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Rasmussen, R. A.

Publications and source records attributed to Rasmussen, R. A..

At least 37 records · Page 2

Tropospheric methane in the mid-latitudes of the Southern Hemisphere

More than 800 methane concentration measurements have been obtained for the Southern Hemisphere's troposphere over the September 1980-March 1983 period. Concentrations are noted to increase throughout the troposphere during the study period, adding further support to the view that CH4 concentrations are currently increasing on a global scale. In the surface methane data, a seasonal cycle with a peak-to-peak amplitude of 28 ppbv is found. Maxima and minima are on September-October and March, respectively. The phase and amplitude of the cycle are qualitatively consistent with the concept that the major sink for methane is oxidation by hydroxyl radicals. Evidence is found for a positive vertical gradient in methane content.

Fraser, P. J.↗

The atmospheric lifetime experiment. I - Introduction, instrumentation, and overview

The Atmospheric Lifetime Experiment is designed to determine accurately the atmospheric concentrations of the four halocarbons CFCl3, CF2Cl2, CCl4, and CH3CCl3, and also of N2O with emphasis on measurement of their long-term trends in the atmosphere. Comparison of these concentrations and trends for the four halocarbons with estimates of their industrial emission rates then enables calculations of their global circulation rates and globally averaged atmospheric lifetimes. The experiment utilizes automated dual-column electron-capture gas chromatographs which sample the background air about 4 times daily at the following globally distributed sites: Adrigole, Ireland, Cape Meares, Oregon; Ragged Point, Barbados; Point Matatula, American Samoa, and Cape Grim, Tasmania. The climatology of these 'clean air' sites and their ability to describe the global air mass are reviewed. The instrumentation and methods for data acquisition and processing are then described. An overview of the data obtained and the trends derived during the 3-year period from July 1978 through June 1981 for each of the five species being measured is presented.

Prinn, R. G.↗

The Atmospheric Lifetime Experiment. II - Calibration

The calibration standards used in the Atmospheric Lifetime Experiment (ALE) for CFCl3, CF2Cl2, CH3CCl3, and CCl4 are described. This includes the preparation of the primary standards by static dilution and their propagation and stability for the period 1977-1982. Two independent assessments of the absolute concentrations of the primary standards used to initiate the ALE measurements in 1977-1978 are reported. For consistency in the ALE program the values assigned to the primary standards and subsequent working standards used in the field were not altered during the experiment when results of better estimates of the original concentration values were obtained. Rather, the appropriate factors by which the ALE mixing ratios for a given species should be multiplied to obtain the best estimate of the current concentration of a given species, are provided.

Rasmussen, R. A.↗

The atmospheric lifetime experiment. III - Lifetime methodology and application to three years of CFCL3 data

Observations of the chlorofluorocarbon CFCl3 obtained several times daily over the period July 1978 to June 1981 at Adrigole, Ireland; Ragged Point, Barbados; Point Matatula, American Samoa; and Cape Grim, Tasmania are reported. In addition, observations at Cape Meares, Oregon are given for the period January 1980 to June 1981. On January 1, 1980, the average mixing ratio of CFCl3 in the lower troposphere is esimated to have been 168 pptv, and this is calculated to have been increasing 5.7 percent annually. Assuming that the only destruction of CFCl3 occurs in the stratosphere, the lifetime, on January 1, 1980, estimated by a trend technique is 83 + 73, or -27 years; the lifetime estimated from the global inventory of CFCl3 is to + 89 or -25 years. The maximum likelihood current lifetime estimate obtained by combining the estimates from both analysis techniques is 78 years.

Cunnold, D. M.↗

The Atmospheric Lifetime Experiment. IV - Results for CF2Cl2 based on three years data

Observations of dichlorodifluoromethane obtained several times daily over the period July 1978 to June 1981 at Adrigole, Ireland (52 deg N, 10 deg W), Ragged Point, Barbados (13 deg N, 59 deg W), Point Matatula, American Samoa (14 deg S, 171 deg W), and Cape Grim, Tasmania (41 deg S, 145 deg E), are reported. Observations at Cape Meares, Oregon (45 deg N, 124 deg W), are also given for the period November 1980 to June 1981. On January 1, 1980, the average mixing ratio of dichlorodifluoromethane in the lower troposphere is estimated to have been 285 pptv and to have been increasing at 6.0 percent/year. The atmospheric lifetime of this compound is estimated from this data by adjusting its destruction rate in a two-dimensional model of the atmosphere so as to provide the best fit to the observations. Assuming destruction of CF2Cl2 in the stratosphere only, the lifetime estimate for January 1, 1980, by the inventory technique is 69 + 36 or - 18 years. The trend technique principally provides a lower limit to the lifetime of 81 years. The results suggest a need for further assessment of dichlorodifluoromethane release estimates, particularly those from the USSR and eastern Europe.

Cunnold, D. M.↗

Increase and seasonal cycles of nitrous oxide in the earth's atmosphere

It is determined that nitrous oxide (N2O) is increasing at about 0.9 ppb/yr in the northern hemisphere and at about 0.7 ppb/yr in the southern hemisphere, based on about 9000 ground-level measurements at Cape Meares, Oregon (45 deg N), and Cape Grim, Tasmania (42 deg S), spanning a three-year period. It is also shown that the N2O concentrations vary with season in the northern hemisphere, where the concentrations are 0.8 ppbv higher during April, May, and June compared to the rest of the year, and in the southern hemisphere where the concentrations are about 0.5 ppbv lower during March, April, and May compared to the rest of the year. An explanation of this increase as a sizeable anthropogenically-controlled land-based source is presented, based on an examination of the existing estimates of natural and anthropogenic sources of N2O. Mass-balance calculations are also presented which suggest that a natural land-based source, peaking in spring, would explain the main features of the observed seasonal cycle. A growth model is employed to extrapolate the observed increase of N2O into the future and the results are compared with exponential extrapolations.

Khalil, M. A. K.↗

Sources, sinks, and seasonal cycles of atmospheric methane

It is shown that a lifetime of approximately 8 years is most consistent with the observed latitudinal variation of atmospheric methane, requiring the current global emissions of methane to be around 550 teragrams per year. The repeating pattern of a rapid rise of CH4 concentrations in the fall in the Northern Hemisphere indicates a large fall source at latitudes above 30 deg N. The remaining observed seasonal variations are seen as consistent with the seasonal cycle of OH, which removes methane from the atmosphere. An extensive set of self-consistent measurements of methane is reported and analyzed, revealing that methane has increased during the past 3-4 years at rates of 1-1.9 percent per year all over the world at sites ranging from inside the Arctic Circle to the South Pole. The observational results are used in estimating the sources, sinks, and seasonal cycles of CH4 and the effects of human activities on its atmospheric abundance.

Khalil, M. A. K.↗

Natural and anthropogenic trace gases in the southern hemisphere

The complexity of the global environment makes it necessary that many important trace gases in the earth's atmosphere be measured on a global scale before predictions can be made regarding the effects of human activities on the environment. A description is presented of measurements of 14 atmospheric trace gases in the lower atmosphere (0-4 km) of the southern hemisphere. Concentrations are considered of CCl3F, CCl2F2, CHClF2, C2.Cl3.F3, CH3CCl3, CCl4, C2.Cl4, CH3I, CHCl3, CO, CH3Cl, CH4, N2O, and OCS. The obtained data are analyzed and interpreted to statistically quantify the possible differences of concentrations in and above the boundary layer, to model the vertical profile of CH3I, and to use the data in support of previous findings that CH4 is increasing in the atmosphere.

Rasmussen, R. A.↗

Atmospheric methyl iodide /CH3I/

It is found that atmospheric concentrations of CH3I are not greater than about 3 pptv over most of the earth's surface and drop to less than half this value above the boundary layer, suggesting that the compound is not likely to play such important roles, on a global scale, as the destruction of tropospheric O3 and free radicals and the increasing of the NO2/NO ratio and hydroxyl radical densities. It is hypothesized that a large portion of the global CH3I comes from oceanic regions of high biomass productivity, where the compound may play a key role in local atmospheric chemistry. Attention is given to CH3I measurement uncertainties with regard to global distribution, sources, and sinks.

Rasmussen, R. A.↗

Atmospheric methane /CH4/ - Trends and seasonal cycles

On the basis of 22 months of almost continuous automated, GC/FID measurements of atmospheric CH4 and Cape Meares (45 deg N), it is shown that the concentration of CH4 is increasing at about 2% per yr (+ or - 0.5%/yr). The data also revealed stable seasonal cycles with peak concentrations in October and minimum concentrations in July. The magnitude of the seasonal variations during these months is about + or - 20 ppby from the average (+ or - 1.2%). If the current trend continues, the increased CH4 concentration may result in a 0.2 K to 0.4 K average increase in earth's surface temperature over the next 40 years or so (based on calculations of Wang et al. (1976)). The coupling of CH4 to tropospheric and stratospheric chemical processes is discussed.

Rasmussen, R. A.↗

Trends of atmospheric methane in the Southern Hemisphere

Atmospheric observations spanning the past three years show that methane increased at 1.2 (plus or minus 0.3)% per year at Cape Grim in Tasmania (41 deg S). This rate of increase can be compared to the 1.9 (plus or minus 0.4)% per year observed at Cape Meares in Oregon (45 deg N) over the past two years. Over the corresponding period the concentration at Cape Grim increased by 1.4 (plus or minus 0.4)% per year. The Southern Hemisphere data also suggest seasonal variations with minimum concentrations in March and maximum in September. These results are based on 26 large-volume stable air samples collected cryogenically in stainless steel flasks and 75 smaller-volume air samples collected in glass flasks, all analyzed by a gas chromatograph using a flame ionization detector.

Fraser, P. J.↗

Global atmospheric distribution and trend of methylchloroform /CH3CCl3/

Results of global measurements of the concentration of atmospheric methylchloroform, a man-made gas with potentially harmful environmental consequences, performed over a two-year period are presented. Samples were collected weekly at Pt. Barrow and Poker Flats, Alaska, Cape Meares, Oregon, Cape Kumakahi, Hawaii, Samoa, and Cape Grim, Tasmania, and yearly at the South Pole, and methylchloroform concentrations were determined by electron capture-gas chromatographic techniques. A latitudinal profile of CH3CCl3 concentrations derived from the data exhibits a bump at high northern latitudes, where most of the sources are located. Average concentrations calculated for the Northern and Southern Hemispheres showed a rise in global concentrations at a rate of 6.7 + or - 2.0%/year for the period from January 1979 to January 1981, with concentrations rising more slowly in 1980 than in 1979. These yearly increases are also smaller than earlier rates of increase, explainable by a reduction in the rate of emission increase, and are consistent with an atmospheric lifetime of between 6 and 10 years.

Rasmussen, R. A.↗

Atmospheric trace gases - Possibility of sources in the Southern Hemisphere

When measurements of globally distributed trace gases establish their existence in the Southern Hemisphere, it is not always clear whether their presence is due to transport from the Northern Hemisphere or partly from significant sources in the Southern Hemisphere. In this paper a simple criterion is developed whereby one can determine if significant Southern Hemisphere sources exist for a given trace gas. Despite the limitations of the model, there are strong indications that C2 hydrocarbons (C2H2, C2H4, C2H6), CO and CH4 have significant Southern Hemisphere sources.

Khalil, M. A. K.↗

Interlaboratory comparison of fluorocarbons-11, -12, methylchloroform and nitrous oxide measurements

Measurements conducted by 19 participating laboratories were considered in the reported interlaboratory comparison study. The results show that there is considerable disagreement among laboratories regarding the absolute concentrations of all four trace gases (CCl3F, CCl2F2, H3CCl3, N2O). The magnitude of this disagreement is discussed. Laboratories in Group II showed considerable disagreement among themselves. Their results were scattered within large intervals of concentration. Laboratories in Group I (using common standards) were in excellent (+ or - 5%) agreement among themselves. A systematic disagreement was noted between Groups I and II laboratories. Generally, the mean values of concentrations determined from the measurements of Group II laboratories were lower than the mean values reported by Group I laboratories.

Rasmussen, R. A.↗

Differences in the concentrations of atmospheric trace gases in and above the tropical boundary layer

Weekly air samples were collected at Cape Kumakahi (0 km) and at nearby Mauna Loa Observatory (3.4 km) which is above the boundary layer. EC/GC and GC/FID techniques were used to measure CH3I, CHCl3, CO and CH4 which are largely natural in origin, and C2Cl4, CCl4, CH3CCl3, (F-11), CCl2F2, (F-12), CHClF, (F-22) and C2F3Cl3 (F-113), which are due to anthropogenic (CCl3F) etc. activities. It was found that all these gases are significantly (alpha is equal to or less than 0.05) more abundant in the boundary layer than above it.

Rasmussen, R. A.↗

Concentration distribution of methyl chloride in the atmosphere

Electron capture gas chromatography techniques were used to obtain measurements of methyl chloride concentrations in the atmosphere, at latitudes ranging from about 65 N to 90 S. Most of the measurements were made over the Pacific Ocean. Average global concentrations within the boundary layer were found to be 815 plus or minus 25 pptv in 1977 and 755 plus or minus 37 pptv in 1978. Lower concentrations were observed above the boundary layer with average values of 629 plus or minus 23 pptv and 618 plus or minus 23 pptv in 1977 and 1978, respectively. Within 20 deg of the equator, the boundary layer concentrations were significantly higher than those above the boundary layer. The sources, the sinks, the budgets, and the latitudinal distributions of methyl chloride are discussed in the paper.

Rasmussen, R. A.↗

CHClF2 /F-22/ in the earth's atmosphere

Recent global measurements of CHClF2 (F-22) are reported. Originally, GC/MS techniques were used to obtain these data. Since then, significant advances using an O2-doped electron capture detector have been made in the analytical techniques, so that F-22 can be measured by EC/GC methods at ambient concentrations. The atmospheric burden of F-22 calculated from these measurements (average mixing ratio, mid-1979, approximately 45 pptv) is considerably greater than that expected from the estimates of direct industrial emissions (average mixing ratio, mid-1979, approximately 30 pptv). This difference is probably due to underestimates of F-22 emissions.

Rasmussen, R. A.↗

Nitrous oxide measurements in the eastern tropical Pacific Ocean

The paper considers nitrous oxide measurements in the eastern tropical Pacific Ocean. The concentration of N2O in the marine air showed a direct relationship to the N2O in the surface sea water, with the highest N2O mixing ratios over highly supersaturated regions; water samples were also collected down to depths of 300 m at seven hydrocast stations. The stations showed two distribution patterns for N2O concentration vs depth for the region between the surface and 300 m; two stations in the oxygen deficient region off the coast of Peru showed considerable N2O super-saturation at all depths, and results indicate that the role of N2O in the nitrogen cycle of the ocean may be more complex than previously suggested.

Pierotti, D.↗