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41.
An ab-initio molecular dynamics procedure without precalculation of the Born-Oppenheimer energy surface based on an iterative non-local density functional method employing Gaussian atomic basis has been developed. Analytical gradients are calculated and used for the propagation of nuclei. Sufficiently long trajectories can be calculated at an acceptable computational cost, allowing for analysis of dynamical behaviour of small metallic clusters. This is illustrated on an example of the Li8 cluster. Temperature behaviour of different type of isomers has been investigated. Calculated power spectra allow to identify the presence of more than one isomeric forms along the given trajectories.  相似文献   
42.
It was demonstrated that some foreign metal monolayers formed by underpotential deposition have pronounced catalytic effects on the oxidation of formic acid on platinum. The explanation of these effects was sought within the framewor of existing data on the formic acid oxidation and the underpotential deposition. It was found that the catalytic effect of foreign metal monolayers originates in the decrease of hydrogen adsorption thus preventing the formation of the main poisoning species COH. At the same time these experiments confirm the previously postulated mechanism of formation of the poisoning species involving adsorbed hydrogen.  相似文献   
43.
The existence of zeros ofZ (k)(t) in short intervals of the type [T, T+H] is established, whereHT a(k)logT, . Hitherto the sharpest bounds for the constanta(k) are obtained by employing a certain exponential averaging technique and the estimation of the relevant exponential sums. Bounds for are also derived, under the assumption that orZ(t) does not vanish in certain short intervals.  相似文献   
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We report results of a study of the Stark broadening of halogen atom lines from (1 D)n p levels. Wall stabilized arc is used as a plasma source. Electron densities 2.2–3.2×1022 m?3 are determined from the width ofH α line and electron temperature 9300–10000 K from plasma composition data. The agreement with the results of simple semiclassical calculations is within the limits of the estimated errors of both experiment and theory. An explanation for the large discrepancy between theory and experiment detected for three BrI lines is offered.  相似文献   
48.
We report measured Stark shifts and widths of neutral flourine and chlorine lines. Wall stabilized arc is used as a plasma source. Electron densities 2–4×1022 m?3 are determined from the width of theH β line and electron temperatures 9500–10 000 K from plasma composition data. Experimental results for FI and ClI Stark widths and FI Stark shifts agree within 10% with semiclassical calculations. ClI Stark shifts are systematically smaller for about 20% than theoretical data with the only exception of the line from multiplet no. 15 where the discrepancy goes up to 49%. Results of investigation of similarities and regularities of Stark widths are in agreement with the study of Wiese and Konjevi?. Comparison of experimental Stark shifts shows certain types of regularities.  相似文献   
49.
The subject of this report is the determination of lysophospholipids; lysophosphatidylcholine, lysophosphatidylethanolamine, lysophosphatidylserine and lysophosphatidic acid, by matrix-assisted laser desorption/ionisation time-of-flight mass spectrometry (MALDI-TOF MS). The mean signal-to-noise ratio (S/N) was used for the first time as a measure of lysophospholipid concentration. Two different sample preparation procedures were applied, the 'standard' procedure and the 'premix' in order to check to what extent these methods influence the results of the lysophospholipid quantification. Results can be summarised as follows: (a) All classes of lysophospholipids can be easily and sensitively analysed by MALDI-TOF MS. The smallest detectable amount of lysophospholipids was 0.09 pmol on the sample plate. That is about two orders of magnitude lower than the amount detectable by standard chromatographic methods. (b) The mean S/N of all peaks detected in the positive ion mass spectra can be used as a measure of the lysophospholipid concentration. Whereas the S/N for neutral lysophospholipids correlated with the applied concentrations only when the samples were analysed as 'premix', the sample preparation and application procedure did not influence the quantification of acidic lysophospholipids. The standard deviations were not higher than 10% of the mean value. (c) All spectra were additionally analysed in the presence of CsCl. The addition of caesium ions makes the peak identification unambiguous in phospholipid mixtures, but the Cs adducts of lysophospholipids do not properly reflect their concentration and, therefore, they were not useful for quantification. (d) The applicability of the method was demonstrated on the organic extract of human neutrophils.  相似文献   
50.
A systematic study for the optimization and implementation of high-performance capillary electrophoresis (HPCE) in conjunction with negative ion electrospray ionization-quadrupole time of flight-tandem mass spectrometry (ESI-QTOF-MS/MS) for the analysis of complex glycolipids is described. The performance of the capillary electrophoresis (CE) and off-line CE/ESI-QTOF-MS approach has been explored for screening a complex ganglioside mixture from bovine brain. All instrumental and solution parameters demonstrated to require special adjustment and to have the most substantial effect on the CE separation, abundance of product ions produced in a low-energy collision-induced dissociation (CID) process and their detection by MS/MS, when attempting to identify and sequence single ganglioside molecular species from CE eluted fractions. Upon optimization of the experimental parameters, an efficient methodology emerged providing the general basic requirements for combined CE/ESI-MS analysis of this type of complex glycoconjugate.  相似文献   
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