Identifying Reaction Pathways in Phase Space via Asymptotic Trajectories

TL;DR

This paper introduces an asymptotic trajectory indicator and an efficient algorithm to identify reaction pathways and phase space structures in chemical reactions, offering an alternative to perturbation theory with demonstrated accuracy in models.

Contribution

The paper presents a reformulated metric and algorithm for reaction pathway identification, applicable to higher-dimensional systems beyond previous methods.

Findings

Accurately reproduces phase space structures like turnstiles in 1D models.

Demonstrates applicability to 3D systems with Langevin baths.

Provides an efficient alternative to perturbation theory for reaction analysis.

Abstract

In this paper, we revisit the concepts of the reactivity map and the reactivity bands as an alternative to the use of perturbation theory for the determination of the phase space geometry of chemical reactions. We introduce a reformulated metric, called the asymptotic trajectory indicator, and an efficient algorithm to obtain reactivity boundaries. We demonstrate that this method has sufficient accuracy to reproduce phase space structures such as turnstiles for a 1D model of the isomerization of ketene in an external field. The asymptotic trajectory indicator can be applied to higher dimensional systems coupled to Langevin baths as we demonstrate for a 3D model of the isomerization of ketene.