CH_4和CD_4解离吸附的量子含时动力学研究

运用含时波包法 (time -dependentwavepacketmethod) ,对CH4和CD4在光滑静止的Ni( 10 0 )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 CH_4

A time dependent wave packet method was used to study the dynamics of dissociative adsorption of CH 4 and CD 4 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 CH 4 when cpmpared to CD 4 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.