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1.
A photochemical box model has been used to simulate the mixing ratio ofozone under conditions reflecting those encountered in the marine boundarylayer at Cape Grim, Tasmania, where a decade-long record of ozone mixingratio is available. The model is based on the proposition that ozone loss byphotolysis, atmospheric reaction with hydroperoxy and hydroxyl radicals, andsurface deposition is balanced by ozone gain via entrainment from the lowerfree troposphere with a small additional source in summer from photolysis ofnitrogen dioxide. This model simulates very well the observed ozone records,reproducing both the small diurnal cycle in ozone mixing ratio observedduring the summer months, and the factor of two seasonal ozone cycle showinga distinct winter maximum and summer minimum. The model result confirms thatunder the low-NOx conditions of the clean marine boundarylayer net photochemical loss of ozone occurs at all times of year.  相似文献   

2.
Abstract

The dependence of ozone formation on the mixing ratios of volatile organic compounds (VOCs) and nitrogen oxides (NOx) has been widely studied. In addition to the atmospheric levels of VOCs and NOx, the extent of photochemical processing of VOCs has a strong impact on ozone levels. Although methods for measuring atmospheric mixing ratios of VOCs and NOx are well established and results of those measurements are widely available, determination of the extent of photochemical processing of VOCs, known as photochemical age (PCA), is difficult. In this article a recently developed methodology for the determination of PCA for individual compounds based on the change in their stable carbon isotope composition is used to investigate the dependence between ozone and VOC or NOx mixing ratios at a rural site in Ontario, Canada, during fall and winter. The results show that under these conditions the variability in VOC mixing ratios is predominantly a result of the varying impact of local emissions and not a result of changes in the extent of atmospheric processing. This explains why the mixing ratio of ozone shows no systematic dependence on the mixing ratios of VOCs or NOx in this environment and at this time of the year.  相似文献   

3.
A simulated study of mechanism for variations and distributions of ozone and its precursors was made by using the three-dimensional regional Eulerian model.The results showed that the ozone production was controlled by NOx,but there is a complicated nonlinear relation between them.The photochemical reactions controlled by solar radiation are the determinative factors affecting the variations of the surface ozone and its precursors.The relations of ozone and CO,PAN were studied.We compared the simulated and observed results during the PEM-WEST A in order to better understand the photochemical processes of ozone and its precursors.  相似文献   

4.
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   

5.
Ozone photochemical production and loss in very different environments at Waliguan baseline station and Lin'an background station were simulated by using the measurement data and photochemical box model.The results show that net ozone photochemical production rate is negative,about 0.5 ppb/d,at Waliguan baseline sation,because of very low precursor concentrations.But at Lin'an background station,the net photochemical ozone production is positive,about 2-3 ppb/h.which is very closed with the measurement at Lin'an.That means ozone production was controlled by photochemical reactions at Lin'an background station,because of the higher precursor concentrations.The net destruction rate,at Waliguan Mt.,is not large,so that future increase in anthropogenic emission of reactive nitrogen will lead to larger production rates of steady-state O3 concentration.  相似文献   

6.
利用2010—2012年对流层臭氧（O3）及其多种前体物的卫星遥感资料和全球水汽再分析资料,研究东亚区域O3及其前体物的时空分布,以及在中国东部（分为南、北两部分）相关性的季节变化。结果表明:东亚区域NO2与CO的对流层柱含量均表现为冬季高、夏季低的时空变化形式。O3对流层柱含量夏季达到峰值,冬季为谷值。中国东部的北部与南部地区O3与NO2均在夏秋季呈正相关,冬春季呈负相关。夏季大部分地区NOx的光化学循环反应对O3生成有积极的促进作用,冬季大部分地区O3的光化学循环生成受到抑制。O3与CO在北部地区夏秋季和南部地区夏季正相关性最大,无论是在北部还是南部地区,O3与CO的相关性在轻污染情况下最大,而在重污染和背景情况下较小,表明重污染气团向下风方的输送更有利于O3的光化学生成。O3与水汽在北部和南部地区的多数时间均呈较显著的正相关性,而在南部地区夏季和北部地区冬季具有较大的负相关性,反映出不同的环流形式、气团来源及伴随的天气条件变化对O3分布的影响。  相似文献   

7.
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8.
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   

9.
The effects of deep convection on the potential for forming ozone (ozone production potential) in the free troposphere have been simulated for regions where the trace gas composition is influenced by biomass burning. Cloud dynamical and photochemical simulations based on observations in 1980 and 1985 Brazilian campaigns form the basis of a sensitivity study of the ozone production potential under differing conditions. The photochemical fate of pollutants actually entrained in a cumulus event of August 1985 during NASA/GTE/ABLE 2A (Case 1) is compared to photochemical ozone production that could have occurred if the same storm had been located closer to regions of savanna burning (Case 2) and forest burning (Case 3). In each case studied, the ozone production potential is calculated for a 24-hour period following convective redistribution of ozone precursors and compared to ozone production in the absence of convection. In all cases there is considerably more ozone formed in the middle and upper troposphere when convection has redistributed NOx, hydrocarbons and CO compared to the case of no convection.In the August 1985 ABLE 2A event, entrainment of a layer polluted with biomass burning into a convective squall line changes the free tropospheric cloud outflow column (5–13 km) ozone production potential from net destruction to net production. If it is assumed that the same cloud dynamics occur directly over regions of savanna burning, ozone production rates in the middle and upper troposphere are much greater. Diurnally averaged ozone production following convection may reach 7 ppbv/day averaged over the layer from 5–13 km-compared to typical free tropospheric concentrations of 25–30 ppbv O3 during nonpolluted conditions in ABLE 2A. Convection over a forested region where isoprene as well as hydrocarbons from combustion can be transported into the free troposphere leads to yet higher amounts of ozone production.  相似文献   

10.
Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH4 and NO x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO x emissions during this period while the contribution of CH4 to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.  相似文献   

11.
A photochemical box model has been used to model themeasured diurnal ozone cycle in spring at Jungfraujochin the Swiss Alps. The comparison of the modelleddiurnal ozone cycle with the mean measured diurnalozone cycle in spring, over the period 1988–1996,shows a good agreement both with regard to the shapeand amplitude. Ozone concentrations increase duringthe daytime and reach a maximum at about 16:00–17:00(GMT) in both the modelled and the mean observed ozonecycle, indicative of net ozone production during thedaytime at Jungfraujoch in spring. The agreement isbetter when the modelled ozone cycle is compared withthe mean measured diurnal cycle (1988–1996) filteredfor north-westerly winds >5 m/s (representative ofregional background conditions at Jungfraujoch). Inaddition to ozone, the modelled diurnal cycle of[HO2] + [CH3O2] also shows rather goodagreement with the mean diurnal cycle of the peroxyradicals measured during FREETEX '96, a FREETropopsheric Experiment at Jungfraujoch in April/May1996. Furthermore, this mean diurnal cycle of the sumof the peroxy radicals measured during FREETEX '96 isused to calculate, using steady-state expressions, therespective diurnal cycle of the OH radical. Thecomparison of the OH diurnal cycle, calculated fromthe peroxy radical measurements during FREETEX '96,with the modelled one, reveals also good agreement.The net ozone production rate during the day-time is0.27 ppbv h-1 from the model, and 0.13 ppbvh-1 from the observations during FREETEX '96. Theobservations and model results both suggest that thediurnal ozone variation in spring at Jungfraujoch isprimarily of photochemical origin. Furthermore, theobserved and modelled positive net ozone productionrates imply that tropospheric in situphotochemistry contributes significantly to theobserved high spring ozone values in the observedbroad spring-summer ozone maximum at Jungfraujoch.  相似文献   

12.
The mixing ratios for ozone and NOx (NO+NO2) have been measured at a rural site in the United States. From the seasonal and diurnal trends in the ozone mixing ratio over a wide range of NOx levels, we have drawn certain conclusions concerning the ozone level expected at this site in the absence of local photochemical production of ozone associated with NOx from anthropogenic sources. In the summer (June 1 to September 1), the daily photochemical production of ozone is found to increase in a linear fashion with increasing NOx mixing ratio. For NOx mixing ratios less than 1 part per billion by volume (ppbv), the daily increase is found to be (17±3) [NOx]. In contrast, the winter data (December 1 to March 1) indicate no significant increase in the afternoon ozone level, suggesting that the photochemical production of ozone during the day in winter approximately balances the chemical titration of ozone by NO and other pollutants in the air. The extrapolated intercept corresponding to [NOx]=0 taken from the summer afternoon data is 13% less than that observed from the summer morning data, suggesting a daytime removal mechanism for O3 in summer that is attributed to the effects of both chemistry and surface deposition. No significant difference is observed in the intercepts inferred from the morning and afternoon data taken during the winter.The results contained herein are used to deduce the background ozone level at the measurement site as a function of season. This background is equated with the natural ozone background during winter. However, the summer data suggest that the background ozone level at our site is elevated relative to expected natural ozone levels during the summer even at low NOx levels. Finally, the monthly daytime ozone mixing ratios are reported for 0[NOx]0.2 ppbv, 0.3 ppbv[NOx]0.7 ppbv and 1 ppbv[NOx]. These monthly ozone averages reflect the seasonal ozone dependence on the NOx level.  相似文献   

13.
A one-year set of surface ozone measurements in a four-station network located in the Venezuelan savannah is reported. The diurnal ozone variation is typical of continental stations with a maximum in the afternoon, when vertical turbulent mixing is strongest. The annual O3 average concentration, based on the monthly averages of daily maxima, was 17±2 ppb, which is in good agreement with values reported for similar latitudes. The boundary-layer ozone levels did not fall below 8 ppb, in contrast with previous sporadic measurements made in tropical latitudes. No evidence was found that mesoscale O3 downdrafts in the ITCZ in the South American continent are an important source of surface ozone. Finally, it is suggested that the relatively high ozone levels observed at the end of the dry season are probably of photochemical origin.  相似文献   

14.
Measurements of the sum of peroxy radicals [HO2 + RO2],NOx (NO + NO2) and NOy (the sum of oxidisednitrogen species) made at Mace Head, on the Atlantic coast of Ireland in summer 1996 and spring 1997 are presented. Together with a suite of ancillary measurements, including the photolysis frequencies of O3 O(1D)(j(O1D)) and NO2 (j(NO2)), the measured peroxy radicals are used to calculate meandailyozone tendency (defined as the difference of the in-situphotochemical ozone production and loss rates); these values are compared with values derived from the photochemical stationary state (PSS) expression. Although the correlation between the two sets of values is good, the PSS values are found to be significantly larger than those derived from the peroxy radical measurements, on average, in line with previous published work. Possible sources of error in these calculations are discussed in detail. The data are further divided up into five wind sectors, according to the instantaneous wind direction measured at the research station. Calculation of mean ozone tendencies by wind sector shows that ozone productivity was higher during spring (April–May) 1997 than during summer (July–August) 1996across all airmasses, suggesting that tropospheric photochemistry plays an important role in the widely-reported spring ozone maximum in the Northern Hemisphere. Ozone tendencies were close to zero for the relatively unpolluted south-west, west and north-west wind sectors in the summer campaign, whereas ozone productivity was greatest in the polluted south-east sector for both campaigns. Daytime weighted average ozone tendencies were +(0.3± 0.1) ppbv h–1 for summer 1996 and +(1.0± 0.5) ppbvh–1 for spring 1997. These figures reflect the higher mixing ratios of ozone precursors in spring overall, as well as the higher proportion of polluted air masses from the south-east arriving at the site during the spring campaign. The ozone compensation point, where photochemical ozone destruction and production processes are in balance, is calculated to be ca. 14 pptv NO for both campaigns.  相似文献   

15.
One-dimensional photochemical diffusion model which includes oxygen-hydrogen-sodium atmosphere has been used to examine the relation between sodium and hydroxyl nightglow and the role of ozone in it. It is found that both emissions can be obtained on the basis of photochemistry. The following reactionsNa + O3→NaO + O2 and H + O3 → OH* + O2 play key role in sodium and hydroxyl emission respectively. Further it is found that variations in both emissions are controlled by the variation in the concentration of ozone.  相似文献   

16.
Abstract

A coupled 1‐D radiative‐convective and photochemical diffusion model is used to study the influence of ozone photochemistry on changes in the vertical temperature structure and surface climate resulting from the doubling of atmospheric CO2, N2O, CH4 and increased stratospheric aerosols owing to the El Chichón volcanic eruption. It is found when CO2 alone is doubled, that the total ozone column increases by nearly 6% and the resulting increase in the solar heating contributes a smaller temperature decrease in the stratosphere (up to 4 K near the stratopause level). When the concentration of CO2, N2O and CH4 are simultaneously doubled, the total ozone column amount increases by only 2.5% resulting in a reduced temperature recovery in the stratosphere. Additional results concerning the effect of the interaction of ozone photochemistry with the stratospheric aerosol cloud produced by the El Chichón eruption show that it leads to a reduction in stratospheric ozone, which in turn has the effect of increasing the cooling at the surface and above the cloud centre while causing a slight warming below in the lower stratosphere.  相似文献   

17.
By means of a three-dimensional meteorological model (MM5) and a chemical model,the distributions of tropospheric ozone and its precursors over China have been simulated in summer and winter time,16-18 August 1994 and 7-9 January 1995.The distribution of ozone over the Tibetan Plateau in summer time is deeply discussed.The simulated results indicate that thedistributions of surface ozone and NOx are in good agreement with observed results,and human activities and photochemical reactions are the main factors controlling the surface ozone and NOx concentrations.In addition,higher ozone concentrations are coincided with the air convergence,and the lower concentrations are related to the air divergence.In summer,over the Tibetan Plateau the strong flow convergence results in higher ozone concentrations in the lower troposphere:and the strong flow divergence results in lower ozone concentrations in the upper troposphere.In winter time ozone concentrations show large-scale characteristics controlled by westerly flow,and in the jet area they are lower than those outside the jet.  相似文献   

18.
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   

19.
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   

20.
In the present study, an attempt has been made to examine the governing photochemical processes of surface ozone (O3) formation in rural site. For this purpose, measurements of surface ozone and selected meteorological parameters have been made at Anantapur (14.62°N, 77.65°E, 331 m asl), a semi-arid zone in India from January 2002 to December 2003. The annual average diurnal variation of O3 shows maximum concentration 46 ppbv at noon and minimum 25 ppbv in the morning with 1σ standard deviation. The average seasonal variation of ozone mixing ratios are observed to be maximum (about 60 ppbv) during summer and minimum (about 22 ppbv) in the monsoon period. The monthly daytime and nighttime average surface ozone concentration shows a maximum (55 ± 7 ppbv; 37 ± 7.3 ppbv) in March and minimum (28 ± 3.4 ppbv; 22 ± 2.3 ppbv) in August during the study period. The monthly average high (low) O3 48.9 ± 7.7 ppbv (26.2 ± 3.5 ppbv) observed at noon in March (August) is due to the possible increase in precursor gas concentration by anthropogenic activity and the influence of meteorological parameters. The rate of increase of surface ozone is high (1.52 ppbv/h) in March and lower (0.40 ppbv/h) in July. The average rate of increase of O3 from midnight to midday is 1 ppbv/h. Surface temperature is highest (43–44°C) during March and April months leading to higher photochemical production. On the other hand, relative humidity, which is higher during the rainy season, shows negative correlation with temperature and ozone mixing ratio. It can be seen that among the two parameters are measured, correlation of surface ozone with wind speed is better (R 2=0.84) in compare with relative humidity (R 2=0.66).  相似文献   

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