Dynamics between reactants and products are often mediated by a rate-determining barrier and an associated dividing surface leading to the transition state theory rate. This framework is challenged when the barrier is time-dependent because its motion can give rise to recrossings across the fixed dividing surface. A non-recrossing time-dependent dividing surface can neverthless be attached to the TS trajectory resulting in recrossing-free dynamics. We extend the formalism —contstructed using Lagrangian Descriptors— to systems with additional bath degrees of freedom. The propagation of reactant ensembles provides a numerical demonstration that our dividing surface is recrossing-free and leads to exact TST rates.

中文翻译：

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使用拉格朗日描述符获得时间相关的多维分割面

反应物和产物之间的动力学通常由决定速率的障碍和导致过渡态理论速率的相关分界面介导。当障碍物是随时间变化的时，此框架将受到挑战，因为障碍物的运动会引起在固定分隔面上的交叉。无论如何，非穿越时间相关的分割表面都可以附着在TS轨迹上，从而实现无穿越的动力学。我们将形式主义（使用拉格朗日描述符构造）扩展到具有更多浴自由度的系统。反应物集合体的传播提供了一个数值证明，证明我们的分隔表面无交叉，可产生精确的TST速率。