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2.
Ozone tendencies due to chemistry and transport are calculated by a mesoscale model using a fine horizontal resolution (3 km × 3 km), over South-Eastern France. Over that region where the anthropogenic emissions are very strong, ozone pollution is highlighted during two intensive observations periods of the ESCOMPTE campaign, when the sea breeze penetrates far into the Durance and Rhone valleys and the up-slope breezes are developed. From a fine analysis of time series of ozone concentration at different ground stations along these valleys and from numerical results, it is possible to discriminate the tendency due to chemistry from the tendency due to dynamical processes. We can distinguish both processes, either local chemical production/loss or dynamical increase/decrease (transport, deposition) on maps of ozone budget according to the meteorological conditions. In particular, we show that the variations due to transport can be have the same order of magnitude than those due to chemistry, reaching 20 ppbv h−1, whereas those due to chemistry are around 30 ppbv h−1.  相似文献   

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4.
In this paper, the “Expérience sur Site pour COntraindre les Modèles de Pollution atmosphérique et de Transport d'Emissions” (ESCOMPTE) program is presented. The ESCOMPTE program is used to produce a relevant set of data for testing and evaluating regional pollution models. It includes high-resolution (in space and time) atmospheric emission inventories and field experiments, and covers an area of 120×120 km, centered over the Marseilles-Berre area in the southeast of France during Summer 2001. This region presents a high occurrence of photochemical pollution events, which result from numerous industrial and urban sources of primary pollutants. From the dynamical characteristics of the area, sea-breeze circulation and channeling effects due to terrain features highly influence the location of the pollutant plumes. ESCOMPTE will provide a highly documented framework for dynamics and chemistry studies.Campaign strategies and experimental set up are described. During the planning phase, existing modeling results helped defining the experimental design. The campaign involved surface measurement networks, remote sensing, ship-borne, balloon-borne, and airplane measurements. Mean standard meteorological parameters and turbulent fluxes, ozone, ozone precursors, photochemically active trace gases, and aerosols were measured. Five intensive observation periods (IOPs) were documented using a wide spectrum of instruments, involving aircraft (7) (one of them equipped with a Doppler lidar, the others for in situ meteorological and chemical measurements), constant volume balloons (33), ozone lidars (5), wind profilers (15 sodars and radars), Doppler scanning lidar (1), radiosonde systems (at 4 locations), instrumented ships (2). In addition to the air quality networks from environmental agencies, 15 supplementary ground stations equipped for chemistry and/or meteorology and/or surface flux measurements, were operational. All instruments were calibrated and compared during a Quality Control/Quality Assurance (QC/QA) week, at the very beginning of the campaign.Fifteen days were intensively documented during five IOPs, referenced as 1, 2a, 2b, 3, and 4. High pollution levels were encountered during sea-breeze conditions observed during IOPs 2b and 3, whereas IOPs 2a and 4 corresponded to moderate wind, and channeled plume regimes. In addition, hourly emissions inventories for all IOPs were established to complete data sets and to finalize the ESCOMPTE database (EDB).Two other projects were associated to ESCOMPTE: urban boundary layer (UBL) and tropospheric water vapor content by GPS tomography (GPS/H2O). They took advantage of the scientific environment provided by ESCOMPTE.  相似文献   

5.
The new MOdèle de Chimie Atmosphérique à Grande Echelle (MOCAGE) three-dimensional multiscale chemistry and transport model (CTM) has been applied to study heavy pollution episodes observed during the ESCOMPTE experiment. The model considers the troposphere and lower stratosphere, and allows the possibility of zooming from the planetary scale down to the regional scale over limited area subdomains. Like this, it generates its own time-dependent chemical boundary conditions in the vertical and in the horizontal. This paper focuses on the evaluation and quantification of uncertainties related to chemical and transport modelling during two intensive observing periods, IOP2 and IOP4 (June 20–26 and July 10–14, 2001, respectively). Simulations are compared to the database of four-dimensional observations, which includes ground-based sites and aircraft measurements, radiosoundings, and quasi-continuous measurements of ozone by LIDARs. Thereby, the observed and modelled day-to-day variabilities in air composition both at the surface and in the vertical have been assessed. Then, three sensitivity studies are conducted concerning boundary conditions, accuracy of the emission dataset, and representation of chemistry. Firstly, to go further in the analysis of chemical boundary conditions, results from the standard grid nesting set-up and altered configurations, relying on climatologies, are compared. Along with other recent studies, this work advocates the systematic coupling of limited-area models with global CTMs, even for regional air quality studies or forecasts. Next, we evaluate the benefits of using the detailed high-resolution emissions inventory of ESCOMPTE: improvements are noticeable both on ozone reactivity and on the concentrations of various species of the ozone photochemical cycle especially primary ones. Finally, we provide some insights on the comparison of two simulations differing only by the parameterisation of chemistry and using two state-of-the-art chemical schemes for regional photochemical modelling. Regional air quality modelling is found to be highly sensitive to the emission inventory dataset and also to the vertical and horizontal boundary conditions and detailed representation of chemistry. Interestingly enough, they infer the same range of errors compared to total model errors.  相似文献   

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7.
A modified ceilometer has been used during the second Intensive Observation Period (IOP) of the “Expérience sur Site pour COntraindre les Modèles de Pollution atmosphériques et de Transport d'Émission” (ESCOMPTE) to perform continuous remote observations of aerosol accumulations in the first 3 km of the atmosphere. These observations encompassed an episode of intense particulate and photochemical pollution. The submicronic particles density, measured at an altitude of 600 m, went from a very low point of a few tens of particles per cubic centimeter (at the end of a Mistral episode in the free atmosphere) to a high point of more than 4500 particles per cubic centimeter (when pollutants were trapped by thermal inversions).The main result is that this instrument enables a fine documentation of the mixing layer height and of aerosol particles stratifications and circulation. Airborne aerosol measurements have been made above the mountainous region of Mérindol in order to validate in situ the remote sensing measurements. Ozone measurements near the summit of the mountains as well as in the valley were performed in order to correlate aerosol accumulation and ozone concentration. As a notable example, the two-layer aerosol stratification seen in the first 2 days of IOP 2b in that part of the ESCOMPTE domain confirms the results of another team which used backtrajectories. The low-altitude pollution for this timeframe had a local origin (the Fos industrial area), whereas above 500 m, the air masses had undergone regional-scale transport (from north-eastern Spain).The second major result is the highlighting of a pattern, in sea breeze conditions and in this part of the ESCOMPTE experiment zone, of nocturnal aerosol accumulation at an altitude of between 500 and 2000 m, followed by high ozone concentration the next day.  相似文献   

8.
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   

9.
The variability of Antarctic total column ozone in 1980–2018 is considered. The study analyzes trends in Antarctic total column ozone during the study period as well as the physical and chemical processes affecting the seasonal variability of total column ozone. The main attention is paid to the influence of dynamical processes on the stability of the Antarctic polar vortex, to the formation of polar stratospheric clouds, and to the influence of gas-phase and heterogeneous processes on the surface of polar stratospheric clouds and sulfate aerosol. The method of research is the analysis of the results of ground and satellite observations and numerical modeling of physical and chemical processes over the Antarctic using a global chemistry transport model with the dynamical parameters specified from reanalysis data.  相似文献   

10.
Volatile organic compounds (VOCs) emissions by vegetation present in the Mediterranean area are not well known. They may contribute with anthropogenic VOC emissions to the tropospheric ozone formation that reaches important level in the European Mediterranean region. The present work, carried out as part of the European ESCOMPTE project «fiEld experimentS to COnstrain Models of atmospheric Pollution and Transport of Emissions», adds a new contribution to the inventory of the main natural hydrocarbons sources likely to participate in the ozone production. The corresponding measurement campaign was conducted in La Barben, a site close to Marseilles (France), with the aim to quantify the terpenic emission pattern and the behaviour of Pinus halepensis, an important Mediterranean species slightly studied.The determination of biogenic emissions from P. halepensis was done by the enclosure of an intact branch in a Teflon cuvette. Main emitted monoterpenes were β trans-ocimene and linalool. The total monoterpenic emission rates thus recorded were found to reach maximum values around 30 μg gdry weight−1 h−1. The normalized emission rates calculated at 30 °C and 1000 μmol m−2 s−1 with Guenther's algorithm was 14.76, 8.65 and 4.05 μg gdry weight−1 h−1, respectively, for the total monoterpenes, β trans-ocimene and linalool.  相似文献   

11.
During the summer (8 June through 3 September) of 2008, 9 ozone profiles are examined from Dakar, Senegal (14.75°N, 17.49°W) to investigate ozone (O3) variability in the lower/middle troposphere during the pre-monsoon and monsoon periods. Results during June 2008 (pre-monsoon period) show a reduction in O3 concentrations, especially in the 850–700 hPa layer with Saharan Air Layer (SAL) events. However, O3 concentrations are increased in the 950–900 hPa layer where the peak of the inversion is found and presumably the highest dust concentrations. We also use the WRF-CHEM model to gain greater insights for observations of reduced O3 concentrations during the monsoon periods. In the transition period between 26 June and 2 July in the lower troposphere (925–600 hPa), a significant increase in O3 concentrations (10–20 ppb) occur which we suggest is caused by enhanced biogenic NOX emissions from Sahelian soils following rain events on 28 June and 1 July. The results suggest that during the pre-monsoon period ozone concentrations in the lower troposphere are controlled by the SAL, reducing ozone concentrations through heterogeneous chemical processes. At the base of the SAL we also find elevated levels of ozone, which we attribute to biogenic sources of NOX from Saharan dust that are released in the presence of moist conditions. Once the monsoon period commences, lower ozone concentrations are observed and modeled which we attribute to the dry deposition of ozone and episodes of ozone poor air that is horizontally transported into the Sahel from low latitudes by African Easterly Waves (AEWs).  相似文献   

12.
Ozone episodes (> 100 ppbv) were observed frequently in Jinan, an urban site located between the highly polluted Yangtze Delta and Beijing–Tianjin region in East China. In this study, the ozone episodes observed in 2004 were analysed using the Hybrid Single-particle Lagrangian Integrated Trajectory (HYSPLIT) model and surface meteorological data, as well as Air Pollution Index (API). The meteorological conditions of episode days and non-episode days were compared and examined, and categorization of 6 groups of backward trajectories was performed. The results show that, most episodes were caused by local photochemical production (e.g., induced by sufficient sunshine duration and high temperature) and pollutant accumulation (e.g., induced by little rainfall and low wind speed), and transport of pollutants from the highly polluted regions could significantly influence the air quality at the site, especially from Yangtze Delta region. In addition, three typical ozone episodes were analysed using HYSPLIT model to infer any long-distance transport and surface meteorological data to infer the local ozone production potential. At last, the functions and inadequacies about the usage of HYSPLIT model combined with surface meteorological data for the analysis of photochemical pollution were discussed.  相似文献   

13.
The relationship between the emission of ozone precursors and the chemical production of tropospheric ozone(O3) in the Pearl River Delta Region(PRD) was studied using numerical simulation.The aim of this study was to examine the volatile organic compound(VOC)-or nitrogen oxide(NOx =NO+NO2)limited conditions at present and when surface temperature is increasing due to global warming,thus to make recommendations for future ozone abatement policies for the PRD region.The model used for this application is the U.S.Environmental Protection Agency’s(EPA’s) third-generation air-quality modeling system;it consists of the mesoscale meteorological model MM5 and the chemical transport model named Community Multi-scale Air Quality(CMAQ).A series of sensitivity tests were conducted to assess the influence of VOC and NOx variations on ozone production.Tropical cyclone was shown to be one of the important synoptic weather patterns leading to ozone pollution.The simulations were based on a tropicalcyclone-related episode that occurred during 14-16 September 2004.The results show that,in the future,the control strategy for emissions should be tightened.To reduce the current level of ozone to meet the Hong Kong Environmental Protection Department(EPD) air-quality objective(hourly average of 120 ppb),emphasis should be put on restricting the increase of NOx emissions.Furthermore,for a wide range of possible changes in precursor emissions,temperature increase will increase the ozone peak in the PRD region;the areas affected by photochemical smog are growing wider,but the locations of the ozone plume are rather invariant.  相似文献   

14.
Understanding the chemical links between ozone (O3) and its two main precursors, nitrogen oxides (NOx) and volatile organic compounds (VOC), is important for designing effective photochemical smog reduction strategies. This chemical relationship will determine which precursor (NOx or VOC) emission reduction will be more effective for decreasing the ozone formation. Under certain conditions, ozone levels decrease as a result of a reduction in NOx emissions but do not respond significantly to changes in VOC emissions (NOx-sensitive condition), while under other conditions ozone concentrations decrease in response to reductions in VOCs and may even increase when NOx emissions are reduced (VOC-sensitive conditions). Indicator species can be used to assess the sensitivity of ozone to changes in the emissions of its precursors. These indicators are species or species ratios involved in ozone photochemistry which reflect the primary chemical process through which the ozone was formed. In this work we use the MM5-CAMx model system to explore the behaviour of various indicator species during two meteorological situations featuring different atmospheric conditions in a complex terrain area. The results show that indicators based on nitrogen compounds (i.e,. NOy and NOz) are suitable for defining the transition range from VOC- to NOx-sensitive chemistry, and that despite the uncertainties associated with the use of chemical indicators, the ratios O3/NOy and O3/NOz may provide a simple and useful way to summarize the response of ozone to changes in NOx and VOC emissions in Southwestern Spain.  相似文献   

15.
The development of the future atmospheric chemical composition is investigated with respect to NO y and O3 by means of the off‐line coupled dynamic‐chemical general circulation model ECHAM3/CHEM. Two time slice experiments have been performed for the years 1992 and 2015, which include changes in sea surface temperatures, greenhouse gas concentrations, emissions of CFCs, NO x and other species, i.e., the 2015 simulation accounts for changes in chemically relevant emissions and for a climate change and its impact on air chemistry. The 2015 simulation clearly shows a global increase in ozone except for large areas of the lower stratosphere, where no significant changes or even decreases in the ozone concentration are found. For a better understanding of the importance of (A) emissions like NO x and CFCs, (B) future changes of air temperature and water vapour concentration, and (C) other dynamical parameters, like precipitation and changes in the circulation, diabatic circulation, stratosphere‐troposphere‐exchange, the simulation of the future atmosphere has been performed stepwise. This method requires a climate‐chemistry model without interactive coupling of chemical species. Model results show that the direct effect of emissions (A) plays a major rôle for the composition of the future atmosphere, but they also clearly show that climate change (B and C) has a significant impact and strongly reduces the NO y and ozone concentration in the lower stratosphere.  相似文献   

16.
We present a comprehensive discussion on what cause high ozone episodes at a suburban photochemical observation site of the Seoul Metropolitan Area (population ～23 million). The observational site, Taehwa Research Forest (TRF), is situated ～30 km from the center of Seoul. In June 2011, we observed two very distinctive ozone periods-high ozone (peak up to 120 ppbv) and low ozone (peak up to 60 ppbv) in the mid and early month, respectively. The trace gas measurement dataset, especially CO and NO X clearly indicate that less anthropogenic influences during the high ozone period. Volatile organic compound (VOC) measurement results show that at the observational site, biogenic VOCs (mostly isoprene) contribute most of chemical reactivity towards OH, although toluene from anthropogenic activities was observed in higher concentrations. Back-trajectory analysis indicates that air-masses from the forest part of Korea Peninsula were dominant influences during the high ozone episode event. On the other hand, Aged air masses from China were the dominant influence during the low ozone episode event. Model calculations conducted using the University of Washington Chemical Mechanism (UWCM) box model, also consistently show that BVOC, especially isoprene photochemistry, can be the significantly contribution to local ozone formation in the given photochemical environments of TRF. These research results strongly suggest that ozone control strategy in the Eastern Asian megacities, mostly situated in surrounding forest areas should be based on the comprehensive scientific understanding in BVOC photochemistry and interplays between anthropogenic and biogenic interactions.  相似文献   

17.
This work presents the temporal evolution and spatial distribution of nitrogen dioxide (NO2) measured with the help of passive diffusion tubes in different environments: rural, sub-urban, urban, at La Réunion Island in December 1997 and November 2000 (austral spring), respectively. NO2 concentration exhibits notable enhancement from 1997 to 2000. For instance, its mean concentration was 16 and 20 μg/m3 in December 1997 and November 2000, respectively, at La Réunion Island, especially in inhabited regions due to increase of local anthropogenic activities, mainly traffic circulation, in the absence of house heating and biomass burning. We also observe a net increase of pollutant levels by a factor two in rural/remote areas within 3 years, which is tied to the extension of inhabited areas and air-flows from enhanced local sources. The increase of atmospheric pollutants is mainly due to enhancement of anthropogenic activities (traffic) since the 1990s at La Réunion Island, which results from a constant increase of population and consequently, from a higher number of vehicles in circulation. Importantly, in cities like Saint-Denis, where traffic network has been subject to notable improvement (e.g. single to double lanes, etc.), pollutant levels exhibit little variability as in temperate continental latitudes. Semi-continuous NO2 concentration measured in parallel with ozone in November 2000 also showed that daytime photochemical ozone production is influenced by pollutant and precursor (NO2) levels at Saint-Denis, while nighttime ozone increase is mainly tied to dynamical processes. The November 2000 ozone diurnal pattern is notably different from that observed in September 1995, during which a daytime ozone loss was observed, pointing out that atmospheric conditions have been subject to notable changes, i.e., clean to moderately polluted, within a few years at La Réunion Island. The results presented here point out that the ‘source enhancement effect’ is superimposed on dynamical and photochemical processes to influence pollutants variability and hence atmospheric chemistry, in a quite ‘pristine’ tropical oceanic region.  相似文献   

18.
A Eulerian air pollution model for Europe with nonlinear chemistry   总被引：1，自引：0，他引：1  
A long-range transport model with nonlinear chemical reactions is described. The model contains 35 pollutants and 70 chemical reactions. This is a Eulerian model defined on a space domain containing the whole of Europe. The spherical space domain (corresponding to the Earth's surface covered by the model) is mapped into a square plane domain and discretized by using a 32×32 grid. The grid increments are equidistant (both along the Ox axis and along the Oy axis). The choice of values of the physical parameters involved in the model and the numerical treatment of the model are shortly discussed. The model is tested with meteorological data for 1985 and 1989. The numerical results are compared with measurements at stations located in different European countries. Extensive comparisons of ozone concentrations for July 1985 with measurements taken at 24 European stations are also carried out. Results concerning three episodes in July 1985 as well as results obtained in the study of the sensitivity of the ozone concentrations to variations of NO x and/or anthropogenic VOC emissions are presented. The advantages and the limitations of such a model are discussed. The model is continuously improved by adding new modules to it. The plans for improvements in the near future are outlined.  相似文献   

19.
北京奥运会期间CBM-Z化学机制的模拟应用   总被引：1，自引：0，他引：1  
利用CBM-Z化学机制模拟了中国科学院大气物理研究所气象塔站在北京奥运会期间高臭氧时段O3浓度的日变化,评估了气象条件、北京奥运会加强控制措施以及O3前体物浓度对近地面O3生成的影响。结果表明:(1)CBM-Z化学机制较好地模拟了北京奥运会期间典型时段气象塔站O3、NO、NO2日变化特征。(2)有利于局地高臭氧事件发生的气象条件非常相似;北京奥运会加强控制措施的实施显著减少了NOx及VOCs的排放量,导致近地面O3浓度的明显下降。(3)奥运会期间VOCs和CO是影响气象塔站O3生成量的关键因素。  相似文献   

20.
Three online coupled chemical transport model simulations were analyzed for three summer months of 2015 in Poland. One of them was run with default emission inventory, the other two with NOx and VOC emissions reduced by 30%, respectively. Obtained ozone concentrations were evaluated with data from air quality measurement stations and ozone sensitivity to precursor emissions was estimated by ozone concentration differences between simulations and with the use of indicator ratios. They were calculated based on modeled mixing ratios of ozone, total reactive nitrogen and its components, nitric acid and hydrogen peroxide. The results show that the model overestimates ozone concentrations with the largest errors in the morning and evening, which is primarily related to the way vertical mixing is resolved by the model. Better model performance for ozone is achieved in rural than urban environment, as PBL and mixing mechanisms play more significant role in urban areas. Modeled ozone shows mixed sensitivity to precursor concentrations, similarly to other European regions, but indicator ratios have different values than are found in literature, particularly H2O2/HNO3 is larger than in southern Europe. However, indicator ratios often differ between locations and transition values need to be established individually for a given region.  相似文献   

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