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Studies of the air and water chemistry in the Amazon region of Brazil were undertaken. Harvard scientists were invited to participate in several experiments at INPA facilities, at other sites in Brazil, and aboard the RV Calypso of the Cousteau Society. Expeditions and participants are summarized.
Soils in an Amazonian rainforest are observed to release N2O at a rate larger than the global mean by about a factor of 20. Emissions from a New England hardwood forest are approximately 30 times smaller then Brazilian values. Atmospheric methane is consumed by soils in both systems. Tropical forests would provide a major source of atmospheric N2O if the Brazilian results are representative.
The basic processes that cause N2O emission from soils are briefly discussed, and the rate of the processes is shown to vary widely in space and time, depending on soil, climate, and agrotechnical conditions. Although significant amounts of N2O are indeed emitted from the land, the complexity of the soil processes involved and the wide variation of measured rates still prevents the quantitative evaluation, global budgeting, and reliable prediction of atmospheric N2O. Increased atmospheric N2O abundance increases the levels of odd-nitrogen in the stratosphere, which, in turn, decreases the stratospheric ozone density via a catalytic cycle. Using appropriate atmospheric models and current chemical kinetic data, it has been found that the dependence of ozone reduction on N2O increase is nearly linear; a simulated doubling of N2O leads to a predicted decrease of about 14 percent in total ozone column density. A 10 percent increase in N2O yields a predicted increase in nonmelanoma skin cancer of several percent, and a possible raising of surface temperature of 0.03 K.
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Estimates of continental sources of CFC-11, CFC-12, CCl4, CH3CCl3 and N2O are derived from the atmospheric lifetime experiment in Adrigole, Ireland, and anthropogenic emissions of CCl4 and N2O from Europe have been identified. Relative source strengths are consistent with global budgets for the halocarbons and N2O. Different industrial release patterns for halocarbons are observed for Europe, the western United States and Australia.
Daytime and nighttime vertical profiles of the tropospheric trace gas N2O were determined from grab sample collections off the Atlantic and Gulf coasts of Florida. The grab samples were collected during the week of October 7-13, 1984, from a Lear jet during descent spirals over an altitude range of 12.5-0.3 km in approximately 1.2-km intervals. During this period there were two distinct airflow regimes sampled: (1) the surface boundary layer (less than 2 km), in which the wind direction was typically easterly; and (2) the regime above the boundary layer, which was predominantly characterized by westerly flow. N2O mixing ratios, normalized to dry air, were determined from 148 daytime and nighttime samplings. N2O was found to be uniformly mixed at all altitudes at 301.9 + or - 2.4 parts per billion by volume.
Measurements of stratospheric N2O were made from Mauna Kea in Hawaii in June 1983, and in May and June 1986, by observing thermal emission of the molecule in a rotational transition at about 1 mm wavelength. Analyses of the data yield altitude profiles in the middle and upper stratosphere. Useful measurements of N2O may be made in one to two hours. The N2O profiles agree reasonably well with model predictions and with published satellite data, though significantly more N2O is reported near the stratopause than shown by the satellite measurement, and significantly more N2O in the middle stratosphere than in one of the models. The discrepancy between these data and the satellite measurement may be due in part to variations induced by the solar cycle.
New information on seasonal and secular trends in the releases of CFCl3, CF2Cl2, CCl4, CH3CCl3, and N20 from Europe was obtained as part of the Atmospheric Lifetime Experiment. Semicontinuous measurements of these pollutants were made at Adrigole, Ireland, using lean air from the Atlantic Ocean as a baseline. The results obtained include unambiguous evidence for elevated levels of N2O occurring concurrent with halocarbon pollution events; the detection of trends in the relative emission of different halocarbons; the discovery of seasonal variations in emission of CF2Cl2, CCl4, and CH3Cl3; the characterization of typical summer and winter pollution episodes; and the identification of weather patterns over Europe that are associated with high concentrations of chlorofluorocarbons at Adrigole. It was estimated that the European source of N2O represents 25 percent of the global emissions associated with combustion and 10 percent of the integrated stratospheric losses.
The chemical lifetime of N2O is about 150 years, which makes it an excellent dynamical tracer of air motion on the time scale of the ozone depletion event. For these reasons it was chosen to help test whether dynamical theories of ozone loss over Antarctica were plausible, particularly the theory that upwelling ozone-poor air from the troposphere was replacing ozone-rich stratospheric air. The N2O measurements were made with the Airborne Tunable Laser Absorption Spectrometer (ATLAS) aboard the NASA ER-2 aircraft. The detection technique involves measuring the diffential absorption of the IR laser radiation as it is rapidly scanned over an N2O absorption feature. For the AAOE mission, the instrument was capable of making measurements with a 1 ppb sensitivity, 1 second response time, over an altitude range of 10 to 20 kilometers. The AAOE mission consisted of a series of 12 flights from Punta Arenas (53S) into the polar vortex (approximately 72S) at which time a vertical profile from 65 to 45 km and back was performed. Comparison of the observed profiles inside the vortex with N2O profiles obtained by balloon flights during the austral summer showed that an overall subsidence had occurred during the winter of about 5 to 6 km. Also, over the course of the mission (mid-August to late September), no trend in the N2O vertical profile, either upward or downward, was discernible, eliminating the possibility that upwelling was the cause of the observed ozone decrease.
In situ N2O measurements were made using an airborne tunable laser absorption spectrometer (ATLAS) on 12 flights into the Antarctic vortex, as well as on five transit flights outside the vortex region in August and September 1987, as part of the Airborne Antartic Ozone Experiment. Vertical profiles of N2O were obtained within the vortex on most of these flights and were obtained outside the vortex on several occasions. Flights into the vortex region show N2O decreasing southward between 53 and 72 S latitude on constant potential temperature surfaces in the lower stratosphere. The data lead to two important conclusions about the vortex region: (1) the lower stratosphere in August/September 1987 was occupied by 'old' air, which had subsided several kilometers during polar winter; (2) the N2O profile in the vortex was in an approximately steady state in August/September 1987, which indicates that the spring upwelling, suggested by several theories, did not occur.
The importance of seasonal cycles of N2O flux from tropical ecosystems and the possibility that tropical deforestation could contribute to the ongoing global increase in N2O concentrations were assessed by measuring N2O flux from forest, cleared land, and pasture over an annual cycle in the central Amazon. A pasture that had been converted from tropical forest had threefold greater annual N2O flux than a paired forest site; similar results were obtained in spot measurements in other pastures. If these results are general, such tropical pastures represent a globally significant source of increased N2O.
The recent discovery of an artifact producing increased levels of N2O in combustion gas samples collected and stored in grab bottles before chemical analysis has resulted in the downgrading of fossil-fuel combustion and the questioning of biomass burning as important sources of N2O. As almost all reported analyses of N2O produced from biomass burning have involved essentially the same collection and analysis protocols as used in the fossil-fuel studies, this source of N2O must also be reexamined. Here, measurements of N2O made over a large prescribed fire using a near real-time in situ measurement technique are reported and compared with measurements of N2O from simultaneously collected grab-bottle samples. The results from 27 small laboratory biomass test fires are also used to help clarify the validity of earlier assessments. It is concluded that biomass burning contributes about seven percent of atmospheric N2O, as opposed to earlier estimates of several times this value.
Measurements of CH4 uptake and N2O emissions in native, nitrogen-fertilized, and wheat-growing prairie soils from spring to late autumn, 1990 are reported. It is found that nitrogen fertilization and cultivation can both decrease CH4 uptake and increase N2O production, thereby contributing to the increasing atmospheric concentrations of these gases.
A linear reference relationship between O3 and N2O has been used to estimate polar winter O3 loss from aircraft data taken in the lower stratosphere. Here, this relationship is evaluated at high latitudes by comparing it with a 2D model simulation and with NIMBUS 7 satellite measurements. Although comparisons with satellite measurements are limited to January through May, the model simulations are compared during other seasons. The model simulations and the satellite data are found to be consistent with the winter O3 loss analysis. It is shown that such analyses are likely to be inappropriate during other seasons.
A study has been conducted which compared N2O results obtained over large prescribed fires or wildfires, in which 'grab-sampling' with storage had been used with N2O measurements made in near-real time. CO2-normalized emission ratios obtained initially from the laboratory fires are substantially lower than those obtained over large-scale biomass fires. Combustion may not be the only source of N2O in large fire smoke plumes; physical, chemical, and biochemical processes in the soil may be altered by large biomass fires, leading to large N2O releases.
Simulations of N2O and CO2 emissions from soils were conducted with a rain-event driven, process-oriented model (DNDC) of nitrogen and carbon cycling processes in soils. The magnitude and trends of simulated N2O (or N2O + N2) and CO2 emissions were consistent with the results obtained in field experiments. The successful simulation of these emissions from the range of soil types examined demonstrates that the DNDC will be a useful tool for the study of linkages among climate, soil-atmosphere interactions, land use, and trace gas fluxes.
The NASA Langley 3D GCM chemical transport model is used to investigate the distribution of atmospheric N2O up to 60 km altitude. The transport characteristics of the model is evaluated without the complications of a detailed chemical formulation for all of the relevant stratospheric minor constituents. Interpretation of the yearly average zonal mean N2O distribution in terms of transport by the yearly averaged meridional circulation and stratospheric photochemical loss indicates large regions in the Northern Hemisphere stratosphere where dynamical mixing apparently plays a large role in maintaining the N2O distribution. In these regions, slopes of the N2O mixing ratio isopleths are maintained by competition between advection by the meridional circulation acting to steepen and dynamical mixing acting to flatten the slopes.