Ozone in the Marine Boundary Layer at Cape Grim: Model Simulation     

G. P. Ayers  H. Granek  R. Boers 《Journal of Atmospheric Chemistry》1997,27(2):179-195

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-NO_x conditions of the clean marine boundarylayer net photochemical loss of ozone occurs at all times of year.  相似文献   

Ammonia measurements at Niwot Ridge,Colorado and point arena,California using the tungsten oxide denuder tube technique     

James M. Roberts  Andrew O. Langford  Paul D. Goldan  Fred C. Fehsenfeld 《Journal of Atmospheric Chemistry》1988,7(2):137-152

The applicability of the tungsten oxide denuder tube technique for the measurement of ammonia in the rural troposphere was investigated. The technique is based on selective chemisorption of NH₃ from a gas stream, thermal desorption, conversion to NO, and analysis by NO–O₃ chemiluminescence. Nitric acid, which is also collected and desorbed as NO, was distinguished from NH₃ by differences in desorption temperature. Substituted amines were also collected, but desorbed at a slightly lower temperature than NH₃ in dry air. At high relative humidities, alkylamines may be hydrolyzed to NH₃ on the denuder surface and hence detected as NH₃. Overheating of the denuder tube during the temperature-programmed desorption was found to cause significant irreversible degradation of system performance.The technique was used to measure NH₃ mixing ratios at two rural locations in the United States. At a mountain site in Colorado during the winter of 1984, the average NH₃ mixing ratio was 0.20 ppbv (=0.08 ppbv). At an isolated coastal site in northern California during the spring of 1985, the average NH₃ mixing ratio was 0.36 ppbv (=0.17 ppbv). Correlations of the latter measurements with wind direction and NO _x level suggest that the NH₃ mixing ratio in Pacific marine air at 40°N is <-0.25 ppbv.  相似文献   

An optimized chemiluminescence detector for tropospheric NO measurements     

John W. Drummond  Andreas Volz  Dieter H. Ehhalt 《Journal of Atmospheric Chemistry》1985,2(3):287-306

A detector for the chemiluminescent measurement of NO in background air is described. A large reduction of interferences is achieved by using a stabilized ozone generator which allows operation of the instrument at lower O₃ concentrations. Purification and humidification of the O₃ stream further reduces interferences and shortens the instrumental clean-up time, which is important for aircraft missions. From a series of laboratory tests and from measurements performed aboard an aircraft it is demonstrated that the remaining interferences are acceptable for measurements in the undisturbed troposphere. In particular, no remnant NO signal is observed in clean air at night. During flight, a detection limit (2) of 20 ppt is achieved for a 1 min integration time.  相似文献   

A model investigation of the impact of increases in anthropogenic NO x emissions between 1967 and 1980 on tropospheric ozone     

Jane Dignon  Sultan Hameed 《Journal of Atmospheric Chemistry》1985,3(4):491-506

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   

Evaluation of the tungsten oxide denuder tube technique as a method for the measurement of low concentrations of nitric acid in the troposphere     

J. M. Roberts  R. B. Norton  P. D. Goldan  F. C. Fehsenfeld 《Journal of Atmospheric Chemistry》1987,5(2):217-238

The applicability of the tungsten oxide denuder tube technique for the measurement of nitric acid in the rural troposphere was investigated. The technique is based on selective chemisorption of HNO₃ from the gas stream, thermal desorption, conversion to NO, and analysis by NO–O₃ chemiluminescence. Ammonia, which is also collected and desorbed as NH₃ and NO, was separated from the HNO₃-derived NO by linear temperature-programed thermal desorption. Possible interferences by NO₂, HCN, PAN, and n-propyl nitrate (NPN) were tested and found to be significant under conditions found in the lower troposphere. Simultaneous ambient measurements of HNO₃ were made with the tungsten oxide denuder tube and nylon filter methods at a rural site in the Colorado mountains (Niwot Ridge, CO). Nitric acid levels measured by the tungsten oxide denuder tube averaged a factor of 3 higher than levels measured by the nylon filter technique. Tests involving the placement of nylon materials in front of the tungsten oxide denuder tube show that there are species, as yet unidentified, present in the atmosphere that interfere with the measurement of HNO₃ by the tungsten oxide technique.  相似文献   

Tropospheric ozone profiles near equator and meteorological parameters     

Namita Kundu  A. K. Saha 《Journal of Atmospheric Chemistry》1987,5(3):243-253

This is a study of ozone profile shapes in the 800 to 100 millibar range obtained with balloonsonde data over Trivandrum (8.5° N) during 1975–76 and possible associations of these shapes to some meteorological parameters.Whereas monotonic ozone profiles were noted with clear weather conditions, those associated with cloud cover show three basic anomalous features. Some bulges of increased values are observed in the range of 800 to 500 mb. In the 500–100 mb range, short range or localized cloud cover or passing weather disturbances are associated with fluctuation patterns in the ozone profile and an average depleted value of ozone. The fluctuations are also associated with changing wind speed and direction at these heights.Possible causative mechanisms are discussed. Lightning associated with thundestorm, producing additional CO and NO are sought to interpret the bulges at lower heights. The decrease in values as well as the fluctuation patterns are suggested as due to possible incursion of water vapour from troposphere to stratosphere in the tropical region and dynamical effects associated with it.  相似文献   

Simultaneous measurements of peroxy and nitrate radicals at Schauinsland   总被引：3，自引：0，他引：3  

D. Mihelcic  D. Klemp  P. Müsgen  H. W. Pätz  A. Volz-Thomas 《Journal of Atmospheric Chemistry》1993,16(4):313-335

We present simultaneous field measurements of NO₃ and peroxy radicals made at night in a forested area (Schauinsland, Black Forest, 48° N, 8° N, 1150 ASL), together with measurements of CO, O₃, NO _x , NO _y , and hydrocarbons, as well as meteorological parameters. NO₂, NO₃, HO₂, and (RO₂) radicals are detected with matrix isolation/electron spin resonance (MIESR). NO₃ and HO₂ were found to be present in the range of 0–10 ppt, whilst organic peroxy radicals reached concentrations of 40 ppt. NO₃, RO₂, and HO₂ exhibited strong variations, in contrast to the almost constant values of the longer lived trace gases. The data suggest anticorrelation between NO₃ and RO₂ radical concentrations at night.The measured trace gas set allows the calculation of NO₃ and peroxy radical concentrations, using a chemical box model. From these simulations, it is concluded that the observed anthropogenic hydrocarbons are not sufficient to explain the observed RO₂ concentrations. The chemical budget of both NO₃ and RO₂ radicals can be understood if emissions of monoterpenes are included. The measured HO₂ can only be explained by the model, when NO concentrations at night of around 5 ppt are assumed to be present. The presence of HO₂ radicals implies the presence of hydroxyl radicals at night in concentrations of up to 10⁵ cm^–3.  相似文献   

Comparison of the EMEP, RADM2 and RACM Mechanisms     

Allan Gross  William R. Stockwell 《Journal of Atmospheric Chemistry》2003,44(2):151-170

A comparison of the atmospheric chemistry mechanisms EMEP (Co-operative Programme for Monitoring and Evaluation of the Long-Range Transmission of Air Pollutants in Europe), RADM2 (Regional Acid Deposition Model, version 2) and RACM (Regional Atmospheric Chemistry Mechanism) has been conducted. Each mechanism was used to simulate the PLUME case of Kuhn et al. (1998) and to simulate an additional 150 and 81 scenarios with and without emissions, respectively. These simulations covered scenarios that ranged from relatively clean, through rural and polluted urban conditions. Ozone isopleths and scatter plots were generated from the simulations. The mechanisms were compared primarily on the basis of calculated ozone and ozone precursor concentrations. For the gas-phase ozone precursors the differences between the mechanisms were rather small under clean conditions and more significant under polluted conditions. The differences were especially significant for the concentrations of NO₂ and organic peroxy radicals. In general the EMEP mechanism yielded the most ozone and the RADM2 mechanism yielded the least. Furthermore the results suggest that a broad range simulation conditions should be used to compare mechanisms and not just a few selected scenarios.  相似文献   

A Database for Volatile Organic Compounds     

K. Mannschreck  K. Bächmann  K. H. Becker  Th. Heil  R. Kurtenbach  M. Memmesheimer  V. Mohnen  A. Obermeier  D. Poppe  R. Steinbrecher  Th. Schmitz  A. Volz-Thomas  F. Zabel 《Journal of Atmospheric Chemistry》2002,42(1):281-286

The database for volatile organic compounds (VOC data base) was created with the aim of providing an overview of tropospheric hydrocarbon measurements. The data base contains 202 substances, for which atmospheric and useful kinetic data such as rate coefficients, photolysis frequencies, mixing ratios, emission data and ozone formation potentials are compiled from available literature. The database file can be downloaded without charge from http://www.physchem.uni-wuppertal.de/voc-database. Registered users will be informed about the appearance of updates.  相似文献   

应用GPS资料反演南极大气可降水量的试验分析   总被引：7，自引：0，他引：7       下载免费PDF全文

程晓  徐冠华  周春霞  王清华  鄂栋臣 《极地研究》2002,14(2):136-144

本文研究的主要内容是从对流层天顶延迟来反演大气中的可降水量。利用我国长城和中山两站 1 998、1 999、2 0 0 0年参加全南极GPS国际联测所取得的南极地区的GPS数据 ,组成各期GPS网 ;采用高精度的GAMIT/GLOBK软件进行基线解算和网平差处理 ,使用多种数据处理方案 ,得到各时段两站对流层的天顶总延迟值 ,采用了Saastamonien和Hopfield两种模型分别进行天顶静力学延迟的解算来分离天顶静力学延迟。从两站的历史气象资料出发 ,通过回归计算得到适合两站 1、2月份的转换系数K ;然后进行天顶湿延迟至可降水量的转换 ,结合现场的气象资料进行对比分析。各期数据均取得了较为满意的结果。  相似文献