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1.
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   

2.
漠河地区臭氧的观测和计算   总被引：2，自引：0，他引：2  
1997年3月上旬,在黑龙江漠河地区对地面和整层臭氧、太阳辐射等进行了短期观测,以初步了解该地区臭氧和辐射的变化规律以及它们之间的相互关系.研究发现,漠河地区近地面臭氧日变化明显,其峰值出现在每日10:00(北京时间)左右,并早于紫外辐射(UV)峰值出现时间.整层大气臭氧总量的日变化特征不明显.基于UV能量守恒,建立了臭氧与其影响因子-光化学、散射、UV等因子之间较好的定量关系和经验模式,并将其用于计算地面、整层大气臭氧小时值和日平均值.结果表明,计算值与观测值吻合的都比较好,它们相对偏差的平均值分别为:地面臭氧小时值(11.9%)和日平均值(9.0%);整层大气臭氧小时值和日平均值-7.4%、1.8%.因此,地面和整层臭氧的经验算法是合理和可行的.利用散射辐射/直接辐射(D/S)和散射辐射/总辐射(D/Q)可以描述大气中的物质如气溶胶、云等的散射作用.采用D/Q表示散射作用可以提高地面臭氧和整层大气臭氧计算的准确度,特别是对云量较大的情况.    相似文献   

3.
The seasonal and diurnal variations of ozone mixing ratios have been observed at Niwot Ridge. Colorado. The ozone mixing ratios have been correlated with the NO x (NO+NO2) mixing ratios measured concurrently at the site. The seasonal and diurnal variations in O3 can be reasonably well understood by considering photochemistry and transport. In the winter there is no apparent systematic diurnal variation in the O3 mixing ratio because there is little diurnal change of transport and a slow photochemistry. In the summer, the O3 levels at the site are suppressed at night due to the presence of a nocturnal inversion layer that isolated ozone near the surface, where it is destroyed. Ozone is observed to increase in the summer during the day. The increases in ozone correlate with increasing NO x levels, as well as with the levels of other compounds of anthropogenic origin. We interpret this correlation as in-situ or in-transit photochemical production of ozone from these precursors that are transported to our site. The levels of ozone recorded approach 100 ppbv at NO x mixing ratios of approximately 3 ppbv. Calculations made using a simple clean tropospheric chemical model are consistent with the NO x -related trend observed for the daytime ozone mixing ratio. However, the chemistry, which does not include nonmethane hydrocarbon photochemistry, underestimates the observed O3 production.  相似文献   

4.
The Pic 2005 field campaign took place from 13 June to 7 July 2005 close to the high-altitude permanent atmospheric observatory Pic-du-Midi (PDM), situated at 2875 m asl in the French Pyrenees. The experimental set-up combined in situ ground-based observations at PDM with ozone lidar measurements at two lower sites in close vicinity (600 m asl/28 km away, and 2380 m asl/500 m away). Such an experimental configuration is appropriate to address the question of the vertical layering of the chemical atmosphere in a mountain area and above the plain nearby, and how this influences measurements conducted on a mountain summit under the influence of horizontal transport at regional scale, and vertical transport at local scale. Forecast tools made it possible to plan and carry out 6 one-day Intensive Observation Periods (IOPs), mostly in anticyclonic conditions favoring local thermally induced circulations, with and without local pollution in the lower troposphere.It was thus possible to document i) ozone diurnal variations at PDM; ii) correlation between ozone measurements at PDM and their counterparts at the same altitude in the free troposphere; iii) ozone variability in the vicinity of PDM.The field campaign provided direct experimental evidence that at daytime in the encountered conditions (mostly anticyclonic), PDM failed in a large extent to be representative of the troposphere above the surrounding flat areas at similar altitude. First, ozone daily averages at PDM were found lower than their free-tropospheric counterpart. Thermally induced circulations and convection pumping clean air from the rural boundary layer can account qualitatively for ozone depletion observed at PDM during daytime. However the surface measurements do not support the hypothesis of direct lifting of near-surface air masses up to PDM. Thus, mixing with free-tropospheric air, photochemistry and surface deposition in the valleys appear to be needed ingredients to account quantitatively for the observed variations (in proportions that further studies should determine). Second, ozone variability was found to be much lower at PDM than in the free troposphere—again an indication of atmospheric mixing. In particular at daytime, the PDM observatory did not allow for detection of ozone-rich layers simultaneously visible above the plain. Beyond these first results, the data set presented here paves way to detailed studies of the IOPs.  相似文献   

5.
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   

6.
The summertime ozone valley over the Tibetan Plateau is formed by two influences,the Asian summer monsoon(ASM) and air column variations.Total ozone over the Tibetan Plateau in summer was ～33 Dobson units(DU) lower than zonal mean values over the ocean at the same latitudes during the study period 2005-2009.Satellite observations of ozone profiles show that ozone concentrations over the ASM region have lower values in the upper troposphere and lower stratosphere(UTLS) than over the non-ASM region.This is caused by frequent convective transport of low-ozone air from the lower troposphere to the UTLS region combined with trapping by the South Asian High.This offset contributes to a ～20-DU deficit in the ozone column over the ASM region.In addition,along the same latitude,total ozone changes identically with variations of the terrain height,showing a high correlation with terrain heights over the ASM region,which includes both the Tibetan and Iranian plateaus.This is confirmed by the fact that the Tibetan and Iranian plateaus have very similar vertical distributions of ozone in the UTLS,but they have different terrain heights and different total-column ozone levels.These two factors(lower UTLS ozone and higher terrain height) imply 40 DU in the lower-ozone column,but the Tibetan Plateau ozone column is only ～33 DU lower than that over the non-ASM region.This fact suggests that the lower troposphere has higher ozone concentrations over the ASM region than elsewhere at the same latitude,contributing ～7 DU of total ozone,which is consistent with ozonesonde and satellite observations.  相似文献   

7.
通过对广州鼎湖山近地面O3、NOx、太阳辐射,气象参数等项目的观测和理论分析,研究了地面O3与NOx等微量气体及太阳可见光辐射的变化规律,详细讨论了可见光波段、不同天气条件地面O3与NOx、光化学反应、气溶胶、可见光辐射等之间复杂的关系.提出以光能量传输与守恒的观点来考虑大气中与可见光辐射有关的主要过程,并以此来研究大气光化学过程中所遵循的能量规律,建立了一个简单、实用、省时的统计模式,用于计算地面O3浓度.结果表明:不同情况下,计算值与观测值吻合得均比较一致.  相似文献   

8.
地面臭氧的变化规律和计算方法的初步研究Ⅰ.紫外波段   总被引：5，自引：1，他引：4  
通过对广州鼎湖山近地面O3、NOx、太阳辐射、气象参数等项目的观测和理论分析,研究了地面O3与NOx等微量气体及太阳辐射的变化规律,详细讨论了紫外波段、不同天气条件地面O3与NOx,光化学反应、气溶胶、光化辐射等之间复杂的关系.用光能量传输与守恒的观点来考虑大气中与紫外辐射有关的主要过程,并以此来研究大气光化学过程中所遵循的能量规律,建立了一个简单、实用、省时的统计模式,用于计算地面O3浓度.结果表明,不同情况下计算值与观测值均吻合较好.  相似文献   

9.
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   

10.
地面臭氧光化学过程规律的初步研究   总被引：8，自引：2，他引：6  
给出了1996年夏季在广东肇庆鼎湖山对光化辐射、地面O3、NO、NO2浓度的观测结果,对影响地面O3、NO、NO2的主要因子进行了分析。晴天,地面O3、NO、NO2浓度有明显的日变化;阴天,它们的日变化比较复杂。晴天和阴天,在lnQUVB/m和lnQvis/m(其中QUVB为紫外B辐射,Qvis为可见光辐射,m为大气质量)与地面O3、NO,NO2浓度、整层大气水汽含量(q1、q2、q3、q4)之间存在着很好的相关关系。利用得到的关系式计算了地面O3浓度,在紫外和可见光波段,计算值与观测值符合得都比较好。  相似文献   

11.
By using the 2-D stratospheric-tropospheric dynamic-radiative-chemical coupled model,somesensitivity experiments have been done,which are interactions among ozone,radiation andtemperature,vapor effects,as well as effects of source and sink.The result of temperatureexperiment shows that feedback interaction among ozone,radiation and temperature,mainlyoccurs in the upper and middle stratosphere,the maximum of ozone concentration decrease is 1ppm,the maximum of temperature change is 6 K,and the maximum of total ozone change is 20DU.From the experiment of water vapor,we can see that the area of the middle and high latitudesof the Northern Hemisphere is sensitive to vapor change.When the maximum difference betweenboth surface sources is in the Antarctic,the maximum of ozone change is also there.Because thecharacter of surface varies with latitude,dry deposition is different in different latitudes.Thechange of dry deposition makes ozone in boundary layer quite obvious,especially in both poles.The maximum change of total volume ozone in experiments of vapor,source and sink is more than12 DU.  相似文献   

12.
By using the 2-D stratospheric-tropospheric dynamic-radiative-chemical coupled model,some sensitivity experiments have been done,which are interactions among ozone,radiation and temperature,vapor effects,as well as effects of source and sink.The result of temperature experiment shows that feedback interaction among ozone,radiation and temperature,mainly occurs in the upper and middle stratosphere,the maximum of ozone concentration decrease is 1ppm,the maximum of temperature change is 6 K,and the maximum of total ozone change is 20 DU.From the experiment of water vapor,we can see that the area of the middle and high latitudes of the Northern Hemisphere is sensitive to vapor change.When the maximum difference between both surface sources is in the Antarctic,the maximum of ozone change is also there.Because the character of surface varies with latitude,dry deposition is different in different latitudes.The change of dry deposition makes ozone in boundary layer quite obvious,especially in both poles.The maximum change of total volume ozone in experiments of vapor,source and sink is more than 12 DU.  相似文献   

13.
鼎湖山森林地区臭氧及其前体物的变化特征和分析   总被引：18，自引：2，他引：16  
通过对鼎湖山森林地区近地面O3和NOx浓度、太阳辐射、气象参数等为期一年的观测和资料分析,给出了地面O3和NOx浓度、太阳辐射的变化规律及其相互之间的关系.地面O3、NOx、CO、SO2浓度以及紫外辐射、太阳总辐射等有明显的日变化和季节变化.不同因子对O3的敏感性试验结果表明,晴天和实际天气,O3浓度对NO、NO2浓度的变化最为敏感,其次是水汽、气溶胶,最后是紫外辐射.所有因子的变化均引起O3在湿季比干季更大的变化率,因此在研究臭氧化学和光化学时,应该考虑水汽以及OH自由基的重要作用.对于晴天和实际天气的逐时值和日平均值而言,O3浓度与NO2/NO之间存在很好的正相关关系,比值NO2/NO可以作为判断O3峰值出现的一个指标.O3极值的出现既受NO和NOx影响,也受气象因素(温湿度、云、风、雾、降雨)和辐射的影响.周末O3、NOx浓度及NO2/NO有规律的增大,表明实验地点的大气受到人为污染源的影响.  相似文献   

14.
利用1979—2018年太阳后向散射紫外辐射计SBUV(/2)星下点臭氧遥感资料,结合ERA-Interim和MERRA-2大气温度再分析资料,考察青藏高原区域内拉萨和共和两地春季臭氧和大气温度变化趋势的差异性。结果表明拉萨和共和两个地区的臭氧和大气温度逆转趋势均发生于1999年。对比2008年以来青藏高原整体臭氧总量变化速率（4.5 DU/(10 a)),拉萨臭氧总量变化更快,为5.9 DU/(10 a),共和相对较慢,仅为3.7 DU/(10 a);同时,1999年以来拉萨和共和春季下平流层（100~30 hPa）大气温度分别以0.5~1.4℃/(10 a)和0.01~0.9℃/(10 a)速率增加,上对流层(250~175 hPa)大气温度分别以0.2~1.5℃/(10 a)和0.2~1.2℃/(10 a)速率降低。与2008年以来高原整体大气温度变化相比较,均慢于高原下平流层（125~70 hPa) 1~2℃/(10 a)的增温速率,快于高原上对流层（225~175 hPa）0.4~1.1℃/(10 a)的降温速率。两地臭氧与大气温度的相关系数和回归系数计算结果表明,拉萨和共和两个地区1999年以来春季臭氧恢复速率的不同是导致两地同期下平流层-上对流层温度逆转速率差异的重要因子之一。  相似文献   

15.
大气臭氧变化在全球气候和环境中具有重要作用,是当今大气科学领域的重要研究对象之一。对比分析了中国科学院大气物理研究所河北香河大气综合观测试验站2014～2016年Dobson和Brewer两种臭氧总量观测仪器探测结果的一致性,并使用1979～2016年Dobson观测数据分析了香河地区臭氧总量的长期变化趋势。结果表明:进行有效温度修正后,两种臭氧总量仪器观测结果一致性较好,平均偏差仅为-0.14DU(多布森单位),平均绝对偏差为8.00 DU,标准差为36.09 DU,相关系数达0.964。整体来说,两类仪器观测臭氧总量吻合较好。SO2浓度对Dobson仪器数据精度有一定影响,两组仪器数据在SO2浓度为0～0.2DU、0.2～0.4DU和0.4DU大气条件情况下的平均偏差分别为4.8 DU、7.0 DU和8.0 DU,平均偏差随SO2浓度升高而增大。过去38年香河地区的臭氧总量季节差异性强,春、冬两季臭氧总量高,夏、秋两季臭氧总量相对低,季节变化趋势差异明显。从长期变化上看,臭氧总量变化波动有不同的周期,在4个大的时间段变化趋势不同,2000～2010年臭氧层有显著恢复,但最近几年又有变薄的趋势。  相似文献   

16.
平流层对对流层的作用是准确评估、预测对流层气候变化的一个重要方面。其中平流层成分尤其是臭氧的变化,可以改变平流层乃至对流层的辐射平衡,从而影响平流层、对流层的热动力过程。本文从辐射、动力2个角度介绍了平流层臭氧影响对流层气候变化的若干研究进展。平流层臭氧可以通过长短波辐射的方式对对流层大气造成辐射强迫,利用大气化学气候模式可以定量计算平流层臭氧变化引起的辐射强迫,但是辐射强迫的估算受模式中辐射传输模块本身缺陷的影响存在不确定性。动力方面,平流层臭氧变化产生的辐射效应可以改变温度的垂直和经向梯度,造成波折射指数的变化,进而影响平流层甚至对流层内波的折射与反射,通过上对流层下平流层区域内的波—流相互作用,对对流层气候产生影响。另外,南极臭氧损耗可通过大气环状模影响冬春季中高纬度对流层的天气气候,但是其影响的强度大小以及物理机制仍需进一步的确认。值得注意的是,北极平流层臭氧的变化与北半球中高纬度气候变化之间的关系相比南半球要更加复杂,需要更为深入的研究。  相似文献   

17.
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   

18.
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   

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.
2002年夏季，以北京325m气象塔为观测平台，进行了大气污染物臭氧(O3)及其前体物氮氧化物(NOx)和气象要素加强期的同步观测，并对观测资料做了详尽分析。结果表明：边界层内存在明显的臭氧浓度垂直差异；低层(120m)O3浓度呈明显的日变化，且昼夜振幅较大；夜间高层(280m)O3的化学消耗较弱，可维持较高的浓度；稳定度(Ri)在低层以中性态居多，振幅较小，而在高层以不稳定态居多，振幅较大。两层O3湍流输送通量都呈单峰变化。白天，在O3前体物和局地光化学反应共同作用下，120m左右处的O3污染最大。  相似文献   

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