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At least 181 records · Page 10

The effects of fire on biogenic soil emissions of nitric oxide and nitrous oxide

Measurements of biogenic soil emissions of nitric oxide (NO) and nitrous oxide (N2O) before and after a controlled burn conducted in a chaparral ecosystem on June 22, 1987, showed significantly enhanced emissions of both gases after the burn. Mean NO emissions from heavily burned and wetted (to simulate rainfall) sites exceeded 40 ng N/sq m s, and increase of 2 to 3 compared to preburn wetted site measurements. N2O emissions from burned and wetted sites ranged from 9 to 22 ng N/sq m s. Preburn N2O emissions from these wetted sites were all below the detection level of the instrumentation, indicating a flux below 2 ng N/sq m s. The flux of NO exceeded the N2O flux from burned wetted sites by factors ranging from 2.7 to 3.4. These measurements, coupled with preburn and postburn measurements of ammonium and nitrate in the soil of this chaparral ecosystem and measurements of NO and N2O emissions obtained under controlled laboratory conditions, suggest that the postfire enhancement of NO and N2O emissions is due to production of these gases by nitrifying bacteria.

Levine, Joel S.↗

Exchange of nitrous oxide within the Hudson Bay lowland

The source strength of atmospheric trace gases from natural ecosystems must be quantified in order to assess the effect of such inputs on the background tropospheric chemistry. A static chamber technique and a gas exchange technique were used to determine the emissions of nitrous oxide from five sites within the Hudson Bay Lowland, as part of the Northern Wetland Study. Two mechanisms, one diffusive and the other episodic, were found likely to be responsible for the emissions of nitrous oxide. The annual diffusive flux ranged from -3.8 mg(N2O)/sq m in a treed bog to 7.9 mg(N2O)/sq m in an open fen. The addition of the episodic flux, increased this range to -2.1 mg(N2O)/sq m and 18.5 mg(N2O)/sq m respectively. These episodic emissions occurred in from 2.5% to 16.7% of the samples during the late summer peak emission period. Since the gas exchange rate could not detect the episodic emissions, it was found to be a poor method for water emission rate determination within the wetland. LANDSAT-Thermatic Mapper (TM) imagery was used to scale the emissions, from the chamber level to an integrated average over the entire Hudson Bay Lowland. The total emission rate of N2O from the Hudson Bay Lowland, was determined to be 1.2 Gg(N2O)/year, of which 80% was attributed to episodic emissions.

Schiller, C. L.↗

Evolution of the 1991-1992 Arctic vortex and comparison with the Geophysical Fluid Dynamics Laboratory SKYHI general circulation model

Nitrous oxide (N2O) measured on board the ER-2 aircraft during the Airborne Arctic Stratospheric Expedition 2 (AASE 2) has been used to monitor descent of air inside the Arctic vortex between October 1991 and March 1992. Monthly mean N2O fields are calculated from the flight data and then compared with mean fields calculated from the high-resolution Geophysical Fluid Dynamics Laboratory general circulation model SKYHI in order to evaluate the model's simulation of the polar vortex. From late fall through winter the model vortex evolves in much the same way as the 1991-1992 vortex, with N2O gradients at the edge becoming progressively steeper. The October to March trends in N2O profiles inside the vortex are used to verify daily net heating rates in the vortex that were computed from clear sky radiative heating rates and National Meteorological Center temperature observations. The computed heating rates successfully estimate the descent of vortex air from December through February but suggest that before December, air at high latitudes may not be isolated from the midlatitudes. SKYHI heating rates are in good agreement with the computed rates but tend to be slightly higher (i.e., less cooling) due to meteorological differences between SKYHI and the 1991-1992 winter. Three ER-2 flights measured N2O just north of the subtropical jet. These low-midlatitude profiles show only slight differences from the high-midlatitude profiles (45 deg - 60 deg N), indicating strong meridional mixing in the midlatitude 'surf zone.' Mean midwinter N2O profiles inside and outside the vortex calculated from AASE 2 data are shown to be nearly identical to 1989 AASE profiles, pointing to the N2O/potential temperature relationship as an excellent marker for vortex air.

Strahan, S. E.↗

Infrared Radiative Forcing and Atmospheric Lifetimes of Trace Species Based on Observations from UARS

Observations from instruments on the Upper Atmosphere Research Satellite (UARS) have been used to constrain calculations of infrared radiative forcing by CH4, CCl2F2 and N2O, and to determine lifetimes Of CCl2F2 and N2O- Radiative forcing is calculated as a change in net infrared flux at the tropopause that results from an increase in trace gas amount from pre-industrial (1750) to contemporary (1992) times. Latitudinal and seasonal variations are considered explicitly, using distributions of trace gases and temperature in the stratosphere from UARS measurements and seasonally averaged cloud statistics from the International Satellite Cloud Climatology Project. Top-of-atmosphere fluxes calculated for the contemporary period are in good agreement with satellite measurements from the Earth Radiation Budget Experiment. Globally averaged values of the radiative forcing are 0.536, 0.125, and 0.108 W m-2 for CH4, CCl2F2, and N2O, respectively. The largest forcing occurs near subtropical latitudes during summer, predominantly as a result of the combination of cloud-free skies and a high, cold tropopause. Clouds are found to play a significant role in regulating infrared forcing, reducing the magnitude of the forcing by 30-40% compared to the case of clear skies. The vertical profile of CCl2F2 is important in determining its radiative forcing; use of a height-independent mixing ratio in the stratosphere leads to an over prediction of the forcing by 10%. The impact of stratospheric profiles on radiative forcing by CH4 and N2O is less than 2%. UARS-based distributions of CCl2F2 and N2O are used also to determine global destruction rates and instantaneous lifetimes of these gases. Rates of photolytic destruction in the stratosphere are calculated using solar ultraviolet irradiances measured on UARS and a line-by-line model of absorption in the oxygen Schumann-Runge bands. Lifetimes are 114 +/- 22 and 118 +/- 25 years for CCl2F2 and N2O, respectively.

Minschwaner, K.↗

Evaluation of Relative Sensitivity of SAW and Flexural Plate Wave Devices for Atmospheric Sensing

The objective of this project is to evaluate the suitability of the ultrasonic flexural plate wave (FPW) device as the detector in a gas chromatograph (GC). Of particular interest is the detection of nitrous oxide (N2O). From experimental results we conclude analyte detection is achieved through two mechanisms: changes in gas density, and mass loading of the device membrane due to the sorption of gas molecules. Reducing the dead volume of the FPW chamber increased the FPW response. A comparison of the FPW response to that of the surface acoustic wave (SAW) detector provided with the GC (made by MSI, Microsensor Technologies, Inc.), shows that for unseparated N2O in N2, the FPW exhibits a sensitivity that is at least 550 times greater than that of the SAW device. A Porapak Q column was found to separate N2O from its carrier gas, N2 or He. With the Porapak Q column, a coated FPW detected 1 ppm N2O in N2 or He, with a response magnitude of 7 Hz. A coated SAW exhibited a response of 25 Hz to pure N2O. The minimal detectable N2O concentrations of the sensors were not evaluated.

White, Richard M.↗

The photolysis of CH3ONO

The photolysis of CH3ONO, alone and in the presence of NO, NO-N2 mixtures, and NO-CO mixtures was studied between 25 and 150 C. The major products are CH2O, N2O, and H2O. The quantum yields of N2O were measured. The N2O yield is large at low pressures but approaches a high-pressure limiting value of 0.055 at all temperatures as the excited CH3O produced in the primary step is stabilized by collision. In the presence of excess CO, and N2O yield drops, and CO2 is produced (though not in sufficient amounts to account for the drop in N2O). When pure CH2ONO is photolyzed, CO is produced and NO accumulates in the system. Both products are formed in related processes and result from CH3O attack on CH2O.

Wiebe, H. A.↗

Reaction of NH2 with NO and O2

Experiments were performed on the photooxidation of NH3 at room temperature and the photolysis of NH3-NO mixtures in order to determine the reaction paths of NH2 with O2. NH3 was photolyzed (NH3 + E yields NH2 + H) in the presence of O2 above 0.6 torr at 213.9 nm and 25 C, producing N2 and N2O. Only N2 and N2O were produced with any significant quantum yield, and their quantum yield was invariant with reaction conditions, which imposes a great number of constraints reducing the number of possible reactions greatly. It is argued that the N2 must be produced from the NH2O2 radical which was produced by the reaction between NH2 and O2. Subsequent reactions leading to N2 and N2O are speculative. In the photolysis of NH3 in the presence of NO and NO-O2 mixtures, the products identified were N2, H2, and N2O. Without the presence of O2, the reaction scheme after photolysis is (2) NH2 + NO yields N2 + H2O, (3) H + NO + M yields HNO + M, (4) H + HNO yields H2 + NO, and (5) 2HNO yields N2O + H2O. The average value for the ratio k3 times the square root of k5 divided by k4 was computed to be (1.6 plus or minus 0.6) times 10 to the minus 28th cm to the exponent 9/2 per square root sec. In addition, the presence of 113 mtorr of O2 had no effect on the quantum yields of N2 or H2, so it appears that it does not deactivate electronically excited NH3.

Jayanty, R. K. M.↗

The photochemistry of biogenic gases in the early and present atmosphere

The distribution of gases in the prebiologial paleoatmosphere is investigated using photochemical models. A chart of the photochemical and chemical reactions and reaction rates for CH4, NH3, H2S, N2O, and CO atmospheric gases is given. Mixing ratios and surface mixing ratios for CH4, NH3, CO, and N2O are obtained using thermodynamic equilibrium calculations; an increase in CH4 and N2O is observed. The reactions, which explain the photochemistry of the gases studied, are presented. The sources of these gases and their concentration with regards to altitude are examined. Graphs of the vertical distribution of CH4, NH3, H2S, CO, O2, and N2O in prebiological paleoatmosphere are provided. The data reveals the presence of only N2, CO2, and N2O in the early atmosphere; with the evolution of life, sources of atmospheric gases increased and their influence on the photochemistry of the troposphere and stratosphere increased.

Levine, J. S.↗

Nitrous oxide in the tropical middle atmosphere, observed by ground-based mm-wave spectrometry

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.

Connor, Brian J.↗

Southern Hemispheric nitrous oxide measurements obtained during 1987 airborne Antarctic ozone experiment

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.

Podolske, J. R.↗

Temporal trends and transport within and around the Antarctic polar vortex during the formation of the 1987 Antarctic ozone hole

During AAOE in 1987 an ER-2 high altitude aircraft made twelve flights out of Punta Arenas, Chile (53 S, 71 W) into the Antarctic polar vortex. The aircraft was fitted with fast response instruments for in situ measurements of many trace species including O3, ClO, BrO, NO sub y, NO, H2O, and N2O. Grab samples of long-lived tracers were also taken and a scanning microwave radiometer measured temperatures above and below the aircraft. Temperature, pressure, and wind measurements were also made on the flight tracks. Most of these flights were flown to 72 S, at a constant potential temperature, followed by a dip to a lower altitude and again assuming a sometimes different potential temperature for the return leg. The potential temperature chosen was 425 K (17 to 18 km) on 12 of the flight legs, and 5 of the flight legs were flown at 450 K (18 to 19 km). The remaining 7 legs of the 12 flights were not flown on constant potential temperature surfaces. Tracer data have been analyzed for temporal trends. Data from the ascents out of Punta Arenas, the constant potential temperature flight legs, and the dips within the vortex are used to compare tracer values inside and outside the vortex, both with respect to constant potential temperature and constant N2O. The time trend during the one-month period of August 23 through September 22, 1987, shows that ozone decreased by 50 percent or more at altitudes form 15 to 19 km. This trend is evident whether analyzed with respect to constant potential temperature or constant N2O. The trend analysis for ozone outside the vortex shows no downward trend during this period. The analysis for N2O at a constant potential temperature indicates no significant trend either inside or outside the vortex; however, a decrease in N2O with an increase in latitude is evident.

Proffitt, M. H.↗

Nitrous oxide flux following tropical land clearing

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.

Luizao, Flavio↗

Seasonal nitrous oxide flux from an intensively managed pasture in a humid subtropical ecosystem

Nitrous oxide (N2O) flux from vented chambers was measured over intensively and minimally managed bermuda grass hay meadows in a humid, subtropical ecosystem for several years during scheduled sampling protocol following harvest, fertilization and rainfall events while measuring diel N2O emissions once during each of 5 seasonal day growth cycles which divided each calendar year. Soil pools of nitrite NO2(-), nitrate NO3(-), and ammonia (NH3) were measured in soil samples taken at 2 and 10 cm depths during each emission collection to determine transformations of the nitrogen pools coupled with N2O emissions. The highest diel N2O emission occur midday in the Spring cycle, measuring 9.0 g N/ha/d only for several weeks, while emissions dropped to less than 1.0 g N/ha/day during hot, dry, and colder months. Intensively managed meadows (4 fertilizations and harvests per year plus pest management) induced higher seasonal N2O emissions than minimal treatment (1 fertilization and harvest) averaging 2.75 and 5.97 g N/ha/day. Nitrous oxide emission data as responses to soil parameters and environmental parameters were also measured where air temperature, soil moisture, and fertilization were the most powerful factors.

Brams, Eugene A.↗

Atmospheric emissions and trends of nitrous oxide deduced from 10 years of ALE-GAGE data

Long-term measurements of nitrous oxide (N2O) obtained during the Atmospheric Lifetime Experiment (ALE) and the Global Atmospheric Gases Experiment (GAGE) for a period from 1978 to 1988 are presented and interpreted. It is observed that the average concentration in the Northern Hemisphere is 0.75 +/- 0.16 ppbv higher than in the Southern Hemisphere and that the global average linear trend in N2O lies in the range from 0.25 to 0.31 percent/year. The measured trends and latitudinal distributions are shown to be consistent with the hypothesis that stratospheric photodissociation is the major atmospheric sink for N2O, while the cause of the N2O trend is suggested to be a combination of a growing tropical source and a growing Northern mid-latitude source. A 10-year average global N2O emission rate of (20.5 +/- 2.4) x 10 to the 12th g N2O/year is deduced from the ALE/GAGE data.

Prinn, R.↗

Contributions of a Tunable Diode Laser Instrument (ATLAS) to the Stratospheric Ozone Depletion Question

The Airborne Tunable Laser Absorption Spectrometer - ATLAS - was designed and built at the NASA Ames Research Center and operates on the NASA ER-2 high altitude research aircraft. ATLAS has taken part in a number of important polar and mid-latitude research campaigns, since 1987, focused on various aspects of stratospheric ozone chemistry and dynamics. The chief measurement carried out by the ATLAS second harmonic diode laser spectrometer is of the important atmospheric tracer N2O. Using N2O as an inert tracer we have been able to gain significant new information on polar vortex dynamics and on the correlations of several important long-lived tracers in the stratosphere. The correlation of N2O with NOy (total reactive nitrogen) has been shown to be linear for a great variety of unperturbed stratospheric conditions, and the breakdown of this correlation has been used to detect denitrification by PSCs in the polar vortex, especially in the Antarctic spring. Denitrification is an important step in the process of ozone hole formation in the austral spring. Correlations of N2O with CFCs and CH4 have led to improved estimates of atmospheric lifetimes of these important molecules. Finally the correlation of N2O with CO2, the latter now being measured with great precision by a new instrument on the ER-2, has led to a significant new tool for studying horizontal and vertical mixing in the lower stratosphere, a tool which is very useful in assessing the potential effects of high speed civil transport aircraft in the lower stratosphere. A new, light-weight version of ATLAS is currently being built for unmanned high altitude aircraft, specifically the new Perseus vehicle. We will give a brief description of this effort.

Loewenstein, Max↗

Tropospheric sources of NOx: lightning and biology

Laboratory experiments to quantify the global production of NOx (NO + NO2) in the troposphere due to atmospheric lightning and biogenic activity in soil are presented. These laboratory experiments, as well as other studies, suggest that the global production of NOx by lightning probably ranges between 2 and 20 MT(N)y-1 of NO and is strongly dependent on the total energy deposited by lightning, a quantity not well-known. In our laboratory experiments, nitrifying micro-organisms is soil were found to be a significant source of both NO and nitrous oxide (N2O). The measured production ratio of NO to N2O averaged 2-3 for oxygen partial pressures of 0.5-10%. Extrapolating these laboratory measurements to the global scale, which is somewhat risky, suggests that nitrifying micro-organisms in soil may account for as much as 10 MT(N) y-1 of NO. Additional experiments with denitrifying micro-organisms gave an NO to N2O production ratio ranging from 2 to 4 for an oxygen partial pressure of 0.5% and a ratio of less than unity for oxygen partial pressures ranging from 1 to 20%. The production of NO and N2O, normalized with respect to micro-organism number indicates that the production of both NO and N2O by denitrifying micro-organisms is at least an order of magnitude less than production by nitrifying micro-organisms for the micro-organisms studied.

Atmosphere/chemistry↗

A Model Study of the Impact of Source Gas Changes on the Stratosphere for 1850-2100

The long term stratospheric impacts due to emissions of CO2, CH4, N2O, and ozone depleting substances (ODSs) are investigated using an updated version of the Goddard two-dimensional (2D) model. Perturbation simulations with the ODSs, CO2, CH4, and N2O varied individually are performed to isolate the relative roles of these gases in driving stratospheric changes over the 1850-2100 time period. We also show comparisons with observations and the God- 40 dard Earth Observing System chemistry-climate model simulations for the time period 1970-2100 to illustrate that the 2D model captures the basic processes responsible for longterm stratospheric change. The 2D simulations indicate that prior to 1940, the 45 ozone increases due to CO2 and CH4 loading outpace the ozone losses due to increasing N2O and carbon tetrachloride (CCl4) emissions, so that ozone reaches a broad maximum during the 1920s-1930s. This preceeds the significant ozone depletion during approx. 1960-2050 driven by the ODS loading. During the latter half of the 21st century as ODS emissions diminish, CO2, N2O, and CH4 loading will all have significant impacts on global total ozone based on the IPCC AIB (medium) scenario, with CO2 having the largest individual effect. Sensitivity tests illustrate that due to the strong chemical interaction between methane and chlorine, the CH4 impact on total ozone becomes significantly more positive with larger ODS loading. The model simulations also show that changes in stratospheric temperature, Brewer-Dobson circulation (BDC), and age of air during 1850-2100 are controlled mainly by the CO2 and ODS loading. The simulated acceleration of the BDC causes the age of air to decrease by approx. 1 year from 1860-2100. The corresponding photochemical lifetimes of N2O, CFCl3, CF2Cl2, and CCl4 decrease by 11-13% during 1960-2100 due to the acceleration of the BDC, with much smaller lifetime changes 4%) caused by changes in the photochemical loss rates.

Fleming, E. L.↗

germs-lab/PAPER_miscanthus_soil_response

Nutrient inputs influence the sustainability of bioenergy crop production through contemporary (shortly after addition) and legacy effects (persisting over years) on microbial nitrogen (N) and carbon cycling, which contribute to greenhouse gas emissions. However, the relative importance of contemporary and legacy effects and how that could vary by crop functional types is poorly understood. Considering its rhizomatous roots and perennial growth, we hypothesized that Miscanthus × giganteus (M×g) would be more sensitive to legacy N fertilization and the historical context of its environment than an annual crop like maize. To test this hypothesis, we examined the effects of legacy and contemporary N inputs on nitrous oxide (N2O) and carbon dioxide (CO2) emissions, as well as key N cycling genes in soils where M×g and maize were grown. A 150-day soil incubation experiment was conducted using soils from a long-term M×g and maize fertility experiment with three historic N fertilization rates (0, 112, and 336 kg N ha−1 year−1) and a contemporary amendment (60 mg N kg−1) with negative control (0 mg N kg−1). We observed significant increases in cumulative N2O emissions in Mxg soils relative to maize soils, particularly at higher legacy fertilization rates, while contemporary N had no significant effect. Bacterial amoA gene abundance, which plays a significant role in nitrification in nutrient-rich soils, also increased with higher legacy fertilization rates in M×g soils but was unaffected by the contemporary N. In maize soils, legacy and contemporary N did not significantly affect N2O emissions, but cumulative CO2 emissions and amoA gene abundance significantly increased. The abundances of norB genes were not significantly influenced by either legacy fertilization or contemporary N amendments in either soil. Our findings demonstrate the greater importance of fertilization history over contemporary N in mediating soil N2O emissions, particularly for perennial bioenergy crops.

Lee, Jaejin↗