Quasiclassical Trajectory Calculation On Reactions H+OF And Its Reverse

Due to the atmospheric abundance of oxygenated compounds, reactions involving atomic oxygen either as reactant or as product, are exceedingly important. Among them, the reactions of hydrogen halides with oxygen atoms have been taken more attention because of their contribution to the catalytic destruction cycle. Because of its relatively simple electronic structure, the HOF system has been considered as one of the model systems for reactions and studied widely. The extensive studies can help us to study other complex HOX(X=Cl,Br,I) reactions.The scalar properties and vector properties of the reactions of H+OF and its reverse have been studied using the quasi-classical trajectory (QCT) method in this paper. This dissertation is composed of three parts. The development of the molecular reaction dynamics and stereodynamics and their present situation are presented in the introduction section. In Section two, the related theories of QCT and the vector correlations are introduced. In Section three, the dynamics of the reactions H+OF and its reverse are extensively studied. First, the reaction probability and reactive cross sections of the reaction H+OF(v =0, j =0) have been calculated. The results are inconsistent with Gogtas'the time-dependent quantum wave packet ones, however they agree with the time dependent wavepacket (TDWP) results calculated by Chu very well in the whole collision energy range, which shows the correctness of QCT calculation and the lack of convergence of Gogtas'quantum wave packet results. Compared with quantum method, it is easy to obtain convergent results and the computational cost is less for QCT, so that QCT method can be considered as the tool which judges the convergence of the quantum results. Based on this, the product branching ratios and the rotational alignment of the product molecules HO have been also calculated, the impact of the regent rotational excitation ( v =0, j =1?3) on stereodynamics has been studied; furthermore, the scalar properties (reaction probability, reactive cross section and the product branching ratios ) and vector properties of its isotopic variants D+OF have been studied, the evident influence of isotope to the product polarization is revealed. In addition, the reaction probability, reactive cross section and the distribution of product rotational alignment of F+HO reaction and its isotopic variants F+DO have been studied. And then, we take F+HO reaction as an example, the theory of the product rotation polarization is applied to the study of the axial polarization, the influences of the different mass and PES on the axial of product molecule have been revealed, which enriches the theories of the stereodynamics. At the last, we take H+OF reaction as an example to study the reagents'alignment using QCT method for the first time, and predict that the influence may attribute to the PES'characters.