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1.
New laboratory measurements of NO2 absorption cross-section were performed using a Fourier transform spectrometer at 2 and 16 cm-1 (0.03 and 0.26 nm at 400 nm) in the visible range (380–830 nm) and at room temperature. The use of a Fourier transform spectrometer leads to a very accurate wavenumber scale (0.005 cm-1, 8×10-5 nm at 400 nm). The uncertainty on the new measurements is better than 4%. Absolute and differential cross-sections are compared with published data, giving an agreement ranging from 2 to 5% for the absolute values. The discrepancies in the differential cross-sections can however reach 18%. The influence of the cross-sections on the ground-based measurement of the stratospheric NO2 total amount is also investigated.  相似文献   

2.
Quantitative infrared measurements of ethane (C2H6) in the upper troposphere and lower stratosphere are reported. The results have been obtained from the analysis of absorption features of the 9 band at 12.2 m, which have been identified in high-resolution ballon-borne and aircraft solar absorption spectra. The ballon-borne spectral data were recorded at sunset with the 0.02 cm-1 resolution University of Denver interferometer system from a float altitude of 33.5 km near Alamogordo, New Mexico, on 23 March 1981. The aircraft spectra were recorded at sunset in July 1978 with a 0.06 cm-1 resolution interferometer aboard a jet aircraft at 12 km altitude, near 35°N, 96°W. The balloon analysis indicates the C2H6 mixing ratio decreased from 3.5 ppbv near 8.8 km to 0.91 ppbv near 12.1 km. The results are consistent with the colum value obtained from the aircraft data.  相似文献   

3.
Infrared absorption features due to ClO in the lower stratosphere have been identified from groundbased solar absorption spectra taken from Aberdeen, U.K. (57° N, 2° W) on 20 January 1995. A vertical column abundance of 3.42 (±0.47)×1015 molec cm-2 has been derived from 13 independent absorption features in the P and R branches of the (0–1) vibration-rotation band of 35ClO, spanning the spectral region 817–855 cm-1. The observed absorption features are consistent with very high levels of ClO (approximately 2.6 parts per billion by volume (ppbv)) in the altitude range 16–22 km. A comparison of this profile with a 3D chemical transport model profile indicates the observation was made inside the polar vortex and shows good qualitative agreement but the model underestimates the concentrations of ClO. Simultaneous measurements of other species were made including HCl, HF and ClONO2. These columns yield a value for HCl+ClONO2+ClO of 7.02±0.65×1015 molec cm-2. This is lower than the total inorganic chlorine (ClO y ) column of 10.7±1.6×1015 molec cm-2 estimated from mean measured (HCl+ClONO2)/HF ratios together with in-vortex HF measurements. The discrepancy is probably due to significant amounts of the ClO dimer (Cl2O2) in the lower part of the stratosphere. The measurements of highly elevated levels of ClO are used to estimate O3 loss rates at the 400, 475 and 550 K levels making assumptions about the probable distribution of ClO and Cl2O2. These are compared with loss rates derived from ozone sonde data.  相似文献   

4.
基于FY-3/IRAS利用非线性模式反演OLR   总被引：1，自引：0，他引：1       下载免费PDF全文
FY-3系列卫星星载IRAS仪器设有26个通道,其中20个通道用于探测地球大气在红外波段的热辐射,通道辐射率代表了地球大气系统在大气顶的向外辐射光谱信息,与总波段的射出长波辐射（OLR）通量相关性高。该文基于逐线辐射传输模式计算软件LBLRTM对全球2521条大气廓线的大气顶射出辐射率模拟数据,计算了每条廓线的OLR和FY-3B/IRAS,FY-3C/IRAS通道辐射率,用统计回归方法建立了利用IRAS的多通道辐射率计算OLR的非线性理论回归模式;应用模式和FY-3B/IRAS,FY-3C/IRAS的L1级数据,处理得到2016年4月1-30日的全球日平均、月平均OLR格点产品。与Aqua/CERES,Terra/CERES仪器宽波段观测OLR产品对比表明:对于水平分辨率为1°×1°的全球月平均OLR格点产品,均方根误差为2.22 W·m-2,相关系数为0.9982 W·m-2,平均偏差为-0.2 W·m-2,表明FY-3/IRAS仪器定标及反演模式均达到较高水平。文中还回顾了历史上不同气象卫星的多种OLR反演算法模式,并对不同模式精度进行了比较。  相似文献   

5.
The line-transition parameters of the High Resolution Transmission (HITRAN) 2008 database have been updated relative to previous editions. The transmission spectra and sensitivity to changes in CO2 concentrations using line parameters from the HITRAN 2004 and HITRAN 2008 databases are compared to evaluate the effect of the database updates on retrievals of carbon dioxide vertical columns from nearinfrared reflected sunlight. This comparison is done in three spectral regions covering the 2.06-, 1.61-, and 1.58-μm CO2bands used by the Greenhouse Gases Observatory Satellite (GOSAT) instrument and the planned successor to the Orbiting Carbon Observatory (OCO). The updates to the HITRAN database have the largest effects on the transmittance and the off-line to on-line transmittance ratio in the 2.06-μm region and the smallest effects on these parameters in the 1.58-μm region. The influence of the updates to the HITRAN database on the off-line to on-line ratio calculation in the narrow spectral region 4855-4880 cm-1 could be equivalent to a change in CO2 of more than 50 ppmv. Use of the HITRAN 2004 database will lead to an underestimate of the column CO2abundance in the 2.06- and 1.61-μm spectral regions, whereas it will lead to an overestimate of the column CO2abundance in the 1.58-μm spectral region.  相似文献   

6.
Monthly mean total vertical column abundances of acetylene have been determined from series of infrared solar spectra recorded at the Jungfraujoch station, Switzerland, between June 1986 and April 1991. The data have been obtained by nonlinear least-squares fittings of the 5 band R19 transition of C2H2 at 776.0818 cm-1. The average of 22 monthly mean total vertical columns of C2H2 retrieved during that time interval of almost 5 years was found to be equal to (1.81±0.12)×1015 molec/cm2, which corresponds to an average mixing ratio of (0,22±0.013) ppbv (parts per billion by volume) in a troposphere extending from the altitude of the station (3.58 km), up to 10.5 km. Despite the large variability found from year to year, a least-squares sine fit to the data reveals a seasonal variation with an amplitude of about ±40% of the mean; the maximum occurs during mid-winter and the minimum in the summer. The present results are compared critically with similar in-situ data found in the literature. A sinusoidal fit to all such free troposphere measurements made in-situ between 30°N and 60°N indicates good agreement in shape and phase with the seasonal variation derived above the Jungfraujoch, but their average column abundance, 2.3×1015 molec/cm2, is about 30% higher; this difference is explained on the basis of non-upwelling meteorological conditions generally prevailing during ground-based remote solar observations.  相似文献   

7.
The kinetics of the reaction of nitrous acid (HONO) with nitric acid (HNO3), nitrate radicals (NO3) and dinitrogen pentoxide (N2O5) have been studied using Fourier transform infrared spectroscopy. Experiments were performed at 700 torr total pressure using synthetic air or argon as diluents. From the observed decay of HONO in the presence of HNO3 a rate constant of k<7×10-19 cm3 molecule-1 s-1 was derived for the reaction of HONO with HNO3. From the observed decay of HONO in the presence of mixtures of N2O5 and NO2 we have also derived upper limits for the rate constants of the reactions of HONO with NO3 and N2O5 of 2×10-15 and 7×10-19 cm3 molecule-1 s-1, respectively. These results are discussed with respect to previous studies and to the atmospheric chemistry of HONO.  相似文献   

8.
New laboratory measurements of NO2 absorption cross-sections have been performed between 300 and 500 nm at ambient temperature with improved experimental conditions: low gas pressures, long absorption paths, suitable absorbance values, narrow spectral bandwidths. The data, stored at 0.01 nm intervals, have been compared to those of the more recent studies and some reasons of disagreement are discussed.In the photolysis region below 400 nm, our absorption cross-sections are larger than those previously published, suggesting that the photodissociation coefficient calculated from the current data sets is underestimated. In the structured region of the spectrum above 400 nm, improvement of the resolution gives more precise values useful for optical measurements in atmosphere.Unité de Recherche Associée au CNRS.  相似文献   

9.
Ground-based visible differential absorption spectrometry during twilight has been used for NO2 total column observations at the Antarctica Peninsula, Marambio Base (64S, 56W), during the austral spring of 1989 (9 September to 25 November).Results show moderate NO2 vertical column levels of 1.5 to 2.5×1015 molec cm-2 in the morning and 2 to 3×1015 molec cm-2 in the evening until middle October, highly modulated by planetary wave activity. From that date until the end of the period, a steady increase occurs which is associated with the rising of lower stratosphere temperature as the vortex weakens, reaching values of 5×1015 molec cm-2 in late November, with small a.m.-p.m. differences. NO2 is found to be positively correlated to both total ozone and 50 hPa temperature during the entire spring. However, when analyzing the departures from linear trends, a highly negative correlation has been observed from day 301 onwards.  相似文献   

10.
A large number of experimental and theoretical investigations of carbon dioxide (CO2) spectra have been conducted since the most recent update of the High-Resolution Transmission Molecular Absorption (...  相似文献   

11.
With improved experimental conditions already used for measurements at ambient temperature (Mérienneet al., 1994), new values have been found for the absorption cross-sections of NO2 at 240 and 220 K in the 400–500 nm spectral region. Using a better resolution than in previous studies we show that the temperature effect is not negligible and should be taken into account for the optical measurements of atmospheric NO2 amounts by differential absorption methods.Unité de Recherche Associée au CNRS.  相似文献   

12.
Measurements of stratospheric NO2 by ground-based visible spectrometers rely on laboratory measurements of absorption cross-sections. We review low-temperature laboratory measurements, which disagree by amounts claimed to be significant. Our recalculation of their errors shows that in general disagreements are not significant and that errors in the ratios of cross-sections at low to room temperature are between ±3% and ±8.8%. Of these errors, up to ±3.5% was contributed by errors in the equilibrium constant,K p, in those measurements where the pressure was above 0.1 mbar.We review measurements and calculations ofK p, which were accurate to ±5% from 300 to 233 K. Each method was potentially flawed. For example, infrared measurements of the partial pressure of NO2 ignored the dependence of absorption on total pressure. From thermodynamic theory, formulae forK pcan be derived from expressions for the variation of heat capacity with temperature. Contrary to common belief, coefficients in the formulae used by spectroscopists were not derived from the thermodynamic quantities. Rather, they were fitted to measurements or to calculations. Hence, they are empirical and it is dangerous to extrapolate below 233 K, the lowest temperature of the measurements.There are no measurements of NO2 cross-sections below 230 K. Extrapolation of these cross-sections to analysis of measurements of NO2 at the low temperatures of the Arctic and Antarctic stratosphere is also dangerous. For satisfactory analysis of polar spectra, the NO2 cross-sections should be measured at temperatures down to 190 K with a relative accuracy of ±1%. This difficult experiment would need a cell of minimum length 32 m whose length can be adjusted. Because their effects are circular, many errors cannot be removed simply. Although circular errors also arise in the measurements ofK pand of the infrared spectrum, their weights differ from those in the visible spectrum. The optimum experiment might therefore simultaneously measure the visible and infrared spectra andK p.  相似文献   

13.
Previous experiments in the 400–500 nm region (Coquart et al., 1995) have been extended to the 200–400 nm region to determine the absorption cross-sections of NO2 at 220 K. The NO2 and N2O4 cross-sections are obtained simultaneously from a calculation applied to the data resulting from measurements at low pressures. A comparison between the NO2 cross-sections at 220 K and at ambient temperature shows that the low temperature cross-sections are generally lower, except in the region of the absorption peaks. Comparisons are also made with previous data at temperature close to 220 K.  相似文献   

14.
The UV-visible absorption cross-sections of HOI have been recorded over the wavelength range 278-494 nm and at 298 K following generation of HOI in the gas phase using laser flash photolysis. The gas phase reaction of OH with I2 was used to produce HOI, and the absorption spectrum of HOI was calibrated relative to the consumption of I2. The HOI spectrum recorded exhibits 2 broad absorption maxima of = 3.99 × 10-19 cm2 and = 2.85 × 10-19 cm2, centred at 338.4 nm and 404.8 nm respectively. The spectrum is adequately described by a parameterisation consisting of two semi-logarithmic Gaussian distribution functions. The HOI spectrum is more intense than that recorded in previous work of Jenkin, but is in good agreement with more recent work by Bauer et al. The parameterised HOI absorption spectrum recorded in this work was used in a radiative model to calculate the atmospheric photolysis rate (J-value) of HOI. These results indicate that, under most sunlit conditions, HOI has a lifetime with respect to solar photolysis of the order of minutes. Experiments attempting to generate HOI by the reaction of O atoms with C2H5I led to complex absorption spectra containing a negative contribution to the absorption from the photolytic removal of an unidentified species. In addition, evidence was found for adsorption and desorption of an iodine-containing species in the reaction vessel. This behaviour is rationalised in terms of the disproportionation of HOI to I2O, and an uncalibrated spectrum tentatively attributed to I2O has been recorded.  相似文献   

15.
This paper describes laboratory experiments designed to obtain the infrared spectra of some atmospherically important radical species and related compounds. A Fourier transform spectrometer was used that was capable of yielding resolutions as great as 0.0024 cm-1, and optical paths of up to 512 m were employed. The objective of the experiments was to obtain the spectra for subsequent application to remote sounding measurements in the atmosphere.Radicals were generated by a variety of chemical reactions involving atoms or other highly reactive precursors. Spectra of the 3 band of NO3, at ca. 1500 cm-1, were obtained with up to 0.005 cm-1 resolution using the reaction between NO2 and O3 to produce the radical. The most satisfactory source of ClO was found to be the reaction between Cl and O3, and the (1-0) vibration-rotation band in the region 829–880 cm-1 was recorded at a resolution of 0.02 cm-1. We were unable to observe infrared absorption of HO2 with any of the radical sources that we tested. High-resolution survey spectra were obtained of compounds used as reactants, or formed as side-products in the radical-generating processes. These compounds included N2O5, HNO3, ClONO2, FNO2, Cl2O, HO2NO2, and probably FO2.The ability to monitor concentrations of the NO3 radical in the visible region of the spectrum as well as the concentrations of reactants and other products in the infrared region allowed us to undertake a study of the time-dependent interactions occurring when NO2 reacts with O3. The results indicate the importance of heterogeneous processes, especially when traces of water are present, and lend credence to suggestions that heterogeneous mechanisms in the NO3–N2O5–H2O system might be a viable source of HNO3 in the atmosphere.  相似文献   

16.
Stratospheric volume mixing ratio profiles of N2O5, CH4, and N2O have been retrieved from a set of 0.052 cm–1 resolution (FWHM) solar occultation spectra recorded at sunrise during a balloon flight from Aire sur l'Adour, France (44° N latitude) on 12 October 1990. The N2O5 results have been derived from measurements of the integrated absorption by the 1246 cm–1 band. Assuming a total intensity of 4.32×10–17 cm–1/molecule cm–2 independent of temperature, the retrieved N2O5 volume mixing ratios in ppbv (parts per billion by volume, 10–9), interpolated to 2 km height spacings, are 1.64±0.49 at 37.5 km, 1.92±0.56 at 35.5 km, 2.06±0.47 at 33.5 km, 1.95±0.42 at 31.5 km, 1.60±0.33 at 29.5 km, 1.26±0.28 at 27.5 km, and 0.85±0.20 at 25.5 km. Error bars indicate the estimated 1- uncertainty including the error in the total band intensity (±20% has been assumed). The retrieved profiles are compared with previous measurements and photochemical model results.Laboratoire associé aux Universités Pierre et Marie Curie et Paris Sud.  相似文献   

17.
Seasonal variations of the spectra of wind speed and air temperature in the mesoscale frequency range from 1.3 × 10-4 to 1.5 × 10-3 Hz (10 min to 2 h periods) have been studied through observations over land for one year. Spectrographs [time series of isopleths of spectral densities, f · S(f) vs f] of wind speed and air temperature contain occasional peaks that are attributed to short-lived mesoscale atmospheric activity with narrow frequency bands. Significant spectral peaks of wind speed were found in 19% of the total observations in winter, and in 15–16% in the other seasons; for air temperature, they occured in 12% of observations in autumn, and in 16–19% in the other seasons. The peaks most often occurred in the period range from 30 min to 1 h; most had durations less than 24 h. Mesoscale fluctuations of wind speed and air temperature were highly correlated, and in most cases, phase differences were 90–180 ° with air temperature leading wind speed. Significant spectral peaks of wind speed often occurred during northerly seasonal cold winds in winter, and accompanied tropical and/or mid-latitude cyclones in the other seasons. When the peaks occurred, wind speed was usually relatively high and the atmospheric surface layer was unstable.  相似文献   

18.
The measurement of column content of carbon monoxide,methane,and other atmospheric traces gases as well as aerosols has been conducted during the fall of 1992 and 1997,using an infrared spectrometer of moderate resolution in the cooperation of the Laboratory for Middle Atmosphere and Global Environment Observation(LAGEO),Institute of Atmospheric Physics,Chinese Academy of Sciences,with the Institute of Atmospheric Physics,Russian Academy of Sciences.The variation characteristics of atmospheric CO column content in Beijing area are presented.The analysis of the measurement shows that the CO column concentration of 0.10 mg cm-2 can be considered as the background over Beijing area.and the concentration as high as 0.75 mg cm-2 was observed under some unfavorable meteorological situations.  相似文献   

19.
Rate constants for the reaction of OH radicals with some branched alkyl nitrates have been measured applying a competitive technique. Methyl nitrite photolysis in synthetic air was used as OH radical source at 295±2 K and 1000 mbar total pressure. Using a rate constant of 2.53×10-12 cm3 s-1 for the reaction of OH radicals with n-butane as reference, the following rate constants were obtained (units: 10-12 cm3 s-1): isopropyl nitrate, 0.59±0.22; isobutyl nitrate, 1.63±0.20; 3-methyl-2-butyl nitrate, 1.95±0.15; 2-methyl-1-butyl nitrate, 2.50±0.15; 3-methyl-1-butyl nitrate, 2.55±0.35. These values have been combined with the literature data to recalculate the substituent factors F(X) for the different nitrate groups which can be used to predict OH rate constants for organic nitrates for which experimental data are not available.Preliminary measurements of the photolysis frequency of isopropyl nitrate have shown that for this nitrate as a model substance, OH reactions and direct photolysis are of equal importance under tropospheric conditions.  相似文献   

20.
张楠  陈宏  杨晓君  韩婷婷 《气象科学》2023,43(6):820-828
利用欧洲中期天气预报中心（European Centre for Medium-Range Weather Forecasts， ECMWF）再分析资料，基于大气扰动分解技术，对2012年7月华北东部两次副高边缘大暴雨事件进行扰动分析。结果表明：边界层及对流层低层扰动辐合中心与副高边缘大暴雨中心有较好地对应关系；扰动锋区和扰动比湿大值区（4 g·kg-1）叠加的区域与大暴雨落区相对应，与切变线类暴雨不同，副高边缘暴雨中心并不是出现在冷暖空气対峙扰动（0 ℃线）的位置，而是发生在扰动锋区内的暖区一侧（扰动温度0 ℃以南）；两次过程均存在自南向北的水汽通道，且水汽在输送过程中不断得到抬升，大暴雨落区对应的扰动水汽通量散度中心分别达到-6.8×10-8g·cm-2·hPa-1·s-1和-11.9×10-8g·cm-2·hPa-1·s-1，为大暴雨的形成提供了较好地水汽条件。  相似文献   

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