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1.
The simultaneous measurements of NO, NO2 and HNOA mixing‐ratio profiles carried out on the Stratoprobe balloon flight of 22 July 1974 have been simulated with a time‐dependent model using the measured temperature and ozone profiles. The calculated ratios of NO/NO2, HNO3/NO2 using currently accepted photochemistry are consistent with the measured ratios within the experimental errors of the measurements. The measured NO2/NO ratio is almost a factor of two smaller than predicted, although the discrepancy is still within the experimental errors. A remarkable proportionality in the NO2 and O3 profiles has been noted and is unexplained. A time‐dependent simulation has been employed to convert the measurements into diurnally‐averaged profiles suitable for intercomparison with two‐dimensional stratospheric models and a comparison with constituent profiles from Prinn et al. (1975) is carried out as an example. The NOV mixing ratio, formed from the sum of the NO, NO2 and HNO2 measurements is similar to the NOV mixing ratio from several one‐ and two‐dimensional models used to predict the effects of SST's on the ozone layer. The odd nitrogen mixing ratio is roughly constant from 20 to 35 km at 11 ppbv. 相似文献
2.
3.
Gerhard Kramm Hans Müller David Fowler Klaus D. Höfken Franz X. Meixner Eberhard Schaller 《Journal of Atmospheric Chemistry》1991,13(3):265-288
A modified profile method for determining the vertical deposition (or/and exhalation) fluxes of NO, NO2, ozone, and HNO3 in the atmospheric surface layer is presented. This method is based on the generally accepted micrometeorological ideas of the transfer of momentum, sensible heat and matter near the Earth's surface and the chemical reactions among these trace gases. The analysis (aerodynamic profile method) includes a detailed determination of the micrometeorological quantities (such as the friction velocity, the fluxes of sensible and latent heat, the roughness length and the zero plane displacement), and of the height-invariant fluxes of the composed chemically conservative trace gases with group concentrations c
1=[NO]+[NO2]+[HNO3], c
2=[NO2]+[O3]+3/2·[HNO3], and c
3=[NO]–[O3]–1/2·[HNO3]. The fluxes of the individual species are finally determined by the numerical solution of a system of coupled nonlinear ordinary differential equations for the concentrations of ozone and HNO3 (decoding method). The parameterization of the fluxes is based on the flux-gradient relationships in the turbulent region of the atmospheric surface layer. The model requires only the vertical profile data of wind velocity, temperature and humidity and concentrations of NO, NO2, ozone, and HNO3.The method has been applied to vertical profile data obtained at Jülich (September 1984) and collected in the BIATEX joint field experiment LOVENOX (Halvergate, U.K., September 1989). 相似文献
4.
H. K. Roscoe B. J. Kerridge S. Pollitt N. Louisnard J. M. Flaud C. Camy-Peyret C. Alamichel J-P. Pommereau T. Ogawa N. Iwagami M. T. Coffey W. Mankin W. F. J. Evans C. T. McElroy J. Kerr 《Journal of Atmospheric Chemistry》1990,10(2):111-144
During the 1982 and 1983 Balloon Intercomparison Campaigns, the vertical profile of stratospheric NO2 was measured remotely by nine instruments and that of NO by two. Total overhead columns were measured by two more instruments. Between 30 and 35km, where measurements overlapped, agreement between NO profiles was within ±30%, which is better than the accuracies claimed by the experimenters. Between 35 and 40km there was similarly good agreement between NO2 profiles, but below 30km, differences of greater than a factor three were found. In the second Campaign, NO2 values from most instruments agreed within their quoted errors, except that the Oxford radiometer gave much lower values; but the first Campaign and the column measurements show a more uniform spread of results.These differences below 30km could not be resolved, but new laboratory measurements are planned which should do so. 相似文献
5.
Measurements of absorption properties of some gases in the atmosphere were made by using CO line-tunable laser. Experimental equipment and method are briefly described. Absorption coefficients of NO, NO2, NH3, CO2 and H2O at some definite laser wavelengths are given, and variations of absorption properties with both partial and total pressures are discussed. 相似文献
6.
热带深对流云对CO、NO、NOx和O3的垂直输送作用 总被引：2，自引：1，他引：1
利用2005年11月至2006年2月ACTIVE (Aerosol and Chemical Transport in tropIcal conVEction) 外场试验期间在澳大利亚北部达尔文地区取得的CO、O3、NO和NOx飞机探测资料, 并结合HYSPLIT后向轨迹模式结果, 分析这几种气体成分在对流卷云砧内外的分布情况, 并探讨热带深对流云对于污染气体的垂直输送作用。分析结果显示, 在孤立对流云卷云砧中, 云砧内部O3、NO、NOx浓度均大于云外; 而CO则不同, 只有在近地面浓度高时才如此, 在近地面浓度较小时, 卷云砧内部的浓度反而小于云外。进一步分析造成这两类气体分布差异的原因, 发现CO主要借助深对流云将对流层下层以及对流云周围环境中的CO夹卷并动力垂直输送到对流云顶部卷云砧中, 而对于O3、NO和NOx来说, 除了上述作用以外, 还可能与对流云内部其他物理机制(如闪电), 造成新的O3、NO和NOx有关, 这些新生气体随着风暴内部强烈的上升气流被最终输送进云砧中。 相似文献
7.
Field measurements of NO and NO2 emissions from soils have been performed in Finthen near Mainz (F.R.G.) and in Utrera near Seville (Spain). The applied method employed a flow box coupled with a chemiluminescent NO
x
detector allowing the determination of minimum flux rates of 2 g N m-2 h-1 for NO and 3 g m-2 h-1 for NO2.The NO and NO2 flux rates were found to be strongly dependent on soil surface temperatures and showed strong daily variations with maximum values during the early afternoon and minimum values during the early morning. Between the daily variation patterns of NO and NO2, there was a time lag of about 2 h which seem to be due to the different physico-chemical properties of NO and NO2. The apparent activation energy of NO emission calculated from the Arrhenius equation ranged between 44 and 103 kJ per mole. The NO and NO2 emission rates were positively correlated with soil moisture in the upper soil layer.The measurements carried out in August in Finthen clearly indicate the establishment of NO and NO2 equilibrium mixing ratios which appeared to be on the order of 20 ppbv for NO and 10 ppbv for NO2. The soil acted as a net sink for ambient air NO and NO2 mixing ratios higher than the equilibrium values and a net source for NO and NO2 mixing ratios lower than the equilibrium values. This behaviour as well as the observation of equilibrium mixing ratios clearly indicate that NO and NO2 are formed and destroyed concurrently in the soil.Average flux rates measured on bare unfertilized soils were about 10 g N m-2 h-1 for NO2 and 8 g N m-2 h-1 for NO. The NO and NO2 flux rates were significantly reduced on plant covered soil plots. In some cases, the flux rates of both gases became negative indicating that the vegetation may act as a sink for atmospheric NO and NO2.Application of mineral fertilizers increased the NO and NO2 emission rates. Highest emission rates were observed for urea followed by NH4Cl, NH4NO3 and NaNO3. The fertilizer loss rates ranged from 0.1% for NaNO3 to 5.4% for urea. Vegetation cover substantially reduced the fertilizer loss rate.The total NO
x
emission from soil is estimated to be 11 Tg N yr-1. This figure is an upper limit and includes the emission of 7 Tg N yr-1 from natural unfertilized soils, 2 Tg N yr-1 from fertilized soils as well as 2 Tg N yr-1 from animal excreta. Despite its speculative character, this estimation indicates that NO
x
emission by soil is important for tropospheric chemistry especially in remote areas where the NO
x
production by other sources is comparatively small. 相似文献
8.
本文利用国产XZJ—1型CO选支激光器测量了NO 5.2微米带和NO_2 6.2微米带49个激光频率处的吸收系数,对吸收变化特征进行了初步分析并且讨论了实验误差及实际大气监测中水汽干扰等问题. 相似文献
9.
Abstract Ground‐based measurements of stratospheric NO2, using absorption spectroscopy of twilight sky in the spectral region 437–451 nm, have been made at Calgary (51.08°N, 114.13°W), Alberta, Canada, during the period December 1978‐March 10, 1979. The NO2 showed a rather steady behaviour in the month of December when there was no stratospheric warming in progress; the monthly average of the afternoon vertical column abundance for December was 1.7 × 1015 cm2. In the rest of the observation period the NO2 showed a complex behaviour, but this behaviour appears to be explicable in terms of the stratospheric circulation changes taking place in that period due to the occurrence of a stratospheric warming event. 相似文献
10.
A low pressure laser-excited-fluorescence technique (FAGE) for the direct determination of atmospheric NO2 has been developed. Using a frequency-doubled Nd-YAG pump laser and a signal collection time of 20 s (10 s each signal and background) a detection limit of 450 pptv is calculated under laboratory conditions. Improved sensitivities will be possible with a higher repetition rate laser and lower fluorescence cell pressures. 相似文献
11.
The absorption properties of NO in 5.2 μm band and NO2 in 6.2 μm band are measured for some definite wavelengths by using line-tunable CO laser and long-path absorption cell. The absorption coefficients for 49 CO laser wavelengths are given and variations of absorption withpartial and total pressures are analysed. Fur-thermore, the experimental errors and the interference of water vapour with the absorption at definite laser lines are also discussed. 相似文献
12.
The chemical reactivity of NO and NO2 is so rapid that their fluxes and concentrations can be considerably modified from that expected for conserved variables in the atmospheric surface layer, even as low as a meter above the surface. Fitzjarrald and Lenschow (1983) have calculated flux and mean concentration profiles for NO, NO2 and O3 in the surface layer using numerical techniques. However, their solutions do not approach the photostationary state at large heights. Here we solve a simpler set of equations analytically (i.e. we assume a constant O3 concentration and neutral hydrodynamic stability), and are able to show how the flux profiles behave at large heights assuming that the concentrations approach their photostationary values. We find, for example, that at large heights the ratio of the flux of NO to that of NO2 is equal to the ratio of their concentrations. These results are relevant to estimating surface fluxes of NO and NO2, and are most applicable to nonurban environments where NO and NO2 concentrations are usually much less than O3 concentration.The National Center for Atmospheric Research is sponsored by the National Science Foundation. 相似文献
13.
14.
S. Madronich D. R. Hastie H. I. Schiff B. A. Ridley 《Journal of Atmospheric Chemistry》1985,3(2):233-245
The photodissociation coefficient of NO2, J
NO
2, has been measured from a balloon platform in the stratosphere. Results from two balloon flights are reported. High Sun values of J
NO
2 measured were 10.5±0.3 and 10.3±0.3×10-3 s-1 at 24 and 32 km respectively. The decrease in J
NO
2 at sunset was monitored in both flights. The measurements are found to be in good agreement with calculations of J
NO
2 using a simplified isotropic multiple scattering computer routine. 相似文献
15.
南京北郊冬季大气SO2、NO2和O3的变化特征 总被引：1，自引：0，他引：1
利用差分吸收光谱仪DOAS（differential optical absorption spectroscopy）,对2007年11月—2008年1月南京北郊大气SO2、NO2和O3进行了观测。结合Parsivel降水粒子谱仪和自动气象站的资料,对冬季大气污染气体的浓度变化规律及降水和风速风向对其的影响进行了分析。结果表明,南京北郊大气SO2浓度较高,呈明显双峰特征,分别在12时（北京时,下同）和00时达最大,受附近排放源的影响最大,东风及南风时比静风时SO2浓度更高。降水对SO2湿清除效果明显,清除系数平均为0.168 h-1。NO2气体呈明显单峰特征,在18时达最高值。南京北郊是NO2源区之一,主要受附近高速公路汽车尾气排放源的影响。静风时NO2浓度最高。O3浓度受NO2的影响较明显。O3日变化呈单峰特征,在15时达最大值,静风时O3浓度最低。降水对O3的间接影响较明显,在降水时,白天由于太阳辐射较弱,O3浓度降低;夜晚NO浓度较低,使得O3浓度升高。 相似文献
16.
Vladislav V. Zelenov Elena V. Aparina Andrey V. Ivanov 《Journal of Atmospheric Chemistry》2014,71(1):33-53
Using a coated-insert flow tube reactor coupled to a low-energy electron-impact mass spectrometer with molecular beam sampling, we studied uptake of NO3 by sea salt at room temperature and [NO3]?=?8?1011???4?1013 molecule cm?3. The radical uptake coefficient γ(t) is time dependent: its initial value (γ ini) decreases exponentially with the characteristic time (τ) to its steady-state value (γ ss) at given [NO3]. The parameters γ ini, γ ss and τ depend on [NO3], whereas γ ss is water vapor independent at [H2O]?=?8?1012???1.6?1015 molecule cm?3 and RH ≤ 0.5 %. HCl and NO2 are uptake products detected in the gas phase. We used these findings to estimate γ values under tropospheric conditions for urban coastal and remote marine environments: at high NO3 (~90 ppt), the time dependence becomes important, and the γ value averaged over the aerosol lifetime is 4?10?3; at low NO3 (~1 ppt), the radical uptake is time independent and proceeds faster with γ ini?=?8?10?3 相似文献
17.
T. Nishanth K. M. Praseed M. K. Satheesh Kumar 《Meteorology and Atmospheric Physics》2011,113(1-2):67-73
Surface ozone is mainly produced by the photodissociation of nitrogen dioxide (NO2) by solar UV radiation. Subsequently, solar eclipses provide one of the unique occasions to explore the variations in the photolysis rate of NO2 and their significant impact on the production of ozone at a location. This study aims to examine the diurnal variations in the photodissociation rate coefficient of NO2, (j(NO2*)), and mixing ratios of surface ozone and NO X * (NO?+?NO2*) during the solar eclipse that occurred on 15 January 2010 at Kannur (11.9°N, 75.4°E, 5?m amsl), a tropical coastal site on the Arabian Sea in South India. This investigation was carried out on the basis of the ground level observations of surface ozone and its prominent precursor NO2*. The j(NO2*) values were estimated from the observed solar UV-A flux data. A sharp decline in j(NO2*) and surface ozone was observed during the eclipse phase because of the decreased efficiency of the ozone formation from NO2. The NO2* levels were found to increase during this episode, whereas the NO levels remained unchanged. The surface ozone concentration was reduced by 57.5%, whereas, on the other hand, that of NO X * increased by 62.5% during the solar eclipse. Subsequently a reduction of *% in the magnitude of j(NO2*) was found here during the maximum obscuration. Reductions in solar insolation, air temperature and wind speed were also observed during the solar eclipse event. The relative humidity showed a 6.4% decrease during the eclipse phase, which was a unique observation at this site. 相似文献
18.
D. A. Jaffe R. E. Honrath D. Furness T. J. Conway E. Dlugokencky L. P. Steele 《Journal of Atmospheric Chemistry》1995,20(3):213-227
In this paper we quantify the CH4, CO2 and NO
x
emissions during routine operations at a major oil and gas production facility, Prudhoe Bay, Alaska, using the concentrations of combustion by products measured at the NOAA-CMDL observatory at Barrow, Alaska and fuel consumption data from Prudhoe Bay. During the 1989 and 1990 measurement campaigns, 10 periods (called events) were unambiguously identified where surface winds carry the Prudhoe Bay emissions to Barrow (approximately 300 km). The events ranged in duration from 8–48 h and bring ambient air masses containing substantially elevated concentrations of CH4, CO2 and NO
y
to Barrow. Using the slope of the observed CH4 vs CO2 concentrations during the events and the CO2 emissions based on reported fuel consumption data, we calculate annual CH4 emissions of (24+/–8)×103 metric tons from the facility. In a similar manner, the annual NO
x
emissions are calculated to be (12+/–4)×103 metric tons, which is in agreement with an independently determined value. The calculated CH4 emissions represent the amount released during routine operations including leakage. However this quantity would not include CH4 released during non-routine operations, such as from venting or gas flaring. 相似文献
19.
Mikhail Yu. Gershenzon Sergeid. Il'in Nikolai G. Fedotov Yulii M. Gershenzon Elena V. Aparina Vladislav V. Zelenov 《Journal of Atmospheric Chemistry》1999,34(1):119-135
A simple kinetic mechanism of nitrate radicals uptake on dry sea-salt NaCl, NaBr surfaces is proposed. The mechanism includes adsorption/desorption equilibrium and unimolecular decomposition of the adsorbed complex: NO3(g) + NaX(s) (NO3-NaX)(s); (NO3-NaX)(s) NaNO3 + X(s) Two techniques were used: the matrix isolation ESR and mass spectrometry. The uptake coefficient () is found to be dependent on exposure time of salt to NO3 for raw coating. The initial (t0) is higher than the observable steady-state obs. At room temperature obs is independent of [NO3] at low [NO3] = 3 × 109 - 1011 cm-3, but it is inversely proportional to [NO3] at concentrations higher than 1012 cm-3. At temperatures above 100 °C, obs becomes independent of [NO3] in a wider range of [NO3]. An increased number of dislocations is supposed to exist in the case of raw coating. Due to a wide spread of the surface sites binding energy with the ionic lattice near dislocations, the part of surface complexes has lower binding energy and "burns" more rapidly. That burning determines the transition from (t0) down to obs.The kinetic parameters and elementary rate coefficients are obtained. The recommended for low atmospheric NO3 concentration are in the range of 0.002 ± 0.04 for NaCl and 0.1-0.3 for NaBr depending on a mechanism of the (t) relaxation. 相似文献
20.
An Intercomparison of NO2 and OClO Measurements at Arrival Heights, Antarctica during Austral Spring 1996 总被引：2，自引：0，他引：2
R. W. Sanders S. Solomon K. Kreher P. V. Johnston 《Journal of Atmospheric Chemistry》1999,33(3):283-298
For several years NO2 and OClO, two species important to understanding ozone destruction in the Antarctic stratosphere, have been measured at Arrival Heights, Antarctica by two groups: New Zealand's National Institute of Water and Atmospheric Research (NIWA) and the NOAA Aeronomy Laboratory in Boulder, Colorado. Using data independently collected by these two groups during the Austral spring of 1996, it is shown that the two data sets are in extremely close agreement. Besides offering validation of the instrumentation and analysis techniques of both groups, this result provides confidence in the more complete history of these species gained by combining the two data sets. 相似文献