ., 35, 6371-6378.
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]x103 tonnes/yr, 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.
Kenny, C.M., and Jennings, S.G. (1998). Background bioaerosol measurements at Mace Head. J. Aerosol Sci., 29, S779-S780.
Atmospheric histories of halocarbons from analysis of Antarctic firn air Major Montreal Protocol species
Sturrock, G. A., D. M. Etheridge, C. M. Trudinger, P. J. Fraser, and A. M. Smith (2002), Atmospheric histories of halocarbons from analysis of Antarctic firn air: Major Montreal Protocol species, J. Geophys. Res., 107(D24), 4765, doi:10.1029/2002JD002548.
Air samples extracted from Antarctic firn at Law Dome have been analyzed for the suite of halocarbons that contribute most of the anthropogenic chlorine and about half the anthropogenic bromine presently released into the stratosphere. The species, all included in the Montreal Protocol, are the chlorofluorocarbons (CFCs -11, -12, -113, -114, -115), hydrochlorofluorocarbons (HCFCs -22, -141b, -142b), halons (H -1211, -1301), CH3CCl3 (methyl chloroform) and CCl4 (carbon tetrachloride). The measurements were used to reconstruct the atmospheric history of these species since the 1930s, providing a record considerably predating existing in situ records or other conventional air archives, encompassing virtually the entire history of anthropogenic emissions of CFCs, HCFCs, and halons and giving early 20th century levels for CH3CCl3 and CCl4. Significant features of this study are (1) the narrow age spread (spectral width 5 years) of the individual firn air samples, which reveals rapid atmospheric changes, (2) the use of inversion techniques to infer past atmospheric composition with associated uncertainties, and (3) the low analytical detection limit (<0.1 ppt), which, together with the narrow air age spread, detects early background levels and resolves the time that industrial emissions first appeared in the southern hemisphere atmosphere. Integrity of the data is demonstrated by successful intercomparison of data from independent firn sites on Law Dome with common time-series. An upper limit is given for the potential contribution to atmospheric levels of CH3CCl3 from nonindustrial sources. The atmospheric records produced from firn air are compared to calculations based on the history of their global emissions.
R.G. Prinn, D. Cunnold, R. Rasmussen, P. Simmonds, F. Alyea, A. Crawford, P. Fraser, and R. Rosen. Atmospheric emissions and trends of nitrous oxide deduced from ten years of ALE/GAGE data. J. Geophys. Res., 95, 18369-18385, 1990.
Aitken Nuclei Measurements and Evidence of Gas-to-particle conversion Processes at Mace Head, Ireland
O'Connor, T.C., McGovern, F.M., Jennings, S.G. & Philipp, C.(University of Hannover) (1994)-
Aitken nuclei measurements and evidence of gas-to-particle conversion processes at Mace Head, Ireland. Proceedings of EUROTRAC 94 Symposium, The Hague, SPB Academic Publishing, 1206-1209.
AGAGE Observations of Methyl Bromide and Methyl Chloride at Mace Head, Ireland, and Cape Grim, Tasmania, 1998–2001
Simmonds, P.; Derwent, R.; Manning, A.; Fraser, P.; Krummel, P.; O'Doherty, S.; Prinn, R.; Cunnold, D.; Miller, B.; Wang, H.; Ryall, D.; Porter, L.; Weiss, R.; Salameh, P. ,AGAGE Observations of Methyl Bromide and Methyl Chloride at Mace Head, Ireland, and Cape Grim, Tasmania, 1998–2001, Journal of Atmospheric Chemistry, pg 1573-0662
In situ AGAGE GC-MS measurements of methyl bromide (CH3Br) and methyl chloride (CH3Cl) at Mace Head, Ireland and Cape Grim, Tasmania (1998–2001) reveal a complex pattern of sources. At Mace Head both gases have well-defined seasonal cycles with similar average annual decreases of 3.0% yr−1 (CH3Br) and 2.6% yr−1 (CH3Cl), and mean northern hemisphere baseline mole fractions of 10.37 ± 0.05 ppt and 535.7 ± 2.2 ppt, respectively. We have used a Lagrangian dispersion model and local meteorological data to segregate the Mace Head observations into different source regions, and interpret the results in terms of the known sources and sinks of these two key halocarbons. At Cape Grim CH3Br and CH3Cl also show annual decreases in their baseline mixing ratios of 2.5% yr−1 and 1.5% yr−1, respectively. Mean baseline mole fractions were 7.94 ± 0.03 ppt (CH3Br) and 541.3 ± 1.1 ppt (CH3Cl). Although CH3Cl has astrong seasonal cycle there is no well-defined seasonal cycle in the Cape Grim CH3Br record. The fact that both gases are steadily decreasing in the atmosphere at both locations implies that a change has occurred which is affecting a common, major source of both gases (possibly biomass burning) and/or their major sink process (destruction by hydroxyl radical).