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1.
The fluxes of ozone and NOx out of the atmospheric boundary layer (ABL) over Europe are calculated in a mesoscale chemical transport model (MCT) and compared with the net chemical production or destruction of ozone and the emissions of precursors within the ABL for two 10 days' periods which had quite different synoptic situations and levels of photochemical activity (1–10 July 1991 (JUL91) and 26 October–4 November 1994 (ON94)). Over the European continent, about 8% of the NOx emissions were brought from the ABL to the free troposphere as NOx, while about 15% of the NOx emissions were brought to the free troposphere as NOy–NOx, i.e. as PAN or HNO3. The convection dominates over the synoptic scale vertical advection as a transport mechanism both for NOx and NOy out of the boundary layer in the summertime high pressure situation (JUL91), while in the fall situation (ON94) the convective part was calculated to be the smallest. NOx was almost completely transformed to NOy–NOx or removed within the ABL. Also for NOy the major part of the atmospheric cycle is confined to the ABL both for JUL91 and ON94. The vertical transport time out of the ABL is of the order of 100h both for the total model domain and over the European continent. The net convective exchange of ozone from the ABL is not a dominant process for the amount of ozone in the ABL averaged over 10 days and the whole domain, but convection reduces the maximum ozone concentration in episodes significantly. The ozone producing efficiency of NOx is calculated to increase with height to typically 15–20 in the upper half of the troposphere from around 5 in the ABL, but in the middle free troposphere the concentration of NOx is often too low to cause net chemical formation of ozone there.  相似文献   

2.
During the BERLIOZ field phase on 20 July 1998 a 40 km wide ozone-plume 30 to 70 km north of Berlin in the lee of the city was detected. The ozone mixing ratio inside the plume was app. 15 ppb higher than outside, mainly caused by high ozone precursor emissions in Berlin, resulting in a net chemical ozone production of 6.5 ppb h–1, which overcompensates ozone advection of –3.6 ppb h–1 andturbulent diffusion of –1.1 ppb h–1. That means, although moreozone leaves the control volume far in the lee of Berlin than enters it at the leeside cityborder and although turbulent diffusion causes a loss of ozone in the leeside control volume the chemical production inside the volume leads to a net ozone increase. Using a semi-Lagrangian mass budget method to estimate the net ozone production, 5.0 ppb h–1 are calculated for theplume. This means a fraction of about 20% of ozone in the plume is producedby local emissions, therefore called `home made' by the Berlin emissions. For the same area KAMM/DRAIS simulations using an observation based initialisation, results in a net production rate between 4.0 and 6.5 ppbh–1, while the threefold nested EURAD model gives 6.0 ppbh–1. The process analysis indicates in many cases goodagreement (10% or better) between measurements and simulations not only in the ozone concentrations but also with respect to the physical and chemical processes governing the total change. Remaining differences are caused by different resolution in time and space of the models and measurements as well as by errors in the emission calculation.The upwind-downwind differences in PAN concentrations are partly similar to those of ozone, because in the BERLIOZ case they are governed mainly by photochemical production. While in the stable boundary layer at night and windward of Berlin 0.1 to 0.3 ppb are detected, in the centre of the plume at noon concentrations between 0.75 ppb and 1.0 ppb are measured. The O3/PAN ratio is about 80 to 120 and thus due to the relatively lowPAN concentrations significantly higher than found in previous studies. The low PAN formation on 20 July, was mainly restricted by the moderate nonmethane hydrocarbon levels, whereas high PAN concentrations of 3.0 ppb on 21 July, are caused by local production in the boundary layer and by large scale advection aloft.  相似文献   

3.
In this paper we try to identify and describe the specifics of the Berlin city plume characterised by a zone of enhanced photochemical activity downwind of the urban area, where the major emissions of ozone precursors (NOx and VOC) take place. Two Eulerian CTM systems (EURAD and REM3/CALGRID) and one Euler–Lagrangian model (LaMM5) are applied to thearea of Berlin/Brandenburg to investigate the processes involved in the evolution of the Berlin plume inherent to the models. The study focuses on 20 July 1998,the first special observation period (SOP) during BERLIOZ. The examination includes (1) the role of turbulence and transport and the role of mass flux to the surface during the evolution of the plume, (2) the import situation of the ground based measurement sites, (3)the terms of the ozone budget equation and their contribution to precursor distribution and ozone formation, (4) the substructures of the plume defined by its chemical regimes. Main results show that the complex meteorological conditions during this SOP with considerable turbulent transports demand an Euler–Lagrangian approach to determine the source receptor relationshipsfor the ground based measurement sites. These relations reveal that only a minor part (5%) of the air approaching Pabstthum and the more downwind (north-western) stations origins from Berlin and that the mutual transport between all sites was limited. The latter result afflicts the joint interpretation of data from different stations because the presumption to measure the same air mass is violated in many cases for this SOP. The CTM results reveal that the local net production of ozone within the plume was controlled by transport ad chemical processes both owning the same importance but tending to counteract each other. At this SOP far distance sources of ozone precursors originating from the Bohemian basin did not interfere the Berlin city plume although they generally have the potential to do so.  相似文献   

4.
Summary A diagnostic model (DIAMOD) for the atmosphere over Europe is use at the University of Vienna. Central parameters in each diagnostic column (horizontal resolution 100 km, time resolution 12 hours) are the vertical moisture plus heat flux (the total convective heat fluxh) and the vertical rain flux (r); both are functions of pressure. In this study DIAMOD is applied to validate the output of a forecast model for the simulation of acid deposition (EURAD) which is in use at the University of Cologne. The basic equations of both DIAMOD and EURAD models are summarized with emphasis on the sub-gridscale hydrologic components.First, the nontrivial problem of validating model output versus observations is discussed. Two different validation techniques based upon the budget equations are indentified. The fully prognostic technique compares the forecast of EURAD for the total verification period with the corresponding DIAMOD output. The semiprognostic validation technique involves only one-time-step tendencies. Neither yields an exact correspondence between EURAD and DIAMOD; however, the semiprognostic technique comes somewhat closer to the ideal of an objective validation. The quantities investigated are: The fields, the time tendencies and the fluxesh andr.Second, EURAD is validated versus DIAMOD with both techniques for the EUMAC Joint Wet Case (the Chernobyl episode) in April 1986; the output fields include selected profiles ofh(p) over France (a moist night situation) and over Greece (a dry day situation). The comparison demonstrates for both that the EURAD forecasts are acceptable for ther-fluxes but are relatively poor for theh-fluxes. Reasons for the differences are discussed.With 11 Figures  相似文献   

5.
Model calculations and field measurements have shown that when air masses accumulate emissions of hydrocarbons and nitrogen oxides from sources in continental Europe and then move towards Scandinavia without any synoptic scale break-up of the atmospheric boundary layer (e.g. frontal passages), elevated PAN concentrations in southern Norway or Sweden in the range 1–5 ppb may be caused by long-range transport. The model calculations showed that over sea, the persistence of PAN was comparable to that of ozone in an ageing air mass when the temperatures were fairly low (5–10°C). At higher temperatures the thermal decomposition of PAN made the compound less persistent than ozone. Over land, the situation may be different since the ground removal is typically three times more efficient for ozone than for PAN.According to the model, the concentration of PAN did not change very much when an ageing air mass was exposed to moderate emissions of hydrocarbons, nitrogen oxides, or both. The concentration of PAN decreased less than the concentration of ozone when an ageing air mass was exposed to high emissions of nitrogen oxides.  相似文献   

6.
Summary In this paper the results of simulations of air pollution carried out with the mesoscale model system KAMM/DRAIS are presented. They are compared with results of the European scale model EURAD which have been provided by the EURAD-Group, Cologne. With this comparison it is intended to analyse to what extent better resolution of topography and emission data used by the mesoscale model effects the model results. The simulations have been carried out for July 15, 1986, a typical summer day. The model domain contains south-west Germany and part of Alsace with a resolution of 5 km. The emissions for this resolution have been derived by a combination of the coarse EURAD emission data with the data of the TULLA experiment which are available on a much finer grid. The initial and boundary conditions for the species concentrations are determined from the results of the EURAD model. This coupling introduces the long range transport of pollutants into the mesoscale simulation.The meteorological and concentration data of the EURAD model are compared with the corresponding DRAIS model results. The mesoscale flow field is characterized by the channeling along the Upper Rhine Valley, which is not resolved in the EURAD model. The concentration distributions of both models are similar during midday, because of the strong vertical mixing. In the night and especially, in the morning and evening hours the spatial distribution is much better represented by the DRAIS model results. The better resolution of the emissions and the topography in the DRAIS model compared with the EURAD model (80 km grid size) becomes really noticeable. The difference of the ozone concentrations between cities and the, surrounding areas and between the Rhine Valley and the limiting mountains are in the order of 30 ppb as compared to a few ppb in the EURAD simulation. In the morning NO concentrations of about 200 ppb are simulated in the area between Heilbronn and Stuttgart. The EURAD model provides only about 5 ppb. Comparisons with measurements show that the DRAIS simulations are more realistic than the EURAD model results. The features mentioned are also found in an evaluation of the concentration variations in areas corresponding to a grid cell of the EURAD model. Two completely different areas are selected to demonstrate the possible range of the concentration variation. In the area around the City of Stuttgart the ozone concentration in the morning and the evening varies between zero ppb and 50 ppb, approximately. The mean value is nearly the same in both simulations.List of Abbreviations DRAIS Dreidimensionales Regionales Ausbreitungsund Immissions-Simulationsmodell - EMEP European co-operative program for Monitoring and Evaluation of the long-range transmission of air Pollutants - EUMAC European Modelling of Atmospheric Constituents - EURAD European Acid Deposition Model - EUROTRAC EUROpean experiment on TRAnsport and transformation of environmentally relevant trace Constituents in the troposphere over Europe - JDR Joint Dry Case - KAMM Karlsruher Atmosphärisches Mesoskaliges Modell - MM4 Mesoscale Model 4 - NCAR National Center for Atmospheric Research - RADM Regional Acid Deposition Model - TADAP Transport and Deposition of Acidifying Pollutants - TULLA Transport und Umwandlung von Luftschadstoffen im Lande Baden-Württemberg und aus Anrainerstaaten; in English: Transport and Transformation of Air Pollutants in the State of Baden-Württemberg and from neighbouring countries With 17 Figures  相似文献   

7.
The oxidation of nonmethane hydrocarbons represents a source of tropospheric ozone that is primarily confined to the boundary layers of several highly industrialized regions. (Each region has an area greater than one million km2). Using a photochemical model, the global tropospheric ozone budget is reexamined by including the in-situ production from these localized regimes. The results from these calculations suggest that the net source due to this photochemistry, which takes place on the synoptic scale, is approximately as large as the amount calculated for global scale photochemical processes which consider only the oxidation of methane and carbon monoxide. Such a finding may have a considerable impact on our understanding of the tropospheric ozone budget. The model results for ozone show reasonable agreement with the climatological summer distribution of ozone and the oxides of nitrogen at the surface and with the vertical distribution of ozone and nonmethane hydrocarbons obtained during a 1980 field program.  相似文献   

8.
我国北方地区对流层中下层臭氧收支   总被引：1，自引：0，他引：1       下载免费PDF全文
为了揭示我国北方地区对流层中下层臭氧(O3) 的形成机理以及周边地区的污染输送对我国北方地区对流层中下层O3收支的影响, 在与外场观测数据比较分析的基础上, 利用全球化学输送模式(MOZART-2) 采用收支分析方法定量分析了影响我国北方地区对流层中下层O3的各个物理化学过程。结果表明:我国北方地区对流层下层O3最重要的来源是光化学生成作用, 约占总来源的58.3%(41.5 Tg), 光化学生成反应中HO2对于O3生成的贡献最大; 最大的汇是干沉降过程, 约占总汇的43.2%(26.2Tg); 水平净输送作用对我国北方地区对流层中下层O3收支的影响非常大, 在我国北方地区对流层下层, 41.6%左右的O3来自水平净输送, 随高度增加, 水平输送影响增大, 我国北方地区对流层中层大约81.5%的O3来自水平净输送。  相似文献   

9.
Summary An aircraft-based experimental investigation of the atmospheric boundary layer (ABL) structure and of the energy exchange processes over heterogeneous land surfaces is presented. The measurements are used for the validation of the mesoscale atmospheric model “Lokal-Modell” (LM) of the German Weather Service with 2.8 km resolution. In addition, high-resolution simulations using the non-hydrostatic model FOOT3DK with 250 m resolution are performed in order to resolve detailed surface heterogeneities. Two special observation periods in May 1999 show comparable convective boundary layer (CBL) conditions. For one case study vertical profiles and area averages of meteorological quantities and energy fluxes are investigated in detail. The measured net radiation is highly dependent on surface albedo, and the latent heat flux exhibits a strong temporal variability in the investigation area. A reduction of this variability is possible by aggregation of multiple flight patterns. To calculate surface fluxes from aircraft measurements at low altitude, turbulent energy fluxes were extrapolated to the ground by the budget method, which turned out to be well applicable for the sensible heat flux, but not for the latent flux. The development of the ABL is well captured by the LM simulation. The comparison of spatiotemporal averages shows an underestimation of the observed net radiation, which is mainly caused by thin low-level clouds in the LM compared to observed scattered CBL clouds. The sensible heat flux is reproduced very well, while the latent flux is highly overestimated especially above forests. The realistic representation of surface heterogeneities in the investigation area in the FOOT3DK simulations leads to improvements for the energy fluxes, but an overestimation of the latent heat flux still persists. A study of upscaling effects yields more structures than the LM fields when averaged to the same scale, which are partly caused by the non-linear effects of parameter aggregation on the LM scale.  相似文献   

10.
Turbulent fluxes of sensible and latent heat and ozone were measured aboard a German Aerospace Research Establishment motorglider over the Swiss Plateau during the first field experiment of the Swiss air pollution experiment POLLUMET. In the lower part of the boundary layer, the ozone fluxes are negative (downward) throughout the day as a result of deposition and photochemical destruction at the surface. In the upper part of the boundary layer, the ozone fluxes tend to be negative until mid-afternoon and then become positive. The change in sign occurs after the ozone concentration in the boundary layer exceeds that in the reservoir above the inversion. Downdrafts bringing air parcels with ozone deficits across the inversion then become major contributors to the flux. The positive fluxes at upper levels result in an increase in flux divergence in mid-afternoon that is balanced by a relatively large source term in the ozone concentration budget.  相似文献   

11.
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   

12.
Ozone throughout the troposphere is subject of significant temporal and spatial variability due to photochemical production in the planetary boundary layer and free troposphere, stratospheric intrusions, convective events and long range transport. However, high resolving observations of ozone in the troposphere are generally rare today. That is of special disadvantage for limited area models, which represent mathematically a differential equation system with an initial and boundary problem. As ozone concentrations usually increase from the earth surface to the stratosphere, a proper choice of the background ozone concentrations is necessary to reproduce or even predict the amount and distribution of ozone in a specific region of interest.In this paper the impact of background concentrations of ozone on regional scale model results is analysed during a summer smog episode over Europe. For this purpose ozone is artificially partitioned into individual categories. For each category, transport and chemical transformation is calculated separately. Initial and boundary concentrations of ozone dominate total ozone concentrations increasingly with height. But also in the planetary boundary layer they contribute with more than 30% to thetotal ozone changes and are therefore far from being negligible. Moderately modified assumptions of background ozone concentrations reveal an uncertainty of near surface ozone concentrations of 5–15%depending on the weather situation.  相似文献   

13.
Within the CIRCE project “Climate change and Impact Research: the Mediterranean Environment”, an ensemble of high resolution coupled atmosphere–ocean regional climate models (AORCMs) are used to simulate the Mediterranean climate for the period 1950–2050. For the first time, realistic net surface air-sea fluxes are obtained. The sea surface temperature (SST) variability is consistent with the atmospheric forcing above it and oceanic constraints. The surface fluxes respond to external forcing under a warming climate and show an equivalent trend in all models. This study focuses on the present day and on the evolution of the heat and water budget over the Mediterranean Sea under the SRES-A1B scenario. On the contrary to previous studies, the net total heat budget is negative over the present period in all AORCMs and satisfies the heat closure budget controlled by a net positive heat gain at the strait of Gibraltar in the present climate. Under climate change scenario, some models predict a warming of the Mediterranean Sea from the ocean surface (positive net heat flux) in addition to the positive flux at the strait of Gibraltar for the 2021–2050 period. The shortwave and latent flux are increasing and the longwave and sensible fluxes are decreasing compared to the 1961–1990 period due to a reduction of the cloud cover and an increase in greenhouse gases (GHGs) and SSTs over the 2021–2050 period. The AORCMs provide a good estimates of the water budget with a drying of the region during the twenty-first century. For the ensemble mean, he decrease in precipitation and runoff is about 10 and 15% respectively and the increase in evaporation is much weaker, about 2% compared to the 1961–1990 period which confirm results obtained in recent studies. Despite a clear consistency in the trends and results between the models, this study also underlines important differences in the model set-ups, methodology and choices of some physical parameters inducing some difference in the various air-sea fluxes. An evaluation of the uncertainty sources and possible improvement for future generation of AORCMs highlights the importance of the parameterisation of the ocean albedo, rivers and cloud cover.  相似文献   

14.
The Pacific Atmospheric Sulfur Experiment (PASE) was a field mission that took place aboard the NCAR C-130 airborne laboratory over the equatorial Pacific Ocean near Christmas Island (Kirimati, Republic of Kiribati) during August?CSeptember, 2007. Eddy covariance measurements of the ozone fluxes at various altitudes above the ocean surface, along with simultaneous mapping of the horizontal gradients provided a unique opportunity to observe all of the dynamical components of the ozone budget in this remote marine environment. The results of six daytime and two sunrise flights indicate that vertical transport into the marine boundary layer from above and horizontal advection by the tradewinds are both important source terms, while photochemical destruction consisting of 82% photolysis (leading to OH production), 11% reaction with HO2, and 7% reaction with OH provides the main sink. The overall photochemical lifetime of ozone in the marine boundary layer was found to be 6.5 days. Ocean uptake of ozone was observed to be fairly slow (mean deposition velocity of 0.024?±?0.014 cm s?1) accounting for a diurnally averaged loss rate that was ??30% as large as the net photochemical destruction. From the measurement of deposition velocity an ozone reactivity of ??50 s?1 in seawater is inferred. Due to the unprecedented measurement accuracy of the dynamical budget terms, unobserved photochemistry was able to be deduced, leading to the conclusion that 3.9?±?3.0 ppt (parts per trillion by volume) of NO is present on average in the daytime tropical marine boundary layer, broadly consistent with several previous studies in similar environments. It is estimated, however, that each ppt of BrO hypothetically present would counter each ppt of NO above the requisite 3.9 ppt needed for budget closure. The long-term budget of ozone is further analyzed in the buffer layer, between the boundary layer and free troposphere, and used to derive an entrainment velocity across the trade wind inversion of 0.51 ± 0.38 cm s?1.  相似文献   

15.
Ozone measurements, performed since 1987, at the Swedish TOR/EUROTRACstation Åreskutan (lat. 63.4° N, long. 13.1° E, 1250 m abovesea level) are analyzed. The annual average ozone concentration at the sitehas increased by about 0.4 ppbv (1%) per year during the period1987–1994. The corresponding trends for individual months show adecrease during April–September and an increase during the rest of theyear. The ozone budget at Åreskutan has been investigated using backtrajectories of the air parcels, and the cosmogenic radionuclide7Be as a tracer of stratospheric air. From a simple diagnosticmodel, it is estimated that the contribution of stratospheric ozone to theconcentrations measured at Åreskutan is 5 ppbv (or 14% of themeasured values) on average, reaching a maximum of 23 ppbv (50%),during the episodes of direct stratospheric influence. In spring, thestratospheric contribution to ozone budget at Åreskutan is at itsmaximum, and approximately equal to the net photochemical ozone productionin the air mass affecting the site, whereas in winter, it is compensated byozone chemical sink during the transport of air masses from pollutedEuropean regions, to Scandinavia.  相似文献   

16.
A procedure for the dynamic initialization of wind and temperature fields within the atmospheric boundary layer (ABL) is presented. The procedure uses transilient turbulence theory to assess the turbulent fluxes from observed wind and temperature data, which are used to estimate the eddy transfer coefficients, so enabling a local closure ABL model to be integrated forward in time to a new steady state. The method has been applied to initialize kytoon data taken at Kharagpur (22.3° N, 87.2° E) during the MONTBLEX field programme. Results of a case study for 17 June 1990 are discussed.  相似文献   

17.
Local ozone production and loss rates for the arctic free troposphere (58–85° N, 1–6 km, February–May) during the TroposphericOzone Production about the Spring Equinox (TOPSE) campaign were calculated using a constrained photochemical box model. Estimates were made to assess the importance of local photochemical ozone production relative to transport in accounting for the springtime maximum in arctic free tropospheric ozone. Ozone production and loss rates from our diel steady-state box model constrained by median observations were first compared to two point box models, one run to instantaneous steady-state and the other run to diel steady-state. A consistent picture of local ozone photochemistry was derived by all three box models suggesting that differences between the approaches were not critical. Our model-derived ozone production rates increased by a factor of 28 in the 1–3 km layer and a factor of 7 in the 3–6 kmlayer between February and May. The arctic ozone budget required net import of ozone into the arctic free troposphere throughout the campaign; however, the transport term exceeded the photochemical production only in the lower free troposphere (1–3 km) between February and March. Gross ozone production rates were calculated to increase linearly with NOx mixing ratiosup to 300 pptv in February and for NOx mixing ratios up to 500 pptv in May. These NOx limits are an order of magnitude higher thanmedian NOx levels observed, illustrating the strong dependence ofgross ozone production rates on NOx mixing ratios for the majority of theobservations. The threshold NOx mixing ratio needed for netpositive ozone production was also calculated to increase from NOx 10pptv in February to 25 pptv in May, suggesting that the NOx levels needed to sustain net ozone production are lower in winter than spring. This lower NOx threshold explains how wintertime photochemical ozone production can impact the build-up of ozone over winter and early spring. There is also an altitude dependence as the threshold NOx neededto produce net ozone shifts to higher values at lower altitudes. This partly explains the calculation of net ozone destruction for the 1–3 km layerand net ozone production for the 3–6 km layer throughout the campaign.  相似文献   

18.
斯堪的纳维亚臭氧亏损和地面加热   总被引：3，自引：3，他引：0  
研究表明,冬季在北极的斯堪的纳维亚地区存在一个明显的臭氧亏损区,亏损区的中心值达-50DU.对臭氧亏损和地面加热进行相关分析后指出:斯堪的纳维亚地区的臭氧亏损和该地区地面的感热通量、潜热通量、净辐射通量以及总的热通量关系极其密切,其相关系数均在-0.87以上.由此,我们认为冬季斯堪的纳维亚地区的臭氧亏损可能是由于地面加热引发的物质抬升所造成的.  相似文献   

19.
NO, NOx, NOy and O3 have been measuredduring the airborne EXPRESSO experiment, November 96,which took place near Bangui (Central Africa) at thebeginning of the dry season. This period correspondsto an intense burning activity. Chemical andphotochemical characteristics of the planetaryboundary layer, which corresponds most of the time tothe monsoon layer, and the Harmattan layer, which issituated above the latter, have been studied forsavanna as well as rain forest areas. These two layersare very different when considering the chemicalcomposition (especially for ozone and NOz) andthe photochemical age.The relationship of photochemical ozone productionversus photochemical NOx oxidation products hasbeen investigated. Results indicate an ozoneproduction efficiency (OPE) ranging from 6.3 to 14.8in the planetary boundary layer. Thus, this layer ischaracteristic of a photochemically young and activeair mass. In this layer, the ozone potentialproduction increases with the air mass photochemicalage. On the other hand, the Harmattan layer shows anOPE ranging from 4.6 to 7.4. These values arecharacteristic of photochemically well-aged airmasses. In this layer, the ozone potential productionseems to be exhausted with values around 4.0 (i.e., 4ozone molecules produced for each NOx moleculeemitted).  相似文献   

20.
During the POPCORN campaign between 3 and 24 August 1994 we measured peroxyacetyl nitrate (PAN) in a rural area of Mecklenburg-Vorpommern (North-Eastern Germany) above a corn field. A total of about 5000 PAN measurements were carried out within the three weeks of the campaign. Measured PAN mixing ratios ranged from below the detection limit of 10 ppt up to an afternoon maximum of 1 ppb. The mean value of all data was 140 ppt. The daily mean PAN mixing ratios were typically in the range of 50 to 250 ppt, but during a clean air episode PAN mixing ratios of well below 40 ppt were observed. The characteristic relative diurnal variation of the PAN mixing ratios with a late night/early morning minimum and an afternoon maximum persisted during these episodes. The daily averages of the PAN mixing ratios showed clear episodic variations which coincided with the duration of typical synoptic episodes of two to six days duration. Based on the measurements of the various parameters determining the PAN formation and destruction rates, the local budget for PAN was calculated. During daytime the calculated net photochemical formation rate of PAN was nearly always significantly higher than the observed change of the PAN concentration. This demonstrates that substantial amounts of PAN (often in the range of several hundred ppt/h) were exported from the corn field. The resulting removal of NOx to some extent effects the budget of nitrogen oxides (NOx), but the export of odd oxygen radicals in the form of PAN during daytime often amounted up to 30–50% of the OH-radical formation by ozone photolysis. Thus the importance of PAN as reservoir and transport medium for odd oxygen radicals can be very substantial and may have a significant impact on the budget and distribution of odd oxygen radicals.  相似文献   

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