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1.
The reactions of alkoxy radicals determine to a large extent the products formed during the atmospheric degradations of emitted organic compounds. Experimental data concerning the decompositions, 1,5-H shift isomerizations and reactions with O2 of several classes of alkoxy radicals are inconsistent with literature estimations of their absolute or relative rate constants. An alternative, although empirical, method for assessing the relative importance under atmospheric conditions of the reactions of alkoxy radicals with O2 versus decomposition was derived. This estimation method utilizes the differences in the heats of reaction, (H)=(Hdecomposition–HO 2 reaction), between these two reactions pathways. For (H)[22–0.5(HO 2 reaction)], alkoxy radical decomposition dominates over the reaction with O2 at room temperature and atmospheric pressure of air, while for (H)[25-0.5(HO 2 reaction)], the O2 reaction dominates over decomposition (where the units of H are in kcal mol–1). The utility and shortcomings of this approach are discussed. It is concluded that further studies concerning the reactions of alkoxy radicals are needed.  相似文献   

2.
Summary The performance of evaporation schemes with and approach and their combination within resistance representation of evaporation from bare soil surface is discussed. For this purpose nine schemes, based on different functions of or , on the ratio of the volumetric soil moisture content and its saturated value are used.The quality of the chosen schemes has been evaluated using the results of time integration by the coupled soil moisture and surface temperature prediction model, BARESOIL, using in situ data. A sensitivity analysis was made using two sets of data derived from the volumetric soil moisture content of the top soil layer. One with values below the wilting point (0.17 m3m–3) and the second with values above 0.20m3m–3. Data sets were obtained at the experimental site Rimski anevi, Yugoslavia, from the bare surface of a chernozem soil.With 4 Figures  相似文献   

3.
Measurements at Barrow during the second Arctic Gas and Aerosol Sampling Program (AGASP-II), conducted in April 1986, showed no rapid long-range transport from lower-latitude source regions to Barrow, and only limited vertical transport from above the boundary layer to the surface. New aerosol size distribution measurements in the 0.005–0.1 m diameter size range using a Nuclepore-filter diffusion battery apparatus showed a median diameter of about 0.01 m during times of high condensation nucleus (CN) concentrations. Aerosol black carbon concentrations exceeding 400 ng m–3 were detected at the surface and were more strongly correlated with CN concentrations than with aerosol scattering extinction (sp), suggesting that aerosol carbon was generally associated with small particles rather than large particles. Measurements at Barrow during AGASP-I, conducted in March–April 1983, showed a series of aerosol events detected at the ground that were caused by rapid long-range transport paths to the vicinity of Barrow from Eurasia. These events were strongly correlated with aerosol loading in the vertical column (optical depth).  相似文献   

4.
A numerical case study with a second-order turbulence closure model is proposed to study the role of urban canopy layer (UCL) for the formation of the nocturnal urban boundary layer (UBL). The turbulent diffusion coefficient was determined from an algebraic stress model. The concept of urban building surface area density is proposed to represent the UCL. Calculated results were also compared with field observation data. The height of the elevated inversion above an urban center was simulated and found to be approximately twice the average building height. The turbulent kinetic energy k, energy dissipation rate , and turbulence intensities u 2 and w 2 increase rapidly at the upwind edge of the urban area. The Reynolds stress uw displayed a nearly uniform profile inside the UBL, and the vertical sensible heat flux w had a negative value at the inversion base height. This indicates that the downward transport of sensible heat from the inversion base may play an important role in the formation of the nocturnal UBL.  相似文献   

5.
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   

6.
The rainwater composition in the vicinity of Mainz, FRG, has been investigated with special emphasis on insoluble constituents. The number size distribution was determined in the range from 0.1 m up to 100 m radius. For particles with r>0.5 m radius the shape of the size distribution of insoluble particles in rain follows the shape of the average urban and rural aerosol. In this particular size range no major size selective removal processes could be seen. For r<0.5 m the number size distribution tends to flatten compared to the average aerosol. This might be the indication of a size selective removal process (Greenfield Gap).  相似文献   

7.
The gas and particle phase reaction products of a mixture of the atmospherically important terpenes -pinene and -pinene with the atmospheric oxidants O3 and OH/NOx were investigated using both gas chromatography-mass spectrometry (GC-MS) and high performance liquid chromatography (HPLC) for identification and quantification of reaction products. The nighttime oxidation of a mixture of -pinene and -pinene in the presence of O3/air, and the daytime oxidation of a mixture of -pinene + -pinene with NOx air in the presence of natural sunlight were carried out in the University of North Carolina's large outdoor smog chamber (190 m3) located in Chatham County, North Carolina. Mass balances for gaseous and aerosol reaction products are reported over the course of the reaction. More than twenty-nine products were identified and/or quantified in this study. On average, measured gas and particle phase products accounted for 74 to 80% of the reacted -pinen/-pinene mixture carbon. Measurements show that a number of reaction products were found in both O3 and NOx system [pinonaldehyde, pinic acid, pinonic acid, pinalic-3-acid, 4-hydroxypinalic-3-acid, 4-oxonopinone, 1-hydroxy-nopinone, 3-hydroxy-nopinone, and nopinone]. Pinonic acid, pinic acid, pinalic-3-acid, 4-hydroxypinalic-3-acid, and 10-hydroxypinonic acid were observed in the early stage in the aerosol phase and may play an important role in the early formation of secondary aerosols.  相似文献   

8.
Six locations across mainland Portugal were selected for exposing Parmelia sulcata, for a one-year period (8 months for one site), with simultaneous measurement of total (dry + wet) deposition (one-month periods). The exposed lichens and the total (dry + wet) deposition were analysed for cobalt contents by INAA (instrumental neutron activation analysis) and ICP-MS (inductively coupled plasma mass spectroscopy), respectively. The designated wet deposition was evaluated through the collected water volume; the designated dry deposition was assessed after the (dried) residual mass of the wet deposition. An excellent agreement between Co contents in exposed lichens and the cumulative (1) Co contents in the dry deposition, (2) dry deposition, and (3) wet deposition has been found for the locations with alternate drought and precipitation months, high dry deposition, and high Co contents in the latter. Continuous rainfall was found to hinder the Co accumulation in the lichen due to its release from the lichen and/or lower Co contents in the dry deposition. At three locations, P. sulcata Co contents, after subtraction of the background (before exposure), equalled or exceeded the Co contents in the cumulative dry deposition at the end of the exposure time. The optimal exposure period for this species likely depends on the exposure conditions.  相似文献   

9.
Analyses indicate that the Atlantic Ocean seasurface temperature (SST) was considerably colder at the beginning than in the middle of the century. In parallel, a systematic change in the North Atlantic sea-level pressure (SLP) pattern was observed. To find out whether the SST and SLP changes analyzed are consistent, which would indicate that the SST change was real and not an instrumental artifact, a response experiment with a low-resolution (T21) atmospheric GCM was performed. Two perpetual January simulations were conducted, which differ solely in the Atlantic Ocean (40° S-60° N) SST: the cold simulation utilizes the SSTs for the period 1904–1913; the warm simulation uses the SSTs for the period 1951–1960. Also, a control run with the model's standard SST somewhat between the cold and warm SST was made. For the response analysis, a rigorous statistical approach was taken. First, the null hypothesis of identical horizontal distributions was subjected to a multivariate significance test. Second, the level of recurrence was estimated. The multivariate statistical approaches are based on hierarchies of test models. We examined three different hierarchies: a scale-dependent hierarchy based on spherical harmonics (S), and two physically motivated ones, one based on the barotropic normal modes of the mean 300 hPa flow (B) and one based on the eigenmodes of the advection diffusion operator at 1000 hPa (A). The intercomparison of the cold and warm experiments indicates a signal in the geostrophic stream function that in the S-hierarchy is significantly nonzero and highly recurrent. In the A-hierarchy, the low level temperature field is identified as being significantly and recurrently affected by the altered SST distribution. The SLP signal is reasonably similar to the SLP change observed. Unexpectedly, the upper level stream-function signal does not appear to be significantly nonzero in the B-hierarchy. If, however, the pairs of experiments warm versus control and cold versus control are examined in the B-hierarchy, a highly significant and recurrent signal emerges. We conclude that the cold versus warm response is not a small disturbance that would allow the signal to be described by eigenmodes of the linear system. An analysis of the three-dimensional structure of the signal leads to the hypothesis that two different mechanisms are acting to modify the model's mean state. At low levels, local heating and advection are dominant, but at upper levels the extratropical signal is a remote responce to modifications of the tropical convection.This paper was presented at the International Conference on Modelling of Global Climate Change and Variability, held in Hamburg 11–15 September 1989 under the auspices of the Meteorological Institute of the University of Hamburg and the Max Planck Institute for Meteorology. Guest Editor for these papers is Dr. L. Dilmenil.AWI Publication no. 254  相似文献   

10.
As a component of the Canadian Arctic Haze Study, held coincident with the second Arctic Gas and Aerosol Sampling Program (AGASP II), vertical profiles of aerosol size distribution (0.17 m), light scattering parameters and cloud particle concentrations were obtained with an instrumented aircraft and ground-based lidar system during April 1986 at Alert. Northwest Territories. Average aerosol number concentrations range from about 200 cm–3 over the Arctic ice cap to about 100 cm–3 at 6 km. The aerosol size spectrum is virtually free of giant or coarse aerosol particles, and does not vary significantly with altitude. Most of the aerosol volume is concentrated in the 0.17–0.50 m size range, and the aerosol number concentration is found to be a good surrogate for the SO4 = concentration of the Arctic haze aerosol. Comparison of the aircraft and lidar data show that, when iced crystal scattering is excluded, the aerosol light scattering coefficient and the lidar backscattering coefficient are proportional to the Arctic haze aerosol concentration. Ratios of scattering to backscattering, scattering to aerosol number concentration, and backscattering to aerosol number concentration are 15.3 steradians, 1.1×10–13 m2, and 4.8×10–15 m2 sr–1, respectively. Aerosol scattering coefficients calculated from the measured size distributions using Mie scattering agree well with measured values. The calculations indicate the aerosol absorption optical depth over 6 km to range between 0.011 and 0.018. The presence of small numbers of ice crystals (10–20 crystals 1–1 measured) increased light scattering by over a factor of ten.  相似文献   

11.
Summary The effect of the Alpine orography on prototype cold fronts approaching from the west is investigated by three-dimensional numerical model simulations. The numerical experiments cover a range of parameter constellations which govern the prefrontal environment of the front. Especially, the appearance and intensity of prefrontal northern Alpine foehn varies from case to case.The behaviour of a cold front north of the Alps depends much on the prefrontal condition it encounters. It is found that prefrontal foehn can either accelerate or retard the approaching front.An important feature is the pressure depression along the northern Alpine rim that results from the southerly foehn flow. In cases where this depression compensates the eastward directed pressure gradient associated with the largescale flow, the front tends to accelerate and the foehn breaks down as soon as the front passes. In contrast, the foehn prevents the front from a rapid eastward propagation if it is connected with a strong southerly wind component.No-foehn experiments are performed for comparison, where either the mountains are removed, or the static stability is set to neutral. Also shown are effects of different crossfrontal temperature contrasts.List of Symbols c F propagation speed of a front - x, y horizontal grid spacing (cartesian system) - , horizontal grid spacing (geographic system) - t time step - z vertical grid spacing (cartesian system) - cross-frontal potential temperature difference - i potential temperature step at an inversion - E turbulent kinetic energy - f Coriolis parameter - FGP frontogenesis parameter (see section 2.2) - g gravity acceleration (g=9.81 m s–2) - vertical gradient of potential temperature - h terrain elevation (above MSL) - h i height of an inversion (h i =1000 m MSL) - H height of model lid (H=9000 m MSL) - K M exchange coefficient of momentum - K H exchange coefficient of heat and moisture - longitude - N Brunt-Väisäla-frequency - p pressure - Exner function (=T/) - latitude - q v specific humidity - R d gas constant of dry air (R d =287.06 J kg–1 K–1) - density of dry air - t time - T temperature - potential temperature - TFP thermal front parameter (see section 2.2) - u, v, w cartesian wind components - u g ,v g geostrophic wind components - horizontal wind vector - x, y, z cartesian coordinates Abbreviations GND (above) ground level - MSL (above) mean sea level - UTC universal time coordinated With 20 Figures  相似文献   

12.
E- turbulence model predictions of the neutralatmospheric boundary layer (NABL) are reinvestigated to determine thecause for turbulence overpredictions found in previous applications. Analytical solutions to the coupled E and equations for the case of steady balance between transport and dissipation terms, the dominant balance just below the NABL top, are derived. It is found that analytical turbulence profiles laminarizeat a finite height only for values of closure parameter ratio c 2 /e equal toor slightly greater than one, with laminarization as z for greater . The point = 2 is additionally foundthat where analytical turbulent length scale (l) profilesmade a transition from ones ofdecreasing ( < 2) to increasing ( > 2)values with height. Numerically predicted profiles near the NABL topare consistent with analytical findings. The height-increasingvalues of l predicted throughout the NABL with standard values ofclosure parameters thus appear a consequence of 2.5(> 2), implied by these values (c 2 = 1.92, = 1.3, e = 1). Comparison of numericalpredictions with DNS data shows that turbulence overpredictions obtained with standard-valued parameters are rectifiedby resetting and e to 1.1 and 1.6, respectively, giving, with c 2 = 1.92, 1.3, and laminarization of the NABL's cappingtransport-dissipation region at a finite height.  相似文献   

13.
This study examines the statistical properties of the concentration derivative, , for a dispersing plume in a near-neutrally stratified atmospheric surface layer. Towards this goal, the probability density function (pdf) of , and the conditional pdf of given a fixed concentration level, , have been measured. These pdfs are found to be modeled well by a generalizedq-Gaussian (gqG) distribution with intermittency exponent,q, equal to 0.3 and 3/4, respectively. These results highlight the strong intermittency effect (patchiness) of the small-scale concentration eddy structures in the plume. The distribution of time intervals between successive high peaks in the squared derivative process, x2, is found to be well approximated by a power-law distribution, implying that occurrences of these high peaks are much more clustered than would be predicted by a Poisson or shot-noise process. The results are used to improve models for the joint pdf of and , and for the expected number of upcrossings per unit time interval of a fixed concentration level that have been proposed by Kristensenet al. (1989). The predictions of the improved models are in accord with observations, and suggest that the intercorrelation between and must be explicitly incorporated if good estimates of the upcrossing intensity are to be obtained.  相似文献   

14.
Cloud water and interstitial aerosol samples collected at Mt. Sonnblick (SBO) were analyzed for sulfate and aerosol carbon to calculate in-cloud scavenging efficiencies. Scavenging efficiencies for sulfate (SO) ranged from 0.52 to 0.99 with an average of 0.80. Aerosol carbon was scavenged less efficiently with an average value (AC) of 0.45 and minimum and maximum values of 0.14 and 0.81, respectively. Both SO and AC showed a marked, but slightly different, dependence on the liquid water content (LWC) of the cloud. At low LWC, SO increased with rising LWC until it reached a relatively constant value of 0.83 above an LWC of 0.3 g/m3. In the case of aerosol carbon, we obtained a more gradual increase of AC up to an LWC of 0.5 g/m3. At higher LWCs, _ remained relatively constant at 0.60. As the differences between SO and A varied across the LWC range observed at SBO, we assume that part of the aerosol carbon was incorporated into the cloud droplets independently from sulfate. This hypothesis is supported by size classified aerosol measurements. The differences in the size distributions of sulfate and total carbon point to a partially external mixture. Thus, the different chemical nature and the differences in the size and mixing state of the aerosol particles are the most likely candidates for the differences in the scavenging behavior.  相似文献   

15.
Atmospheric oxidation of monoterpenes contributes to formation of tropospheric ozone and secondary organic aerosol, but their products are poorly characterized. In this work, we report a series of outdoor smog chamber experiments to investigate both gaseous and particulate products in the ozone oxidation of four monoterpenes: -pinene, -pinene, 3-carene, and sabinene. More than ten oxygenated products are detected and identified in each monoterpene/O3 reaction by coupling derivatization techniques and GC/MS detection. A denuder/filter pack sampling system is used to separate and simultaneously collect gas and aerosol samples. The identified products, consisting of compounds containing carbonyl, hydroxyl, and carboxyl functional groups, are estimated to account for about 34–50%, 57%, 29–67%, and 24% of the reacted carbon mass for -pinene, sabinene, -pinene, and 3-carene, respectively. The identified individual products account for >83%, 100%, >90%, and 61% of the aerosol mass produced in the ozone reaction of -pinene, sabinene, -pinene, and 3-carene. The uncertainty in the yield data is estimated to be ±50%. Many of the products partition between gas and aerosol phases, and their gas-aerosol partitioning coefficients are determined and reported here. Reaction schemes are suggested to account for the products observed.  相似文献   

16.
Plume dispersion in the convective boundary layer (CBL) is investigated experimentally in a laboratory convection tank. The focusis on highly-buoyant plumes that loft near or become trapped in the CBL capping inversion and resistdownward mixing. Such plumes are defined by dimensionless buoyancy fluxes F* 0.1, where F* = Fb/(U w* 2 zi), Fb is the stack buoyancy flux,U is the mean wind speed, w* is the convective velocity scale, and zi is the CBL depth. The aim is to obtain statistically-reliable mean (C) and root-mean-square (rms, c) concentration fields as a function of F* and the dimensionless distance X = w*x/(U zi), where x is the distance downstream of the source.The experiments reveal the following mainresults: (1) For 3 X 4and F* 0.1, the crosswind-integrated concentration (CWIC) fields exhibit distinctly uniform profiles below zi with a CWIC maximum aloft, in contrast to the nonuniform profiles obtained earlier by Willis and Deardorff. (2) The lateral dispersion (y) variation with X is consistent with Taylor's theory for * 0.1 and a buoyancy-enhanced dispersion, y/zi F* 1/3X2/3, forF* = 0.2 and 0.4. (3) The entrapment, the plume fraction above zi, has a mean (E) that follows a systematic variationwith X and F*, and a variability (e/E) that is broad ( 0.3 to 2) near the source but subsides to 0.25 far downstream. (4) Vertical profiles of the concentration fluctuation intensity (c/C) are uniform for z < zi and X > 1.5, but exhibit significant increases: (a) at the surface and close to the source (X 1.5), and(b) in the entrainment zone. (5) The cumulative distribution functions (CDFs) of the scaled concentration fluctuations (c/c) separate into mixed-layer and entrainment-layer CDFs for X 2, with the mixed-layer group collapsing to a single distribution independent of z.These are the first experiments to obtain all components of the lateral and vertical dispersion parameters (rms meander, relative dispersion, total dispersion) for continuous buoyant releases in a convection tank. They also are the first tank experiments to demonstrate agreement with field observations of: (1) the scaled ground-level concentration along the plume centreline, and (2) the dimensionless lateral dispersion _y/z_i of buoyant plumes.  相似文献   

17.
Recently Wilson and Flesch (Boundary-Layer Meteorology, 84, 411-426, 1997) suggested that the average increment d z to the orientation = arctan(w/u) of the Lagrangian velocity-fluctuation vector can be used to distinguish the better Lagrangian stochastic models within the well-mixed class. Here it is demonstrated that the specification of d z constitutes neither a sufficient or universally applicable criterion to distinguish the better Lagrangian stochastic models within the well-mixed class. The hypothesis made by Wilson and Flesch that Lagrangian stochastic models with /PE irrotational are zero-spin models, having d z=0, is proven  相似文献   

18.
Thermal comfort of man in different urban environments   总被引:2,自引:4,他引:2  
Summary On July 29, 1985, a hot summer day, biometeorological measurements were performed simultaneously in three different urban structures within the city of Munich and in the trunk space of a nearby tall spruce forest. Based on the results of these experiments the following thermophysiologically relevant biometeorological indices were calculated: Predicted mean vote, skin wettedness and physiologically equivalent temperature. These three indices are derived from different models for the human energy balance. They allow the assessment of the thermal components of the microclimates at the selected sites with regard to application in urban planning. The results quantitatively show the great heat stress in the urban structure street canyon, exposed to south, whereas in the trunk space of the tall spruce forest there is nearly an optimal climate even on hot summer days. Between these extremes the results for street canyon, exposed to north show a little higher heat load than for backyard with trees.
Zusammenfassung An einem heißen Sommertag, dem 29. Juli 1985, wurden in drei Stadtstrukturen in München und im Stammraum eines nahegelegenen Fichtenhochwaldes zeitgleich biometeorologische Messungen durchgeführt. Mit den Meßergebnissen wurden folgende thermophysiologisch relevante biometeorologische Indizes berechnet: Predicted mean vote, Hautbenetzungsgrad und physiologisch äquivalente Temperatur. Diese drei Indizes beruhen auf verschiedenen Modellen zur menschlichen Energiebilanz. Mit den drei Indizes wurden die thermischen Komponenten der Mikroklimate an den ausgewählten Meßplätzen im Hinblick auf Stadtplanungsaufgaben bewertet. Die Ergebnisse zeigen quantitativ die relativ große Hitzebelastung bei der Stadtstruktur Straßenschlucht, nach Süd exponiert, während im Stammraum des Fichtenhochwaldes selbst an heißen Sommertagen nahezu optimale Bedingungen herrschen. Zwischen diesen Extremen liegen die Ergebnisse für die anderen Meßplätze, wobei für Straßenschlucht, nach Nord exponiert die Wärmebelastung etwas höher als für Innenhof mit Bäumen ist.


With 6 Figures  相似文献   

19.
The carbon isotopic ratio of atmospheric carbon dioxide at Tsukuba,Japan   总被引:1,自引:0,他引:1  
To find out the secular and seasonal trends of the 13C value and CO2 concentration in the surface air and the determination of the 13C in the atmospheric CO2 collected at Tsukuba Science City was carried out during the period from July 1981 to October 1983. The monthly average of the 13C value of CO2 in the surface air collected at 1400 LMT ranged from -7.52 to \s-8.45 with an average of -7.96±0.25 and the CO2 concentration in the air varied from 334.5 l 1-1 to 359 l 1-1 with an average of 347.2±6.3 l 1-1. The 13C value is high in summer and low in winter and is negatively correlated with the CO2 concentration. In general, the relationship between the 13C and the CO2 concentration is explainable by a simple mixing model of two different constant carbon isotopic species but the relationship does not always follow the model. The correlation between the 13C value and the CO2 concentration is low during the plant growth season and high at other times. The observed negative deviation of the 13C value from the simple mixing model in the plant growth season is partly due to the isotopic fractionation process which takes place in the land biota.  相似文献   

20.
Summary An analysis of the report of the (U.S.) National Academy of Sciences (NAS) on atmospheric effects of a nuclear exchange leads to conclusions that differ from those of the NAS and of the earlier TTAPS and AMBIO studies. Any cooling of the earth's surface is likely to beshort-lived because of rapid removal of the smoke clouds originating from nuclear burst-initiated fires, andminor because of appreciable green-house effects due to several distinct physical causes. (One of these, neglected in prior analyses, is the infrared absorption from cirrus clouds produced directly by the nuclear bursts.) Taken together, these effects may even induce slight surface warming (nuclear summer) instead of cooling (nuclear winter). The consequences to atmospheric ozone are similarly ambiguous; depending on the detailed nuclear scenario, the net ozone content may increase-rather than decrease as argued by TTAPS. Experiments could settle some uncertainties.With 2 Figures  相似文献   

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