Atmospheric chemistry of diazomethane – an experimental and theoretical study

The kinetics of the O₃, OH and NO₃ radical reactions with diazomethane were studied in smog chamber experiments employing long-path FTIR and PTR-ToF-MS detection. The rate coefficients were determined to be k _CH2NN+O3?=?(3.2?±?0.4)?×?10^?17 and k _CH2NN+OH?=?(1.68?±?0.12)?×?10^?10 cm³ molecule^?1 s^?1 at 295?±?3?K and 1013?±?30 hPa, whereas the CH₂NN?+?NO₃ reaction was too fast to be determined in the static smog chamber experiments. Formaldehyde was the sole product observed in all the reactions. The experimental results are supported by CCSD(T*)-F12a/aug-cc-pVTZ//M062X/aug-cc-pVTZ calculations showing the reactions to proceed exclusively via addition to the carbon atom. The atmospheric fate of diazomethane is discussed.     

N_2和O_2纯转动拉曼光谱(PRRS)的温度特性

计算了N2 和O2 的PRRS ,讨论了其温度特性。提出通过测量N2 和O2 的PRRS计算大气温度的方法。     

Mössbauer and X-ray diffraction characterization of Fe60Al40 coatings prepared by thermal spraying

Microstructured (atomized) and nanostructured (milled) Fe₆₀Al₄₀ powders together with their corresponding coatings synthesized by High Velocity Oxy-fuel (HVOF) or Atmospheric Plasma Spray (APS) thermal spraying techniques have been characterized by Mössbauer Spectroscopy (MS) and X-ray Diffraction (XRD). The evolution of the microstructure and the atomic ordering degree in the powders and coatings are discussed at the light of the various processing conditions. The operational correlation between the parameters of the duplex morphology of coatings and the processing parameters is discussed.     

Iterative regularization methods for atmospheric remote sensing

In this paper we present different inversion algorithms for nonlinear ill-posed problems arising in atmosphere remote sensing. The proposed methods are Landweber's method (LwM), the iteratively regularized Gauss-Newton method, and the conventional and regularizing Levenberg-Marquardt method. In addition, some accelerated LwMs and a technique for smoothing the Levenberg-Marquardt solution are proposed. The numerical performance of the methods is studied by means of simulations. Results are presented for an inverse problem in atmospheric remote sensing, i.e., temperature sounding with an airborne uplooking high-resolution far-infrared spectrometer.     

Intercomparison of retrieval codes used for the analysis of high-resolution, ground-based FTIR measurements

A rigorous and systematic intercomparison of codes used for the retrieval of trace gas profiles from high-resolution ground-based solar absorption FTIR measurements is presented for the first time. Spectra were analyzed with the two widely used independent, retrieval codes: SFIT2 and PROFFIT9. Vertical profiles of O₃, HNO₃, HDO, and N₂O were derived from the same set of typical observed spectra. Analysis of O₃ was improved by using updated line parameters. It is shown that profiles and total column amounts are in excellent agreement, when similar constraints are applied, and that the resolution kernel matrices are also consistent. Owing to the limited altitude resolution of ground-based observations, the impact of the constraints on the solution is not negligible. It is shown that the results are also compatible for independently chosen constraints. Perspectives for refined constraints are discussed. It can be concluded that the error budget introduced by the radiative transfer code and the retrieval algorithm on total columns deduced from high-resolution ground-based solar FTIR spectra is below 1%.     

A new polar nephelometer for measurement of atmospheric aerosols

The angular dependence of light scattered by aerosol particles in the atmosphere—the aerosol phase function—is one of the key properties of every radiative transfer and climate model. Side-scattering in the atmosphere is currently believed to be underestimated by most of the radiative transfer models in certain cases. The aerosol phase function can be measured with polar nephelometers.An innovative polar nephelometer able to measure the phase function of ambient aerosol directly is presented in this publication. The performance of the device was simulated completely using ray-tracing techniques. The results of these simulations are used to interpret the measurement data precisely. The measurements with the new polar nephelometer are fully automated. The quality of the measurement results was verified using different approaches. The values of the statistical and systematic error in measuring atmospheric aerosol are about 4% each. Scattering angles from 10° to 160° were measured and it is shown that with the same design this range can be extended to 3-177° in steps of 0.16° with an aperture of less than 1.8°.Measurements of the aerosol phase function are presented and compared with data taken with an integrating nephelometer and measurements of the particulate matter concentration. All data correlate very well. The described polar nephelometer can measure the phase function and the scattering coefficient of atmospheric aerosol with high accuracy and can be used for continuous monitoring measurements as well as in field campaigns.     

A boundary element method for the calculation of noise barrier insertion loss in the presence of atmospheric turbulence

Atmospheric turbulence is an important factor that limits the amount of attenuation a barrier can provide in the outdoor environment. It is therefore important to develop a reliable method to predict its effect on barrier performance. The boundary element method (BEM) has been shown to be a very effective technique for predicting barrier insertion loss in the absence of turbulence. This paper develops a simple and efficient modification of the BEM formulation to predict the insertion loss of a barrier in the presence of atmospheric turbulence. The modification is based on two alternative methods: (1) random realisations of log-amplitude and phase fluctuations of boundary sources and (2) de-correlation of source coherence using the mutual coherence function (MCF). An investigation into the behaviours of these two methods is carried out and simplified forms of the methods developed. Some systematic differences between the predictions from the methods are found. When incorporated into the BEM formulation, the method of random realisations and the method of MCF de-correlation provide predictions that agree well with predictions by the parabolic equation method and by the scattering cross-section method on a variety of thin barrier configurations.     

Extension of the range of resonator scanning spectrometer into submillimeter band and some perspectives of its further developments

Extension of the working frequency of modern resonator spectrometers into submillimeter wave range is described. Experimental record of atmospheric absorption spectrum covering 45-370 GHz range is demonstrated for the first time, and measured water vapor J′_{ka′, kc′}-J_{ka, kc} = 5_1,5-4_2,2 at 325 GHz line parameters are presented. For the first time pressure lineshift for the 325-GHz water vapor line is measured. Further extension of working range is discussed. New estimations of physical limits of time needed for measurements of absorption in the whole Backward Wave Oscillator (BWO) range are given for phase continuous synthesizer regime. Basic schemes of fast broadband continuous phase synthesized sources are discussed. Verification of the previous measurements of water vapor 3_1,3-2_2,0 at 183 GHz line parameters is presented. Comparisons with ringdown resonator spectrometers are given.     

Atmospheric aerosol limb scanning based on the lunar eclipses photometry

The work is devoted to the analysis of the surface photometric observations of two total lunar eclipses in 2004. The lunar surface relative brightness distribution inside the umbra was used to retrieve the vertical distribution of aerosol extinction of the solar radiation expanding by a tangent path and its dependence on the location at the limb of the Earth. The upper altitude of troposphere aerosol layer was estimated for different latitude zones. The correlation between additional aerosol extinction in the upper troposphere and cyclones was investigated.