Studies On The Reaction Dynamics Of O⁺+D₂ By Time-dependent Quantum Wave Packet Method

With the development of science and technology,the research of water-ions has become a hot-spot,so scientists have paid more attention to the related reactions.As prototypes of the ion-molecule exothermic reaction which involves the transfer of hydrogen atoms.,O +H2→OH +H and its isotope variations have attracted much attention both experimentally and theoretically.In recent years,the time-dependent quantum wave packet method(TDWP)has become more and more important.It is necessary to use the time-dependent quantum wave packet method to deal with tri-atomic and polyatomic systems.The time-dependent quantum wave packet method is intuitive and accurate.First,the key of the TDWP is sloving the time-dependent Schrodinger equation,and then choose the appropriate coordinate system and the basis function space according to the characteristics of the reaction system and the accuracy of the calculation.According to the characteristics of the selected coordinates and basis functions,the initial wave packet of the system is established,and then the initial wave packet is propagated by the propagation method.Finally,by analyzing the wave function after propagation,we can get the dynamic information that we need.O(4S)+D2(X1Σg+)→OD+(X3Σ-)+D(2S)reaction plays an important role in geophysics,combustion chemistry and physical chemistry.In this paper,based on the latest electron ground state H2O+(X4A")potential energy surface(PES)constructed by Song Yuzhi et al.,we have studied the reaction probability,integral scattering cross section(ICS)and other dynamic information by TDWP.The theoretical results after calculation are analyzed and discussed.First,we study the reaction probability of the reaction under different angular momentum quantum numbers J and different collision energies.It can be seen from the reaction probability that because there is a potential well of 0.912eV on the potential energy surface studied,the reactant will form an ion-atom complex when it passes through the potential well,and the complex formation will lead to the formation of resonance phenomenon.In addition,the reaction will give out the heat of 0.54eV,which results in no threshold value of the reaction probability.However,with the increase of J,the reaction-threshold will begin to appear and move to the direction of increasing collision energy.In addition,we show that the reaction probability is positive correlation with the increase of vibrational quantum number,and the reaction probability is negative correlation with the increase of rotational quantum number,which indicates that for this exothermic reaction,the increase of vibration quantum number will speed up the reaction.The increase of rotational quantum number will hinder the reaction.By comparing our theoretical results of the ICS with the experimental results obtained by the predecessors,the theoretical results obtained by us are correct within the allowable range of errors.The Coriolis-coupling effect plays an important role in ion-molecular reaction.It can affect the formation of molecular clusters and also affect the calculation speed and accuracy of dynamics.Therefore,the effect should be considered in the dynamics calculation.We have calculated the kinetic information of the reaction using the Coriolis coupling effect.Finally,we draw the following conclusion:the intensity of the reaction probability for the Coriolis coupling effect(CC)is smaller than that of the Centrifugal Sudden approximation(CS);In the range of low collision energy,the difference between CC and CS results is larger,and with the increasing of collision energy,the difference between them decreases gradually.In the collision energy range we consider,the results of CC are always larger than those of CS.The comparison of the two results also fully proves that the CC plays an important role in the reaction of ions and molecules.My paper will be expanded from the following parts:first,by studying the experimental aspects and the theoretical aspects,the dynamic method is briefly introduced.Secondly,the theoretical method of Chebyshev polynomial is explained in detail through the derivation of the formula.Then,through the analysis and discussion of the obtained information,we get the information we want.In the end,it is a summary of the thesis and the prospect of the future research.