Automated Discovery of Elementary Chemical Reaction Steps Using Freezing String and Berny Optimization Methods

TL;DR

This paper introduces an automated protocol combining freezing string and Berny optimization methods to discover elementary chemical reaction steps, including unknown pathways, enhancing chemical understanding and simulation accuracy.

Contribution

The authors develop a fully automated approach for discovering elementary reaction steps using combined transition-state optimization algorithms, enabling detection of both known and novel pathways.

Findings

Successfully identified known reaction pathways without human intervention.

Discovered new reaction pathways involving significant atom rearrangements.

Demonstrated applicability to combustion and atmospheric chemistry systems.

Abstract

We present a simple protocol which allows fully automated discovery of elementary chemical reaction steps using in cooperation single- and double-ended transition-state optimization algorithms - the freezing string and Berny optimization methods, respectively. To demonstrate the utility of the proposed approach, the reactivity of several systems of combustion and atmospheric chemistry importance is investigated. The proposed algorithm allowed us to detect without any human intervention not only "known" reaction pathways, manually detected in the previous studies, but also new, previously "unknown", reaction pathways which involve significant atom rearrangements. We believe that applying such a systematic approach to elementary reaction path finding will greatly accelerate the possibility of discovery of new chemistry and will lead to more accurate computer simulations of various chemical processes.