论文标题
软盘分子系统和复合物的精确量子动力学发展
Exact quantum dynamics developments for floppy molecular systems and complexes
论文作者
论文摘要
分子旋转,振动,内部旋转,异构化,隧道,弱相互作用的系统的分子间动力学,内部分子内的能量转移,阻碍旋转以及表面上的阻碍翻译是分子运动的重要类型。它们从根本上正确且详细的描述可以通过在势能表面上求解核Schrödinger方程来获得。许多化学有趣的过程都涉及量子核运动,这些核动作在多个势能井上被“离域化”。除了振动问题的高维度外,这些“大振幅”运动还代表了当前(RO)振动方法的挑战。提供了量子核运动方法的综述,确定了解决核schrödinger方程的当前瓶颈,并审查了解决方案策略。对于选定的数值示例,突出显示了在限制模型和与光谱相关的概念方面对这些结果的技术细节,计算结果和分析。
Molecular rotation, vibration, internal rotation, isomerization, tunneling, intermolecular dynamics of weakly and strongly interacting systems, intra-to-inter-molecular energy transfer, hindered rotation and hindered translation over surfaces are important types of molecular motions. Their fundamentally correct and detailed description can be obtained by solving the nuclear Schrödinger equation on a potential energy surface. Many of the chemically interesting processes involve quantum nuclear motions which are `delocalized' over multiple potential energy wells. These `large-amplitude' motions in addition to the high dimensionality of the vibrational problem represent challenges to the current (ro)vibrational methodology. A review of the quantum nuclear motion methodology is provided, current bottlenecks of solving the nuclear Schrödinger equation are identified, and solution strategies are reviewed. Technical details, computational results, and analysis of these results in terms of limiting models and spectroscopically relevant concepts are highlighted for selected numerical examples.