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1.
Recent studies suggest that the destruction of methane by Cl in the marine boundary layer could be accounted for as another major sink besides the methane destruction by OH. High level ab initio molecular orbital calculations have been carried out to study the CH4+Cl reaction, the carbon Kinetic Isotope Effect (KIE) is calculated using Conventional Transition-State Theory (CTST) plus Wigner and Eckart semiclassical tunneling corrections. The calculated KIE is around 1.026 at 300 K and has a small temperature variation. This is by far the largest KIE among different processes involving atmospheric methane destruction (e.g., OH, soil). A calculated mass balance of atmospheric methane including the KIE for the CH4+Cl reaction is found to favor those methane budgets with enhanced biological methane sources, which have relatively lighter carbon isotope composition.  相似文献   

2.
Within the German Tropospheric Research Programme (TFS) numerous kinetic and mechanistic studies on the tropospheric reaction/degradation of the following reactants were carried out: oxygenated VOC, aromatic VOC, biogenic VOC, short-lived intermediates, such as alkoxy and alkylperoxy radicals.At the conception of the projects these selected groups were classes of VOC or intermediates for which the atmospheric oxidation mechanisms were either poorly characterised or totally unknown. The motivation for these studies was the attainment of significant improvements in our understanding of the atmospheric chemical oxidation processes of these compounds, particularly with respect to their involvement in photooxidant formation in the troposphere. In the present paper the types of experimental investigations performed and the results obtained within the various projects are briefly summarised. The major achievements are highlighted and discussed in terms of their contribution to improving our understanding of the chemical processes controlling photosmog formation in the troposphere.  相似文献   

3.
A liquid jet of 90 m diameter and variable length has been utilized to determine absorption rates and, hence, mass accommodation coefficients , of atmospheric trace gases. The compounds investigated are HCl (0.01), HNO3 (0.01), N2O5 (0.005), peroxyacetyl nitrate (>0.001), and HONO (0.005). It is concluded that the absorption of these trace gases by liquid atmospheric water is not significantly retarded by interfacial mass transport. The strengths and limitations of the liquid jet technique for measuring mass accommodation coefficients are explored.  相似文献   

4.
We present the first application of a multi-stage impactor to study volcanic particle emissions to the troposphere from Masaya volcano, Nicaragua. Concentrations of soluble SO4 2–,Cl–, F–, NO3 –, K+, Na+,NH4 +, Ca2+ and Mg2+ were determined in 11 size bins from 0.07 m to >25.5 m. The near-source size distributions showed major modes at 0.5m (SO4 2–, H+,NH4 +); 0.2 m and 5.0 m (Cl–) and 2.0–5.0 m(F–). K+ and Na+ mirrored the SO4 2– size-resolvedconcentrations closely, suggesting that these were transported primarily asK2SO4 and Na2SO4 in acidic solution, while Mg2+ andCa2+ presented modes in both <1 m and >1 m particles. Changes in relative humidity were studied by comparing daytime (transparent plume) and night-time (condensed plume) results. Enhanced particle growth rates were observed in the night-time plume as well as preferential scavenging of soluble gases, such as HCl, by condensed water. Neutralisation of the acidic aerosol by background ammonia was observed at the crater rim and to a greater extent approximately 15 km downwind of the active crater. We report measurements of re-suspended near-source volcanic dust, which may form a component of the plume downwind. Elevated levels ofSO4 2–, Cl–, F–,H+, Na+, K+ and Mg2+ were observed around the 10 m particle diameter in this dust. The volcanic SO4 2– flux leaving the craterwas 0.07 kg s–1.  相似文献   

5.
Summary ¶In order to better understand land-atmosphere interactions and increase the predictability of climate models, it is important to investigate the role of forest representation in climate modeling. Corresponding to the big-leaf model commonly employed in land surface schemes to represent the effects of a forest, a so called big-tree model, which uses multi-layer vegetation to represent the vertical canopy heterogeneity, was introduced and incorporated into the National Center for Atmospheric Research (NCAR) regional climate model RegCM2, to make the vegetation model more physically based. Using this augmented RegCM2 and station data for China during 1991 Meiyu season, we performed 10 experiments to investigate the effects of the application of the big-tree model on the summer monsoon climate.With the big-tree model incorporated into the regional climate model, some climate characteristics, e.g. the 3-month-mean surface temperature, circulation, and precipitation, are significantly and systematically changed over the model domain, and the change of the characteristics differs depending on the area. Due to the better representation of the shading effect in the big-tree model, the temperature of the lower layer atmosphere above the plant canopy is increased, which further influences the 850hPa temperature. In addition, there are significant decreases in the mean latent heat fluxes (within 20–30W/m2) in the three areas of the model domain.The application of the big-tree model influences not only the simulated climate of the forested area, but also that of the whole model domain, and its impact is greater on the lower atmosphere than on the upper atmosphere. The simulated rainfall and surface temperature deviate from the originally simulated result and are (or seem to be) closer to the observations, which implies that an appropriate representation of the big-tree model may improve the simulation of the summer monsoon climate.We also find that the simulated climate is sensitive to some big-tree parameter values and schemes, such as the shape, height, zero-plane displacement height and mixing-length scheme. The simulated local/grid differences may be very large although the simulated areal-average differences may be much lower. The area-average differences in the monthly-mean surface temperature and heat fluxes can amount to 0.5°C and 4W/m2, respectively, which correspond to maximum local/grid differences of 3.0°C and 40W/m2 respectively. It seems that the simulated climate is most sensitive to the parameter of the zero-plane displacement among the parameters studied.  相似文献   

6.
The aerodynamic classification of the resistance laws above solid surfaces is based on the use of a so-called Reynolds roughness number Re s =h s u */, whereh s is the effective roughness height, -viscosity,u *-friction velocity. The recent experimental studies reported by Toba and Ebuchi (1991), demonstrated that the observed variability of the sea roughness cannot be explained only on the basis of the classification of aerodynamic conditions of the sea surface proposed by Kitaigorodskii and Volkov (1965) and Kitaigorodskii (1968) even though the latter approach gains some support from recent experimental studies (see for example Geernaertet al. 1986). In this paper, an attempt is made to explain some of the recently observed features of the variability of surface roughness (Toba and Ebuchi, 1991; Donelanet al., 1993). The fluctuating regime of the sea surface roughness is also described. It is shown that the contribution from the dissipation subrange to the variability of the sea surface can be very important and by itself can explain Charnock's (1955) regime.  相似文献   

7.
The commonly reported temperature coefficient of P. the equilibrium partial pressure of CO2, is (P/T) A,C ,which is about 15 ppm/°C, or 5% of the atmospheric partial pressure of CO2. This coefficient, however, applies only to deep water, not to surface water which can exchange CO2 with the atmosphere. The coefficient (P/T) A,C ,, where designates constancy of the sum of atmospheric and surface-ocean CO2, is the appropriate value for air-sea exchange. Numerical values are mass-dependent because the depth of the exchanging ocean layer must be specified. For a 100-m surface layer, the value is ca. 1.5 ppm/°C, or 0.5% of ambient CO2. Editor's Note:In view of the interdisciplinary importance of the carbon dioxide-climate problem, this note on seawater chemistry should be of interest to specialists beyond the discipline of ocean chemistry.  相似文献   

8.
Summary Interannual modes are described in terms of three-month running mean anomaly winds (u,v), outgoing longwave radiation (OLR), and sea surface temperature (T * ). Normal atmospheric monsoon circulations are defined by long-term average winds (u n,v n) computed every month from January to December. Daily winds are grouped into three frequency bands, i.e., 30–60 day filtered winds (u L,v L); 7–20 day filtered winds (u M,v M); and 2–6 day filtered winds (u S,v S). Three-month running mean anomaly kinetic energy (signified asK L , K M , andK S , respectively) is then introduced as a measure of interannual variation of equatorial disturbance activity. Interestingly, all of theseK L , K M , andK S perturbations propagate slowly eastward with same phase speed (0.3 ms–1) as ENSO modes. Associated with this eastward propagation is a positive (negative) correlation between interannual disturbance activity (K L , K M , K S ) and interannualu (OLR) modes. Namely, (K L , K M , K S ) becomes more pronounced than usual nearly simultaneously with the arrival of westerlyu and negativeOLR (above normal convection) perturbutions. In these disturbed areas with (K L , K M , K S >0), upper ocean mixing tends to increase, resulting in decreased sea surface temperature, i.e.T * 0. Thus, groups (not individual) of equatorial disturbances appear to play an important role in determiningT * variations on interannual time scales. HighestT * occurs about 3 months prior to the lowestOLR (convection) due primarily to radiational effects. This favors the eastward propagation of ENSO modes. The interannualT * variations are also controlled by the prevailing monsoonal zonal windsu n, as well as the zonal advection of sea surface temperature on interannual time scales. Over the central Pacific, all of the above mentioned physical processes contribute to the intensification of eastward propagating ENSO modes. Over the Indian Ocean, on the other hand, some of the physical processes become insignificant, or even compensated for by other processes. This results in less pronounced ENSO modes over the Indian Ocean.With 10 FiguresContribution No. 89-6, Department of Meteorology, University of Hawaii, Honolulu, Hawaii.  相似文献   

9.
Turbulence mechanisms at an agricultural site   总被引：8，自引：0，他引：8  
An extensive set of turbulence data from the 3- and 12-m heights taken over an agricultural site (Marsta, Sweden) are analyzed and compared with data from ideal sites.In unstable air, Monin-Obukhov similarity is found to be valid for the non-dimensional gradients of wind, m , temperature, h , and humidity, e , for (only a few data), for T /|T *|,/ E /|E *| and for the non-dimensionalized inertial subrange spectra of temperature and humidity. Where comparison is possible, the unstable data also agree with those found in the Kansas study, with one remarkable exception, the inertial subrange constant of the temperature spectrum, 1, being only 0.39, compared to the value 0.80 found at the Kansas site.On the stable side, most similarity predictions break down, with most of the data differing systematically from the corresponding Kansas results, the only exception being . The inertial subrange constants for temperature, 1, and for humidity, 1 are found to have the same values, 0.39 and 0.30, respectively, as they do on the unstable side. Remarkable similarity is found for the shape of the stable u- and - and e-spectra. In addition, this shape is found to be identical with that found in Kansas. The peak wavelength of the stable u-, and -spectra is found to be about four times larger than it is for the corresponding Kansas spectra. This is interpreted to be a result of the increased macro-roughness at the Marsta site as compared with that at the Kansas site. A possible explanation for the low 1-value is discussed, suggesting that 1 is not a universal constant, but instead dependent on the turbulent structure.  相似文献   

10.
Summary During an expedition to the high Andes of Southern Peru in June–July 1977, measurements of direct solar radiation in four spectral bands (0.270–0.530–0.630–0.695–2.900 ) were conducted at six sites in elevations ranging from sea level to 5645 m. These measurements were evaluated in Langley plots to determine total optical depths () and irradiances at the top of the atmosphere. In addition, water vapor optical depths (wv) were calculated from the mean radiosounding over Lima during the expedition, and Rayleigh (ray) and ozone (oz) optical depths were obtained from published tabulations. Subtracting ray, oz, and wv from yielded estimates of aerosol optical depth aer. The components ray and oz decrease from the shorter towards the longer wavelength bands and from the lower towards the higher elevation sites; aer also decreases towards the higher elevations. Particularly pronounced is the decrease of aer and from the lowlands of the Pacific coast to the highlands of the interior, reflecting the effect of a persistent lower-tropospheric inversion and the contrast from the marine boundary layer to the clear atmosphere of the high Andes.With 4 Figures  相似文献   

11.
Summary A radiative transfer model has been used to determine the large scale effective 6.6 GHz and 37 GHz optical depths of the vegetation cover. Knowledge of the vegetation optical depth is important for satellite-based large scale soil moisture monitoring using microwave radiometry. The study is based on actual observed large scale surface soil moisture data and observed dual polarization 6.6 and 37 GHz Nimbus/SMMR brightness temperatures over a 3-year period. The derived optical depths have been compared with microwave polarization differences and polarization ratios in both frequencies and with Normalized Difference Vegetation Index (NDVI) values from NOAA/AVHRR. A synergistic approach to derive surface soil emissivity from satellite observed brightness temperatures by inverse modelling is described. This approach improves the relationship between satellite derived surface emissivity and large scale top soil moisture fromR 2=0.45 (no correction for vegetation) toR 2=0.72 (after correction for vegetation). This study also confirms the relationship between the microwave-based MPDI and NDVI earlier described and explained in the literature.List of Symbols f frequency [Hz] - f i(p) fractional absorption at polarizationp - h surface roughness - h h cos2 - H horizontal polarization - n i complex index of refraction - p polarization (H orV) - R s microwave surface reflectivity - T B(p) brightness temperature at polarizationp - T * normalized brightness temperature - T polarization difference (T v-T H) - T s temperature of soil surface - T c temperature of canopy - T max daily maximum air temperature - T min daily minimum air temperature - V vertical polarization - soil moisture distribution factor; also used for the constant to partition the influence of bound and free water components to the dielectric constant of the mixture - empirical complex constant related to soil texture - microwave transmissivity of vegetation (=e –) - * effective transmissivity of vegetation (assuming =0) - microwave emissivity - s emissivity of smooth soil surface - rs emissivity of rough soil surface - vs emissivity of vegetated surface - soil moisture content (% vol.) - K dielectric constant [F·m–1] - K fw dielectric constant of free water [F·m–1] - K ss dielectric constant of soil solids [F·m–1] - K m dielectric constant of mixture [F·m–1] - K o permittivity of free space [8.854·10–12 F·m–1] - high frequency limit ofK wf [F·m–1] - wavelength [m] - incidence angle [degrees from nadir] - polarization ratio (T H/T V) - b soil bulk density [gr·cm–3] - s soil particle density [gr·cm–3] - R surface reflectivity in red portion of spectrum - NIR surface reflectivity in near infrared portion of spectrum - eff effective conductivity of soil extract [mS·cm–1] - vegetation optical depth - 6.6 vegetation optical depth at 6.6 GHz - 37 vegetation optical depth at 37 GHz - * effective vegetation optical depth (assuming =0) - single scattering albedo of vegetation With 12 Figures  相似文献   

12.
Several formulations and proposals to determine the value of the radiometric scalar roughness for sensible heatz 0h,r are tested with respect to their performance in the estimation of the sensible heat flux by means of the profile equations derived from Monin-Obukhov similarity theory. The equations are applied to the data set of spatially averaged surface skin temperature and profiles of wind speed and temperature observed in a pasture field during a growing season. The use of a physical model developed for a dense canopy to estimate scalar roughness for sensible heatz 0h,r produced sensible heat fluxH with a correlation coefficientr=0.884, the ratio of means being H s /H=1.19 in a comparison with reference values ofH s . In comparison, a proposal for a fixed value ofz 0h yieldedr=0.887, H s /H=0.879. In both cases, the validity ofz 0h =z 0h,r was assumed. All expressions derived to estimatez 0h,r from a multiple linear regression with such predictors as leaf area index, solar radiation and the ratio of solar radiation to extraterrestrial radiation, were found to produce a better result, withr better than 0.90 and H s /H around 1.0. However, when the constantsc andf of a linear regression equationHs=cH+f are used to evaluate the equations, a marked difference in performance of each formulation appeared. In general, equations with smaller numbers of predictors tend to produce a biased result, i.e., an overestimation ofH at largeH s . These values ofH are used in conjunction with the energy balance equation to derive values of the latent heat fluxLE, which are shown to be in good agreement with the reference valuesLE s , withr greater than 0.97.  相似文献   

13.
Flux densities of carbon dioxide were measured over an arid, vegetation-free surface by eddy covariance techniques and by a heat budget-profile method, in which CO2 concentration gradients were specified in terms of mixing ratios. This method showed negligible fluxes of CO2, consistent with the bareness of the experimental site, whereas the eddy covariance measurements indicated large downward fluxes of CO2. These apparently conflicting observations are in quantitative agreement with the results of a recent theory which predicts that whenever there are vertical fluxes of sensible or latent heat, a mean vertical velocity is developed. This velocity causes a mean vertical convective mass flux (= cw for CO2, in standard notation). The eddy covariance technique neglects this mean convective flux and measures only the turbulent flux c w. Thus, when the net flux of CO2 is zero, the eddy covariance method indicates an apparent flux which is equal and opposite to the mean convective flux, i.e., c w = – c w. Corrections for the mean convective flux are particularly significant for CO2 because cw and c w are often of similar magnitude. The correct measurement of the net CO2 flux by eddy covariance techniques requires that the fluxes of sensible and latent heat be measured as well.  相似文献   

14.
Summary The influence of agricultural management on the CO2 budget of a typical subalpine grassland was investigated at the Swiss CARBOMONT site at Rigi-Seebodenalp (1025m a.s.l.) in Central Switzerland. Eddy covariance flux measurements obtained during the first growing season from the mid of spring until the first snow fall (17 Mai to 25 September 2002) are reported. With respect to the 10-year average 1992–2001, we found that this growing season had started 10 days earlier than normal, but was close to average temperature with above-normal precipitation (100–255% depending on month). Using a footprint model we found that a simple approach using wind direction sectors was adequate to classify our CO2 fluxes as being controlled by either meadow or pasture. Two significantly different light response curves could be determined: one for periods with external interventions (grass cutting, cattle grazing) and the other for periods without external interventions. Other than this, meadow and pasture were similar, with a net carbon gain of –128±17g Cm–2 on the undisturbed meadow, and a net carbon loss of 79±17g Cm–2 on the managed meadow, and 270±24g Cm–2 on the pasture during 131 days of the growing season, respectively. The grass cut in June reduced the gross CO2 uptake of the meadow by 50±2% until regrowth of the vegetation. Cattle grazing reduced gross uptake over the whole vegetation period (37±2%), but left respiration at a similar level as observed in the meadow.  相似文献   

15.
A simple kinetic mechanism of nitrate radicals uptake on dry sea-salt NaCl, NaBr surfaces is proposed. The mechanism includes adsorption/desorption equilibrium and unimolecular decomposition of the adsorbed complex: NO3(g) + NaX(s) (NO3-NaX)(s); (NO3-NaX)(s) NaNO3 + X(s) Two techniques were used: the matrix isolation ESR and mass spectrometry. The uptake coefficient () is found to be dependent on exposure time of salt to NO3 for raw coating. The initial (t0) is higher than the observable steady-state obs. At room temperature obs is independent of [NO3] at low [NO3] = 3 × 109 - 1011 cm-3, but it is inversely proportional to [NO3] at concentrations higher than 1012 cm-3. At temperatures above 100 °C, obs becomes independent of [NO3] in a wider range of [NO3]. An increased number of dislocations is supposed to exist in the case of raw coating. Due to a wide spread of the surface sites binding energy with the ionic lattice near dislocations, the part of surface complexes has lower binding energy and "burns" more rapidly. That burning determines the transition from (t0) down to obs.The kinetic parameters and elementary rate coefficients are obtained. The recommended for low atmospheric NO3 concentration are in the range of 0.002 ± 0.04 for NaCl and 0.1-0.3 for NaBr depending on a mechanism of the (t) relaxation.  相似文献   

16.
Airborne measurements made during August 1985 over Greenland and its environs show that both accumulation-mode (0.1 m D2.0 m) and giant (D2 m) particles were present in relatively high concentrations in arctic haze layers and that the accumulation-mode particles dominated light scattering. Particles with diameters (D) between 1 and 4 m consisted predominately of mixed materials, small and dense inclusions, and probably organic compounds containing sulfur. Many of the particles from 0.1 to 1 m in diameter were also of mixed composition, with sulfuric acid, ammonium sulfate and organics probably the dominant constituents.  相似文献   

17.
We have examined the potential of using a closed-path sensor to accurately measure eddy fluxes of CO2. Five inlet tubeflow configurations were employed in the experimental setup. The fluxes of CO2 were compared against those measured with an open-path sensor. Sampling air through an intake tube causes a loss of flux, due to the attenuation of CO2 density fluctuations. Adjustments need to be made to correct for this loss and to account for density effects due to the simultaneous transfer of heat and water vapor. Theory quantifying these effects is discussed.The raw CO2 flux measured with the closed-path sensor was smaller than that measured with the open-path sensor by about 15% (on average) for the turbulent tubeflow configurations with a short (3 m) intake tube, by 31% for turbulent tubeflow with a longer (6 m) intake tube and by 24% for laminar tubeflow. The difference was, in part, caused by tube attenuation of the CO2 density fluctuations and inadequate sensor time response. The elimination of the flux adjustment for the simultaneous transfer of sensible heat (i.e., the attenuation of ambient temperature fluctuations in the intake tube) generally accounted for the rest of this difference.The raw flux measured with the closed-path sensor was corrected for frequency response and density effects. Except in the case of laminar tubeflow, the corrected closed-path flux agreed consistently with the corrected open-path flux within a few percent (<5%). These results suggest that closed-path sensors, with appropriate corrections, can be used to measure CO2 flux accurately. Recommendations are included on selecting an optimum flow configuration to minimize the effect of sampling air through a tube.Published as Paper No. 9938, Journal Series, Nebraska Agricultural Research Division.  相似文献   

18.
Turbulence measurements performed in a stable boundary layer over the sloping ice surface of the Vatnajökull in Iceland are described. The boundary layer, in which katabatic forces are stronger than the large-scale forces, has a structure that closely resembles that of a stable boundary layer overlying a flat land surface, although there are some important differences. In order to compare the two situations the set-up of the instruments on an ice cap in Iceland was reproduced on a flat grass surface at Cabauw, the Netherlands. Wind speed and temperature gradients were calculated and combined with flux measurements made with a sonic anemometer in order to obtain the local stability functions m and h as a function of the local stability parameter z/L. Unlike the situation at Cabauw, where m was linear as a function of z/L, in the katabatically forced boundary layer, the dependence of m on stability was found to be non-linear and related to the height of the wind maximum. Thermal stratification and the depth of the stable boundary layer however seem to be rather similar under these two different forcing conditions.Furthermore, measurements on the ice were used to construct the energy balance. These showed good agreement between observed melt and components contributing to the energy balance: net radiation (supplying 55% of the energy), sensible heat flux (30%) and latent heat flux (15%).Local sources and sinks in the turbulent kinetic energy budget are summed and indicate a reasonable balance in near-neutral conditions but not in more stable situations. The standard deviation of the velocity fluctuations u, v, and w, can be scaled satisfactorily with the local friction velocity u* and the standard deviation of the temperature fluctuation with the local temperature scale *.  相似文献   

19.
Wind and temperature profiles in the stable boundary layer were analyzed in the context of MoninObukhov similarity. The measurements were made on a 60-m tower in Kansas during October 1999 (CASES-99). Fluxprofile relationships, obtained from these measurements in their integral forms, were established for wind speed and temperature. Use of the integral forms eliminates the uncertainty and accuracy issues resulting from gradient computations. The corresponding stability functions, which were nearly the same for momentum and virtual sensible heat, were found to exhibit different features under weakly stable conditions compared to those under strongly stable conditions. The gradient stability functions were found to be linear, namely m = 1+ 5.8 and h = 1 + 5.4 up to a limit of the MoninObukhov stability parameter = 0.8; this is consistent with earlier findings. However, for stronger stabilities beyond a transition range, both functions were observed gradually to approach a constant, with a value of approximately 7. To link these two distinct regimes, a general but pliable functional form with only two parameters is proposed for the stability functions, covering the entire stability range from neutral to very stable conditions.  相似文献   

20.
The refractive index of air (n) mainly depends on temperature andwater vapour content. For near-infrared radiation, temperature isthe main determining factor. To determinethe structure parameter of temperature ( ) fromthe structure parameter of the refractive index( ), the influence ofwater vapour content on n needs to be taken into account as acorrection. Three levels of approximation are presented. The firstinvolves the standard deviations of T and q (T andq) as well as the correlation coefficient betweenT and q (RTq). The second approximation involvesRTq and the Bowen ratio (), and the last uses only the Bowen ratio.The latter is the classical Bowen ratio correction.Evaluation of the validity of the assumptions used in the derivationreveals that a large error may be introduced (for situations withRTq < 0.8) by replacing T/qwith the Bowen ratio.Consequently, estimating from using the Bowen ratiocan contain errors of 5–40% for || < 1. Adding RTqas extra information reduces the errors only marginally. For || > 1,the correction is small, and all three approximations give errors of lessthan 1% in . When is used to compute the sensible heat flux,the influence of the quality of the correction forwater vapour fluctuations on the measured energy balance is small: forsmall ||, the correction is large, but the absolute value ofthe heat flux is small, whereas for large ||, the correctionis insignificant.  相似文献   

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