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1.
Abstract

This work presents the climatology of the sulphur dioxide column over Thessaloniki derived from three years of observation with the Brewer spectrophotometer. The SO2 column averages 2.5 m atm‐cm and the shielding of UV‐B by SO2 is investigated and compared with the changes in shielding resulting from an anticipated ozone reduction. Columnar and surface SO2 concentrations over Thessaloniki appear to be typical of those in major industrial‐urban regions of the world. It is concluded that, for urban regions, predictions of changes in UV‐B as a result of man's activities must consider projections of changes in the SO2 column as well as ozone.  相似文献   

2.
A small, lightweight (1.5 kg) and fast-response ozone sensor for direct eddy flux measurements has been built. The basis for detection is the chemiluminescence of an organic dye adsorbed on dry silica gel in the reaction with ozone. The chemiluminescence is monitored with a cheap and small blue-sensitive photomultiplier. At a flow rate of 100 l min-1 the ozone sensor has a 90% response time of significantly better than 0.1 s with a detection limit lower than 50 ppt at S/N=3. There are no interferences from other atmospheric trace gases like NOx, H2O2 and PAN. Water vapour and SO2 enhance the chemiluminescence efficiency of the ozone sensor. Since their response times are 22 seconds and 30 minutes, respectively, no correlation between rapid ozone fluctuations and those of these two trace gases is noticed by the ozone sensor when operating at a frequency of 10 Hz.The ozone sensor was tested for several weeks in continuous measurements of ozone fluxes and deposition velocities over different croplands using the eddy correlation technique. Good agreement was found between ozone dry deposition velocities derived from profile measurements and by eddy correlation.  相似文献   

3.
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   

4.
Abstract

Dry deposition velocity measurements of SO2 and NO2 over a deciduous forest, a carrot field and a snow surface are compared with estimates obtained from the dry deposition module in the regional Eulerian Acid Deposition and Oxidant Model (ADOM). The comparison with measurements taken in the fall and winter shows large model overestimates, sometimes as large as a factor of 5. The NO2 estimates are particularly poor and support existing evidence that models that employ the constant flux assumption for NO2 are inadequate. The canopy and the snow surface resistances are the largest contributors to the total resistances for SO2 and NO2, except for situations in which some of the snow turns into liquid water, when the aerodynamic resistance becomes important.

Increasing the magnitudes, taken from measurements, of the ADOM original values for the stomatal, cuticle, ground and snow resistances and decreasing the NO2 mesophyll resistance and the Leaf Area Index (LAI) yield improved model results, particularly for SO2, reducing the error by almost a factor of 5 at times. The new estimates compare favourably with those from a model that includes Wesely's canopy resistance parametrization. Over snow the NO2 estimates are improved by as much as a factor of 6. Observed deposition velocities for SO2 vary from 0 to 0.65 cm s?2 over a deciduous forest, 0 to 0.60 cm s?2 over a carrot field and are generally less than 0.05 cm s?2 over snow.  相似文献   

5.
Summary Vertical profiles of H2O, CO2, O3, NO and NO2 were measured during the Hartheim Experiment (HartX) to develop and calibrate a multi-layer resistance model to estimate deposition and emission of the cited gaseous species. The meteorological and gas concentration data were obtained with a 30 m high telescopic mast with 7 gas inlets located at 5 m intervals and meteorological sensors at 5, 15 and 30 m above ground; a complete gas profile was obtained every 9 min 20 s. Measured profiles were influenced by several exchange processes, namely evapotranspiration, dewfall, assimilation of CO2 in the tree crowns, soil respiration, deposition of NO2 and O3 to the soil and advection of NOx from the nearby highway. Surprisingly, no decrease in O3 concentration was observed in the crown layer during daytime, probably due to the relatively low density of foliage elements and strong turbulent mixing.The advantage of measuring in-canopy profiles is that turbulent exchange coefficients need not be estimated as a prerequisite to obtaining vertical flux estimates. In recent years, flux-gradient relationships in canopies have been subject to many criticisms. If fluxes are calculated at several heights considering only the transfers between the turbulent air and the interacting surfaces at a certain height, and those fluxes are then integrated vertically in a subsequent step, then exchange estimates (deposition or emission) can be obtained independent of turbulent exchange conditions.Typical estimated deposition velocities calculated for a 3-day period are between 4 and 10 mm/s for NO2 and about 4–9 mm/s for O3 (day and night values respectively). This leads to deposition rates of about 20–40 ng N/m2s for NO2 and about 30–40 mg O3/m2 deposited daily under the conditions encountered during HartX. Sensitivity tests done with the best available and most realistic values for model parametrization have shown that sensitivity is large with respect to the soil and cuticula resistances as well as for gas-phase ozone destruction and that more research is required to describe the effectiveness of cuticula and soil in modifying sink characteristics for NO2 and O3.With 12 Figures  相似文献   

6.
It is important to improve estimates of large-scale carbon fluxes over the boreal forest because the responses of this biome to global change may influence the dynamics of atmospheric carbon dioxide in ways that may influence the magnitude of climate change. Two methods currently being used to estimate these fluxes are process-based modeling by terrestrial biosphere models (TBMs), and atmospheric inversions in which fluxes are derived from a set of observations on atmospheric CO2 concentrations via an atmospheric transport model. Inversions do not reveal information about processes and therefore do not allow for predictions of future fluxes, while the process-based flux estimates are not necessarily consistent with atmospheric observations of CO2. In this study we combine the two methods by using the fluxes from four TBMs as a priori fluxes for an atmospheric Bayesian Synthesis Inversion. By doing so we learn about both approaches. The results from the inversion indicate where the results of the TBMs disagree with the atmospheric observations of CO2, and where the results of the inversion are poorly constrained by atmospheric data, the process-based estimates determine the flux results. The analysis indicates that the TBMs are modeling the spring uptake of CO2 too early, and that the inversion shows large uncertainty and more dependence on the initial conditions over Europe and Boreal Asia than Boreal North America. This uncertainty is related to the scarcity of data over the continents, and as this problem is not likely to be solved in the near future, TBMs will need to be developed and improved, as they are likely the best option for understanding the impact of climate variability in these regions.  相似文献   

7.
The chemical reactivity of NO and NO2 is so rapid that their fluxes and concentrations can be considerably modified from that expected for conserved variables in the atmospheric surface layer, even as low as a meter above the surface. Fitzjarrald and Lenschow (1983) have calculated flux and mean concentration profiles for NO, NO2 and O3 in the surface layer using numerical techniques. However, their solutions do not approach the photostationary state at large heights. Here we solve a simpler set of equations analytically (i.e. we assume a constant O3 concentration and neutral hydrodynamic stability), and are able to show how the flux profiles behave at large heights assuming that the concentrations approach their photostationary values. We find, for example, that at large heights the ratio of the flux of NO to that of NO2 is equal to the ratio of their concentrations. These results are relevant to estimating surface fluxes of NO and NO2, and are most applicable to nonurban environments where NO and NO2 concentrations are usually much less than O3 concentration.The National Center for Atmospheric Research is sponsored by the National Science Foundation.  相似文献   

8.
利用中尺度大气化学模式WRF/Chem对2013年3月6日华南地区一次平流层入侵事件及其对对流层低层臭氧的影响进行模拟研究。通过加入UBC（Upper Boundary Condition）上边界处理方案,弥补WRF/Chem模式未考虑平流层臭氧化学反应的不足。结合臭氧探空廓线资料、地面O3、CO、NOx、相对湿度、温度和风速等观测资料以及再分析资料对模拟结果进行定量评估,结果表明模式能较为真实地模拟本次平流层入侵过程。模拟分析进一步揭示:（1）副热带高空急流是本次平流层入侵的主要原因。当华南地区处在副热带急流入口区左侧下沉区域时,平流层入侵将富含臭氧的干燥空气输送到对流层中低层。（2）本次平流层入侵对对流层低层臭氧收支有重要影响,导致香港地区近地层臭氧体积混合比浓度明显上升,如塔门站夜间臭氧浓度升高21.3 ppb（1 ppb=1×10-9）。地面气象场和化学物种的分析进一步确认了平流层入侵的贡献。（3）采用动力学对流层顶高度时零维箱式模型和Wei公式计算得到的平流层入侵通量相当,分别为-1.42×10-3 kg m-2 s-1和-1.59×10-3 kg m-2 s-1,这一结果与前人研究相吻合,且与采用热力学对流层顶高度计算所得到的结果具有可比性。  相似文献   

9.
Using the new high-frequency measurement equipment of the research aircraft DO 128, which is described in detail, turbulent vertical fluxes of ozone and nitric oxide have been calculated from data sampled during the ESCOMPTE program in the south of France. Based on airborne turbulence measurements, radiosonde data and surface energy balance measurements, the convective boundary layer (CBL) is examined under two different aspects. The analysis covers boundary-layer convection with respect to (i) the control of CBL depth by surface heating and synoptic scale influences, and (ii) the structure of convective plumes and their vertical transport of ozone and nitric oxides. The orographic structure of the terrain causes significant differences between planetary boundary layer (PBL) heights, which are found to exceed those of terrain height variations on average. A comparison of boundary-layer flux profiles as well as mean quantities over flat and complex terrain and also under different pollution situations and weather conditions shows relationships between vertical gradients and corresponding turbulent fluxes. Generally, NOx transports are directed upward independent of the terrain, since primary emission sources are located near the ground. For ozone, negative fluxes are common in the lower CBL in accordance with the deposition of O3 at the surface.The detailed structure of thermals, which largely carry out vertical transports in the boundary layer, are examined with a conditional sampling technique. Updrafts mostly contain warm, moist and NOx loaded air, while the ozone transport by thermals alternates with the background ozone gradient. Evidence for handover processes of trace gases to the free atmosphere can be found in the case of existing gradients across the boundary-layer top. An analysis of the size of eddies suggests the possibility of some influence of the heterogeneous terrain in mountainous area on the length scales of eddies.  相似文献   

10.
This study reports comparisonsbetween model simulations, based on current sulfurmechanisms, with the DMS, SO2 and DMSOobservational data reported by Bandy et al.(1996) in their 1994 Christmas Island field study. For both DMS and SO2, the model results werefound to be in excellent agreement with theobservations when the observations were filtered so asto establish a common meteorological environment. Thisfiltered DMS and SO2 data encompassedapproximately half of the total sampled days. Basedon these composite profiles, it was shown thatoxidation of DMS via OH was the dominant pathway withno more than 5 to 15% proceeding through Cl atoms andless than 3% through NO3. This analysis wasbased on an estimated DMS sea-to-air flux of 3.4 ×109 molecs cm-2 s-1. The dominant sourceof BL SO2 was oxidation of DMS, the overallconversion efficiency being evaluated at 0.65 ± 0.15. The major loss of SO2 was deposition to theocean's surface and scavenging by aerosol. Theresulting combined first order k value was estimated at 1.6 × 10-5 s-1. In contrast to the DMSand SO2 simulations, the model under-predictedthe observed DMSO levels by nearly a factor of 50. Although DMSO instrument measurement problems can notbe totally ruled out, the possibility of DMSO sourcesother than gas phase oxidation of DMS must beseriously considered and should be explored in futurestudies.  相似文献   

11.
A modified profile method for determining the vertical deposition (or/and exhalation) fluxes of NO, NO2, ozone, and HNO3 in the atmospheric surface layer is presented. This method is based on the generally accepted micrometeorological ideas of the transfer of momentum, sensible heat and matter near the Earth's surface and the chemical reactions among these trace gases. The analysis (aerodynamic profile method) includes a detailed determination of the micrometeorological quantities (such as the friction velocity, the fluxes of sensible and latent heat, the roughness length and the zero plane displacement), and of the height-invariant fluxes of the composed chemically conservative trace gases with group concentrations c 1=[NO]+[NO2]+[HNO3], c 2=[NO2]+[O3]+3/2·[HNO3], and c 3=[NO]–[O3]–1/2·[HNO3]. The fluxes of the individual species are finally determined by the numerical solution of a system of coupled nonlinear ordinary differential equations for the concentrations of ozone and HNO3 (decoding method). The parameterization of the fluxes is based on the flux-gradient relationships in the turbulent region of the atmospheric surface layer. The model requires only the vertical profile data of wind velocity, temperature and humidity and concentrations of NO, NO2, ozone, and HNO3.The method has been applied to vertical profile data obtained at Jülich (September 1984) and collected in the BIATEX joint field experiment LOVENOX (Halvergate, U.K., September 1989).  相似文献   

12.
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   

13.
An automated system for measuring the dry deposition fluxes of SO2 on a routine basis based on the micrometeorological gradient technique has been developed for application over grassland and other short vegetation. The ability of the system to determine turbulent exchange parameters such as the friction velocity u * and the heat flux H was investigated by comparison with an automated eddy correlation system.Determinations of u * and H by both methods have generally been found to be in very good agreement for 20 min averages. Aerodynamic resistances derived from both systems showed no systematic differences but individual values differed considerably. From the analysis it appeared that in addition to classical rejection criteria on wind speed and inhomogeneity, etc., periods with large shifts in wind direction also have to be removed from the data set before interpretation.  相似文献   

14.
The growth of monodisperse particles (0.07 to 0.5 µm) exposed to SO2 (0–860 ppb), H2O2 (0–150 ppb) and sometimes NH3 (0–550 ppb) in purified air at 22 °C at relative humidities ranging from 25 to 75% were measured using the Tandem Differential Mobility Analyzer technique. The experiments were performed in a flow reactor with aqueous (NH4)2SO4 and Na2SO4 droplets. For (NH4)2SO4 droplets the fractional diameter growth was independent of size above 0.3 µm but decreased with decreasing size below that. When NH3 was added the fractional growth increased with decreasing size. Measurements were compared with predictions of a model that accounts for solubility of the reactive gases, the liquid phase oxidation of SO2 by H2O2, and ionic equilibria. Agreement between measured and predicted droplet growth is reasonable when the ionic strength effects are included. Theory and experiments suggest that NH3 evaporation is responsible for the decrease in relative growth rates for small aqueous ammonium sulfate particles. The observed droplet growth rates are too slow to explain observed growth rates of secondary atmospheric sulfate particles.  相似文献   

15.
Eddy correlation measurements of NO vertical flux were made periodically from October 1983 through June 1984 at a height of eight meters above grass in northeastern Illinois, U.S.A. From 207 data points, each representing a 25 min average, 19 daytime cases and 8 nighttime cases were selected on the basis of steady, nonadvective atmospheric conditions. Each case was represented by a set of data constituting a 3 to 5 hr average. Concentrations of O3, NO, and NO y (from which NO2 was inferred) and local atmospheric and surface conditions also were measured, to provide the information necessary to assess the relative importance of surface deposition, surface emission, and air chemistry on the observed NO flux. On the basis of a linear regression analysis applied with independent variables representing physical, chemical, and biological processes, surface uptake of NO was very small for data primarily collected in the daytime during spring, and measured deposition velocities at a height of 8 m were very small, much smaller than expected for NO2. For the same time period, the surface emission rates of elemental nitrogen in NO were in the range of 1.4 to 4.2 ng m-2 s-1 for moist, unsaturated soils at temperatures near 15° C. These emissions were partially masked in the measured fluxes by rapid in-air chemical reactions involving O3 and NO2. The effects of rapid in-air chemical reactions involving O3 were to decrease the (upward) flux of NO with height. While the information collected at night was too limited to strongly support hypotheses concerning emissions and deposition, a pathway for NO production by reactions involving NO3 and related compounds was indicated. For daytime conditions, this production pathway is not evident, probably because of the relatively strong effects of photochemical reactions involving NO, NO2, and O3.Formerly with the Chemical Technology Division of Argonne National Laboratory and currently affiliated with Bio-Rad Laboratories, Digilab Division, Minneapolis, MN, U.S.A.  相似文献   

16.
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17.
对临安大气本底站2003-2004年冬、夏季二氧化氮(NO2)、二氧化硫(SO2)、臭氧(O3)进行了分析.结果表明:冬季NO2和SO2平均体积分数分别为19.48×10-9和35.74 x10-9,而夏季的平均体积分数分别为4.81×10-9和8.12×10-9,冬季高于夏季;O3在夏季的平均体积分数为33.55×10-9,略高于冬季的25.44×10-9;夜间NO2和SO2体积分数比白天高,并且NO2呈明显的单峰单谷型分布,O3也呈单峰型但峰值出现在白天.NO2、SO2体积分数存在着明显的“假日效应”,假日比非假日低,周五高于假日和非假日;但O3体积分数没有明显的假日效应.降水对SO2有明显的清除作用,但对NO2的清除作用不明显.与风向对比发现,夏季高体积分数的NO2、SO2都受到NW、WNW风的影响,冬季则分别受NE和SW、SSW风的影响;而O3受风向的影响较复杂,与局地光化学反应有关.  相似文献   

18.
The effect of clouds and cloud chemistry on tropospheric ozone chemistry is tested out in a two-dimensional channel model covering a latitudinal band from 30 to 60° N. Three different methods describing how clouds affect gaseous species are applied, and the results are compared. The three methods are:
  • ?A first order parameterization scheme for the removal of sulphur and other soluble gases by liquid droplets.
  • ?A parameterization scheme for SO2, O3, and H2O2 removal is constructed. The scheme is based on the solubility of gases in liquid droplets, cycling times of air masses between clouds and cloud free areas and on the chemical interaction of SO2 with H2O2 and O3 in the liquid phase.
  • ?Gas-aqueous-phase interactions and aqueous-phase chemical reactions are included in the reaction scheme for a number of components in areas where clouds are present.
    • In all three methods, a full gas-phase chemistry scheme is used. Particular emphasis is given to the study of how the ozone and hydrogen peroxide levels are affected. Significant changes in the distributions are found when aqueous-phase chemical reactions are included. The result is loss of ozone in the aqueous phase, with pronounced reductions in ozone levels in the middle and lower troposphere. Ozone levels are reduced by 10 to 30% with the largest reductions in the remote middle troposphere, bringing the values in better agreement with observations. Changes in H2O2 are harder to predict. Although, in one case study, hydrogen peroxide is produced within the aqueous phase, concentrations are mostly comparable or even lower than in the other cases. Hydrogen peroxide levels are, however, shown to be very pH sensitive. pH values around 5 seem to favour high H2O2 levels. High H2O2 concentrations may be found particularly in the upper part of the clouds under favourable conditions.  相似文献   

    19.
    Surface ozone is mainly produced by the photodissociation of nitrogen dioxide (NO2) by solar UV radiation. Subsequently, solar eclipses provide one of the unique occasions to explore the variations in the photolysis rate of NO2 and their significant impact on the production of ozone at a location. This study aims to examine the diurnal variations in the photodissociation rate coefficient of NO2, (j(NO2*)), and mixing ratios of surface ozone and NO X * (NO?+?NO2*) during the solar eclipse that occurred on 15 January 2010 at Kannur (11.9°N, 75.4°E, 5?m amsl), a tropical coastal site on the Arabian Sea in South India. This investigation was carried out on the basis of the ground level observations of surface ozone and its prominent precursor NO2*. The j(NO2*) values were estimated from the observed solar UV-A flux data. A sharp decline in j(NO2*) and surface ozone was observed during the eclipse phase because of the decreased efficiency of the ozone formation from NO2. The NO2* levels were found to increase during this episode, whereas the NO levels remained unchanged. The surface ozone concentration was reduced by 57.5%, whereas, on the other hand, that of NO X * increased by 62.5% during the solar eclipse. Subsequently a reduction of *% in the magnitude of j(NO2*) was found here during the maximum obscuration. Reductions in solar insolation, air temperature and wind speed were also observed during the solar eclipse event. The relative humidity showed a 6.4% decrease during the eclipse phase, which was a unique observation at this site.  相似文献   

    20.
    We have developed a simple, steady-state, one-dimensional second-order closure model to obtain continuous profiles of turbulent fluxes and mean concentrations of non-conserved scalars in a convective boundary layer without shear. As a basic tool we first set up a model for conserved species with standard parameterizations. This leads to formulations for profiles of the turbulent diffusivity and the ratio of temperature-scalar covariance to the flux of the passive scalar. The model is then extended to solving, in terms of profiles of mean concentrations and fluxes, the NO x –O3 triad problem. The chemical reactions involve one first-order reaction, the destruction of NO2 with decay time τ, and one second-order reaction, the destruction of NO and O3 with the reaction constant k. Since the fluxes of the sum concentrations of NO x = NO + NO2 and O3 + NO2 turn out to be constant throughout the boundary layer, the problem reduces to solving two differential equations for the concentration and the flux of NO2. The boundary conditions are the three surface fluxes and the fluxes at the top of the boundary layer, the last obtained from the entrainment velocity, and the concentration differences between the free troposphere and the top of the boundary layer. The equations are solved in a dimensionless form by using 1/(kτ) as the concentration unit, the depth h of the boundary layer as the length unit, the convective velocity scale w * as the velocity unit, and the surface temperature flux divided by w * as the temperature unit. Special care has been devoted to the inclusion of the scalar–scalar covariance between the concentrations of O3 and NO. Sample calculations show that the fluxes of the reactive species deviate significantly from those of non-reactive species. Further, the diffusivities, defined by minus the flux divided by the concentration gradient may become negative for reactive species in contrast to those of non-reactive species, which in the present model are never negative.  相似文献   

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