CH4和CD4解离吸附的量子含时动力学研究

运用含时波包法(time-dependent wave packet method),对CH4和CD4在光滑静止的Ni(100)表面的解离吸附进行了量子动力学研究与计算.不同振动态下解离几率随平动能的变化曲线表明,反应分子的振动能对分子的解离有重要贡献,其反应趋势,与其它理论模型得到的结果一致.CH4与CD4解离几率的对数随平动能的变化曲线表明,CH4的解离几率比CD4的要高得多,这种同位素效应,是由它们不同的零点能和量子隧道效应引起的,且与实验结果符合得比较好.

Time-dependent quantum dynamics study of dissociative adsorption of CH4

A time dependent wave packet method was used to study the dynamics of dissociative adsorption of CH4 and CD4 on a flat and static surface. The four dimensional dissociation probabilities were calculated for different vibrational states as a function of translational energies. The results show that excited vibrational energy enhance dissociation probability significantly. And the significant enhancement of the dissociation probability of CH4 when cpmpared to CD4 were explained reasonably in terms of quantum mechanical zero-point energies and the tunneling effect. And our results are in good agreement with experiments and other theoritical results.