The photodissociation of HCl in the cluster Ar...HCl by an extremely short pulse was studied using a hybrid quantum mechanical/classical approach. In this method, the H atom is treated quantum mechanically, the heavy atoms classically, and the time‐dependent self‐consistent‐field (TDSCF) approximation is used to couple the quantum with the classical modes. The results are compared with those of classical trajectory calculations. On the whole, good qualitative agreement is found between the results of the (partly quantum) hybrid method and the pure classical ones. However, quantum interference effects of quantitative significance are found both in the angular and in the kinetic energy distribution of the H atom product. These effects, and resonances that contribute to the process, are analyzed in terms of wave packets obtained for the H atom in the hybrid method. The usefulness and applicability of the hybrid method are discussed in the light of the results.
展开▼
机译:HCl在团簇Ar中的光解离...使用混合量子力学/经典方法研究了极短脉冲的 HCl。在这种方法中,H原子被量子力学地处理,重原子被经典地处理,并且使用时间与连字符相关的自连字符一致场(TDSCF)近似来耦合量子与经典模式。将结果与经典轨迹计算结果进行了比较。总的来说,(部分量子)混合方法的结果与纯经典方法的结果之间发现了良好的质量一致性。然而,在H原子产物的角度和动能分布中都发现了具有定量意义的量子干涉效应。这些效应以及有助于该过程的共振,根据在混合方法中获得的 H 原子的波包进行分析。结合研究结果,讨论了混合方法的实用性和适用性。
展开▼