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1.
Direct measurements of nitrogen oxides and ozone fluxes over grassland   总被引：1，自引：0，他引：1  
Using the eddy correlation method, fluxes of nitric oxide, nitrogen dioxide, ozone, water, and sensible heat were measured at a site 20 km north of Denver, Colorado over mature crested wheat grass, 0.75 m high in late June and early July. During this period the weather was fair with no synoptic disturbances. In the early morning a well-mixed diluted urban pollution plume traversed the site, by late morning aged pollution had mixed downward into the local boundary layer, and by afternoon the air came from a relatively unpolluted area of the high plains. The mean trace gas concentrations reflect this repeated pattern of local air flow. The fluxes of the trace gases were influenced both by the variation of the means and by other factors including temperature and biological activity. Ozone fluxes were found to be always negative and proportional to the mean, with an average deposition velocity for this case of about 0.006 m s-1. For the oxides of nitrogen this simple treatment was not appropriate. Both deposition and emission were observed, generally deposition predominated in the morning and emission in the afternoon with observed variations in the fluxes of NOx=NO+NO2 from –0.3 to +0.2 ppbv m s-1.The National Center for Atmospheric Research is sponsored by the National Science Foundation  相似文献   

2.
We describe a fast response methane sensor based on the absorption of radiation generated with a near-infrared InGaAsP diode laser. The sensor uses an open path absorption region 0.5 m long; multiple pass optics provide an optical path of 50 m. High frequency wavelength modulation methods give stable signals with detection sensitivity (S/N=1, 1 Hz bandwidth) for methane of 65 ppb at atmospheric pressure and room temperature. Improvements in the optical stability are expected to lower the current detection limit. We used the new sensor to measure, by eddy correlation, the CH4 flux from a clay-capped sanitary landfill. Simultaneously we measured the flux of CO2 and H2O. From seven half-hourly periods of data collected after a rainstorm on November 23, 1991, the average flux of CH4 was 17 mmol m–2 hr–1 (6400 mg CH4 m–2 d–1) with a coefficient of variation of 25%. This measurement may underrepresent the flux by 15% due to roll-off of the sensor response at high frequency. The landfill was also a source of CO2 with an average flux of 8.1 mmol m–2 hr–1 (8550 mg CO2 m–2 d–1) and a coefficient of variation of 26%. A spectral analysis of the data collected from the CH4, CO2, and H2O sensors showed a strong similarity in the turbulent transfer mechanisms.  相似文献   

3.
A high resolution tunable diode laser absorption spectrometer (TDLAS) was used to measure the broadening effect of water vapor and other gases (dry air, nitrogen, oxygen, hydrogen and helium) on three methane lines in the v4 fundamental. The effects on methane eddy correlation flux measurements amount to a few percent for the least broadened line for expected H2O fluxes, to 10% for the most broadened line for higher H2O and lower CH4 fluxes likely to be encountered. The broadening coefficients of methane measured for air, N2, O2, and He are in good agreement with recently published values.  相似文献   

4.
This study focuses on the determination of optical depths caused by ozone and trace gases absorption in the Chappuis band, 500–700 nm, and the contribution to the Total Minus Rayleigh Optical Depth (TMROD). The optical depths were derived using the transmission functions implemented in the SMARTS parametric model, while the Total Optical Depths (TODs) were derived by solar extinction measurements obtained in Athens during May 1995. From the data analysis it is obvious that both the ozone and trace gases contribute significantly to TMROD in the Chappuis band. More specifically, the trace gases contributions are higher for air with high pollution levels, while ozone's contribution can be significant under clear-sky conditions. Therefore, the correction in TMROD due to ozone and trace gases optical depths is necessary for an accurate determination of the Aerosol Optical Depth (AOD) in the Chappuis band. The optical depth of ozone is generally removed during the process of the AOD retrievals, since the significance of its absorption in the Chappuis band is well understood. Nevertheless, the optical depth of the trace gases (mainly NO2) is not always taken into account in the AOD retrievals, though its contribution can be significant in urban polluted atmospheres. In this respect, the present study attempts to quantify the ozone and trace gases contributions in an urban environment and to provide some new functions that help estimate the contribution of ozone to the TMROD in the Chappuis band.  相似文献   

5.
The spatial variability and temporal behavior of the vertical flux of ozone have been investigated from turbulence measurements collected on aircraft flight legs in the daytime period during two consecutive summer experimental field programs. The data were obtained during horizontal flight legs conducted over agricultural crops and forested land in three different regions of the eastern United States.Results from individual experimental cases and statistics derived from all cases in each region are presented. Ozone flux generally exhibited a significant height dependency. The strongest negative (downward) fluxes in the lowest-level flight legs were primarily attributed to the uptake of ozone by the surface and vegetative cover. Fluxes were near-zero in the middle of the convective boundary layer (CBL) in the afternoon period. As ozone flux was proportional to concentration, slightly stronger fluxes were found in low-level urban plume segments where ozone concentrations were 10–20 ppb higher than in the surrounding area. The derived deposition velocity showed no such bias as a function of position across the urban plume. Ozone flux differences were not apparent between the more heavily forested sections and the primarily agricultural cropland areas in these regions. During the afternoon period when no clear temporal trend was evident, means from values obtained below 0.15Z i (Z i being the CBL height) were -0.421 and -0.431 ppb m-2 s-1 for ozone flux and 0.81 and 0.82 cm s-1 for the derived mean deposition velocity in the southeastern Pennsylvania and central Ohio areas, respectively. These experimental results for ozone provide support to a dry deposition parameterization module which computes grid-area averaged deposition velocities for use in regional-scale models.On assignment from the National Oceanic and Atmospheric Administration, U.S. Department of Commerce.  相似文献   

6.
Summary Long-term ozone recordings at different altitude levels, conducted in remote areas, can make a valuable contribution to an understanding of the background level of ozone, its periodical variations and possible long-term trends.The measuring stations (three high mountain stations between 740 and nearly 3000 m a.s.l. with small horizontal distance) are described together with recording and calibration procedures. Information is provided on the time history of all recordings since 1978, considering not only the annual means but also the monthly and 10-day means as a function of height. An analysis is presented of the annual variations which differ considerably in the respective height levels and—in three-dimensional diagrams—the correlation between daily and annual variation is shown as a function of height. Then follows a careful parameterization: analysis of the frequency distribution of the ozone concentration, correlation with relative humidity, relative sunshine duration, and temperature. It can be seen that the correlations are very different and partly inverse, depending on the altitude level.Many ozone profiles obtained between valley level and nearly 3000 m a.s.l. (cable car O3 radiosonde) give a picture of the typical ozone profile for different meteorological situations and for the case of stratospheric intrusions of ozone into the troposphere. The stratospheric contribution of ozone to the tropospheric ozone budget is discussed.Since obviously a very high photochemical production rate can be established for ozone in the lowest layer above ground (correlation of O3 with the daily variation of the sunshine duration) it was examined if this O3 variation might be caused only by horizontal transport of ozone from remote areas with high anthropogenic activity by the daily quasiperiodical currents near the ground. But this is not the case.The correlation between ozone concentration, other trace gases such as nitrogen-oxygen compounds and hydrocarbons is shown.With 29 Figures  相似文献   

7.
Connection between ozone concentration and atmosphere circulation is investigated based on measurements at BEO station, peak Moussala (2,925 m a.s.l.), for the period 09 August 2006 to 29 January 2008. Ozone concentration data are collected with UV-analyzer “Environnement O3 42” and meteo data with weather station “Vaisala”. There are measurements of 7Be. Data from NOAA HYSPLIT model for particle trajectories are also used. Eight wind directions and three ranges of wind velocities are employed in the analysis. A comparison of ozone concentrations in upward and downward air transport according to HYSPLIT model is made. The number of cases with ozone concentration above 63 ppb has been counted. Mann–Whitney nonparametric test is employed as a basic statistical method. Correlation between atmosphere pressure and tropospheric ozone content is made. The same is done for 7Be and ozone. The main conclusion is that there is not any local or regional pollution effect detectable at peak Moussala, but most of the ozone measured is due to emissions of hydrocarbons and NO x over a larger region. There could be some regional sources of ozone building substances in southwest direction from peak Moussala. Air transported from the north quarter has higher ozone concentrations compared to the south quarter. In vertical direction, upward transport of air masses shows higher values of ozone concentration. Higher wind velocity is associated with low ozone concentrations at peak Moussala. The annual course of ozone concentration has summer maximum and winter minimum. There is right connection between air pressure and ozone concentration. The same is valid for the correlation between 7Be and ozone. Diurnal ozone course shows daytime maximum in winter and nighttime maximum in summer.  相似文献   

8.
A fast-response chemiluminescent ozone sensor was mounted in an aircraft instrumented for air motion and temperature measurements. Measurements of the vertical flux of ozone by the eddy correlation technique were obtained after correcting for time delay and pressure sensitivity in the ozone sensor output. The observations were taken over eastern Colorado for two days in April, one a morning and the other an afternoon flight. Since the correlation coefficient of ozone and vertical velocity is small compared to, for example, temperature and vertical velocity in the lower part of the convective boundary layer, an averaging length of the order of 100 km was required to obtain a reasonably accurate estimate of the ozone flux. The measured variance of ozone appeared to be too large, probably mainly due to random noise in the sensor output, although the possibility of the production of ozone fluctuations by chemical reactions cannot be dismissed entirely. Terms in the budget equation for ozone were estimated from the aircraft measurements and the divergence of the ozone flux was found to be large compared to the flux at the surface divided by the boundary-layer height.Part of this work was carried out while a visitor at Risø National Laboratory, Denmark.The National Center for Atmospheric Research is sponsored by the National Science Foundation.  相似文献   

9.
Daytime variations of ozone eddy fluxes to maize   总被引：1，自引：0，他引：1  
The vertical fluxes of ozone, momentum and heat in the atmospheric surface layer have been measured by eddy correlation above both mature and senescent maize canopies. Aerodynamic formulae are applied to find that the bulk canopy surface resistancer c to ozone uptake and destruction varies between 4.0 and 0.5 s cm−1 during the daytime. Apparently, surface properties tend to control the removal of ozone at the surface of the earth. For a lush canopy, the stomatal diffusion resistance is the most important property, while changes in surface temperature have little effect. Destruction at the soil and exterior plant surfaces appears to account for 20–50% of the total loss if leaf mesophyll resistances are assumed to be very small. Free water at leaf surfaces may at times inhibit ozone removal by both senescent and healthy plants.  相似文献   

10.
Measurements of total ozone column and solar UV radiation under different atmospheric conditions are needed to define variations of both UV and ozone and to study the impact of ozone depletion at the Earth’s surface. In this study, spectral and broadband measurements of UV-B irradiance were obtained along with total ozone observations and aerosol optical depth measurements in the tropical urban region of Hyderabad, south India. We specifically used an Ultra-Violet Multifilter Rotating Shadow band Radiometer (UVMFR-SR), to measure UV irradiance in time and space. To assess the aerosol and O3 effects on ground-reaching UV irradiance, we used measurements from a Microtops II sun photometer in addition to the Tropospheric Ultraviolet Visible radiation (TUV) model. We also assessed the Defense Meteorological Satellite Program – Operational Line Scanner (DMSP-OLS) night time satellite data for inferring biomass burning fires during the study period. Results clearly suggested a negative correlation between the DMSP-OLS satellite derived fire count data and UVMFR-SR data suggesting that aerosols from biomass burning are directly attenuating UV irradiance in the study region. Also, correlation analysis between UV index and ozone measurements from sun photometer and TOMS-Ozone Mapping Instrument (OMI) indicated a clear decrease in ground reaching UV-B irradiance during higher ozone conditions. The higher levels are attributed to photochemical production of O3 during the oxidation of trace gases emitted from biomass burning. Results also suggested a relatively high attenuation in UV irradiance (~6% higher) from smoke particles than dust. We also found a relatively good agreement between the modeled (TUV) and measured UV irradiance spectra for different atmospheric conditions. Our results highlight the factors affecting UV irradiance in a tropical urban environment, south India.  相似文献   

11.
Abstract

Fluxes of temperature, water vapour, O3, SO2 and CO2 were estimated from the measurement of their variances, taken over a wetland region in northern Ontario (Canada) during the summer of 1990 and over a deciduous forest when it was fully leafed during the summer of 1988 and when it was leafless during the winter of 1990. A set of flux‐variance relations was employed, including empirical forms of universal functions that could be adjusted with some constants. Results from the present study show that these constants needed to be adjusted with site‐specific data in order to achieve a closer agreement between estimated and observed fluxes. Best estimates were obtained for the fluxes of temperature and water vapour and it was found that the flux estimates of O3, SO2 and CO2 correlated better with water vapour than with temperature. For these trace gases the flux‐variance method yielded estimates of dry deposition velocities that were either comparable with or larger than those obtained from a resistance analogue model. Both methods yielded values that overestimated the observed dry deposition velocities. The employment of the flux‐variance method in an operational network would require the use of fast‐response sensors and a practical method for reducing the noise level of the measured variances.  相似文献   

12.
Far-infrared emission spectroscopy has beendemonstrated to be a valuable method for remotesensing of trace species in the stratosphere, with theability to simultaneously detect a number of keychemical species. SAFIRE-A is a new far-infraredFourier Transform (FT) spectrometer which has beenspecifically designed to operate on board of a highaltitude aircraft in the lower stratosphere and uppertroposphere regions where relatively few remotesensing measurements have been made. Using newtechnology, the sensitivity of the FT spectrometermethod has been substantially improved for the longwavelength region. Results are reported formeasurements of O3, HNO3 and N2O at 17and 19 km using a detection window near 23 cm-1.Geographical and altitude variability of the volumemixing ratio of these constituents and their relativecorrelation are discussed. Ozone measurements agreewell with in situ measurements, except in regions ofstrong stirring and mixing associated with deformationof the northern vortex edge. Whilst SAFIREmeasurements of trace gases do not capture all of thelocal variability seen by rapid in-situ techniques,they can indicate horizontal variability close to, butnot intercepted by, the aircraft's flight path. Apossible detection of ClO at the low background levelsexpected outside the polar vortex is also reported.  相似文献   

13.
Three independent methods have been used to sort the ozone, carbonmonoxide, and other radiatively important trace gases measured at Mace Head,Ireland, and thereby distinguish clean air masses transported over the NorthAtlantic from the more polluted air masses which have recently travelledfrom the European continent. Over the period April 1987–June 1995 theNorthern Hemisphere surface ozone baseline concentrations exhibited a meanconcentration of 34.8 ppb, with a small positive trend (+0.19 ppbyr-1), while the corresponding trend in air originating fromthe polluted European areas was negative (–0.39 ppbyr-1). Carbon monoxide measurements from March 1990 toDecember 1994 showed negative trends for both the unpolluted (–0.17ppb yr-1) and polluted data (–13.6 ppbyr-1). Overall the continent of Europe was shown to be a smallnet sink of 2.6 ppb for all occasions when European air was transported tothe North Atlantic.  相似文献   

14.
For measurements of eddy fluxes in the atmospheric boundary layer of gases (such as CO2) whose average concentration is very large compared to the fluctuations, corrections for air density fluctuations are required. With the boundary condition of no flux of dry air at the surface, the evaporation correction to eddy fluxes is 2.6 times larger than has been estimated with the boundary condition of no mass flux at all at the surface. The heat flux correction is also increased by a few per cent.  相似文献   

15.
Emissions of N2O, CH4, and CO2 from soils at two sites in the tropical savanna of central Venezuela were determined during the dry season in February 1987. Measured arithmetic mean fluxes of N2O, CH4, and CO2 from undisturbed soil plots to the atmosphere were 2.5×109, 4.3×1010, and 3.0×1013 molecules cm-2 s-1, respectively. These fluxes were not significantly affected by burning the grass layer. Emissions of N2O increased fourfold after simulated rainfall, suggesting that production of N2O in savanna soils during the rainy season may be an important source for atmospheric N2O. The CH4 flux measurements indicate that these savanna soils were not a sink, but a small source, for atmospheric methane. Fluxes of CO2 from savanna soils increased ninefold two hours after simulated rainfall, and remained three times higher than normal after 16 hours. More research is needed to clarify the significance of savannas in the global cycles of N2O, CH4, CO2, and other trace gases, especially during the rainy season.  相似文献   

16.
The friction velocity (u*) and the sensible heat flux density (H) determined with a displaced-beam small aperture scintillometer (DBSAS) and a hot-film eddy correlation system are compared. Random errors in the DBSAS are relatively small, compared to scatter found with two eddy-correlation systems. Assuming that the hot-film system yields the true fluxes, theDBSAS appears to overestimate u* when u* is less than 0.2 m s-1 and to underestimate u* at high wind speeds. This implies that the DBSAS measurements of theinner scale length of turbulence, l0, a direct measure for the dissipation rate of kinetic turbulent energy, are biased. Possible causes for these results are discussedin detail. A correction procedure is presented to account for effects of random noise and of so-called inactive turbulence or sensor vibrations. The errors in u* cause errors in the DBSAS measurements of the structure parameter of temperature CT 2. The derived H appears to be less sensitive to errors in l0 and CT 2, because errors in these quantities tend to cancel out.  相似文献   

17.
Estimates of the Chemical Budget for Ozone at Waliguan Observatory   总被引：6，自引：0，他引：6  
Waliguan Observatory (WO) is an in-land Global Atmosphere Watch (GAW) baseline station on the Tibetan plateau. In addition to the routine GAW measurement program at WO, measurements of trace gases, especially ozone precursors, were made for some periods from 1994 to 1996. The ozone chemical budget at WO was estimated using a box model constrained by these measured trace gas concentrations and meteorological variables. Air masses at WO are usually affected by the boundary layer (BL) in the daytime associated with an upslope flow, while it is affected by the free troposphere (FT) at night associated with a downslope flow. An anti-relationship between ozone and water vapor concentrations at WO is found by investigating the average diurnal cycle pattern of ozone and water vapor under clear sky conditions. This relationship implies that air masses at WO have both the FT and BL characteristics. Model simulations were carried out for clear sky conditions in January and July of 1996, respectively. The chemical characteristics of mixed air masses (MC) and of free tropospheric air masses (FT) at WO were investigated. The effects of the variation in NOx and water vapor concentrations on the chemical budget of ozone at WO were evaluated for the considered periods of time. It was shown that ozone was net produced in January and net destroyed in July for both FT and MC conditions at WO. The estimated net ozone production rate at WO was –0.1 to 0.4 ppbv day–1 in FT air of January, 0.0 to 1.0 ppbv day–1 in MC air of January, –4.9 to –0.2 ppbv day–1 in FT air of July, and –5.1 to 2.1 ppbv day–1 in MC air of July.  相似文献   

18.
Abstract

The exchange of gases between the atmosphere and the oceans may occur directly through the sea surface and indirectly through the mediation of additional transient reservoirs: the bubbles injected into the upper ocean by breaking waves. These bubbles both will increase the gross rate of exchange between air and sea and will tend to force a supersaturation of the upper ocean. These two effects are made explicit by writing the equation for the net air‐sea flux of a gas as F = (K0 + Kb)[C — Sp(1 + ?)], where Kb is the contribution of bubbles to the transfer velocity (gross exchange rate) and ? denotes the supersaturation effect. Significant supersaturations can be attributed to the small (≤150‐μm radius) bubbles, which are commonly advected several metres below the sea surface (Woolf and Thorpe, 1991). The values of Kb attributable to this deep flux of bubbles are negligible for most gases, but much greater values are predicted by considering the total flux of bubbles through the sea surface.

The contribution of bubbles to the transfer velocity, Kb, is approximately proportional to the whitecap coverage. Transfer velocities are a complex function of the diffusivity and solubility of the dissolved gas. This function depends on the distribution of the bubbles. Transfer velocities of relatively soluble gases (and particularly the contribution of small bubbles) are limited by the volume flux of the bubbles, V, through the inequality Kb ≤ V/β where β is the Bunsen solubility of the gas. Values of Kb can be calculated using measurements of the bubbles in a simulated whitecap (Cipriano and Blanchard, 1981). Large (>150‐μm radius) bubbles are the main contributors to the air‐sea transfer velocity. Transfer velocities are less for more soluble gases. The global average value of Kb for carbon dioxide is probably between 2 and 10 cm h‐1; the best estimate is 8.5 cm h‐1.  相似文献   

19.
Summary  Turbulent fluxes of CO2 were continuously measured by eddy correlation for three months in 1997 over a gramineous fen in a high-arctic environment at Zackenberg (74°28′12″N, 20°34′23″W) in NE-Greenland. The measurements started on 1 June, when there was still a 1–2 m cover of dry snow, and ended 26 August at a time that corresponds to late autumn at this high-arctic site. During the 20-day period with snow cover, fluxes of CO2 to the atmosphere were small, typically 0.005 mg CO2 m−2 s−1 (0.41 g CO2 m−2 d−1), wheres during the thawed period, the fluxes displayed a clear diurnal variation. During the snow-free period, before the onset of vegetation growth, fluxes of CO2 to the atmosphere were typically 0.1 mg CO2 m−2 s−1 in the afternoon, and daily sums reached values up to almost 9 g CO2 m−2 d−1. After 4 July, downward fluxes of CO2 increased, and on sunny days in the middle of the growing season, the net ecosystem exchange rates attained typical values of about −0.23 mg m−2 s−1 at midday and max values of daily sums of −12 g CO2 m−2 d−1. Throughout the measured period the fen ecosystem acted as a net-sink of 130 g CO2 m−2. Modelling the ecosystem respiration during the season corresponded well with eddy correlation and chamber measurements. On the basis of the eddy correlation data and the predicted respiration effluxes, an estimate of the annual CO2 balance the calender year 1997 was calculated to be a net-sink of 20 g CO2 m−2 yr−1. Received October 6, 1999 Revised May 2, 2000  相似文献   

20.
Summary A coupled 1-D time-dependent radiative-convective-photochemical diffusion model which extends from the surface to 60 km is used to investigate the potential impact of greenhouse trace gas emissions on long-term changes in global climate, atmospheric ozone and surface UV-B radiation, taking into accoont the influence of aerosol loading into the atmosphere from major volcanic eruptions, of thermal inertia of the upper mixed layer of the ocean and of other radiativephotochemical feedback mechanisms. Experiments are carried out under global and annual average insolation and cloudiness conditions. The transient calculations are made for three different growth scenarios for increase in trace gas concentrations. Scenario 1, which begins in 1850, uses the best estimate values for future trace gas concentrations of CO2, CH4, N2O, CFC-11, CFC-12 and tropospheric O3, based on current observational trends. Scenarios 2 and 3, which begin in 1990, assume lower and upper ranges, respectively, of observed growth rates to estimate future concentrations.The transient response of the model for Scenario 1 suggests that surface warming of the ocean mixed layer of about 1 K should have taken place between 1850 and 1990 due to a combined increase of atmospheric CO2 and other trace gases. For the three scenarios considered in this study, the cumulative surface warming induced by all major trace gases for the period 1850 to 2080 ranges from 2.7 K to 8.2 K with the best estimate value of 5 K. The results indicate that the direct and the indirect chemistry-climate interactions of non-CO2 trace gases contribute significantly to the cumulative surface warming (up to 65% by the year 2080). The thermal inertia of a mixed layer of the ocean is shown to have the effect of delaying equilibrium surface warming by almost three decades with an e-folding time of about 5 years. The volcanic aerosols which would result from major volcanic eruptions play a significant role by interrupting the long-term greenhouse surface warming trend and replacing it by a temporary cooling on a time scale of a decade or less. Furthermore, depending on the scenario used, a reduction in the net ozone column could result in an increase in the solar UV-B radiation at the surface by as much as 300% towards the end of 21st century.With 14 Figures  相似文献   

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