Efficient Reaction Space Exploration with ChemTraYzer-TAD

Journal of Chemical Information and Modeling, vol. 62, pp. 890–902

Abstract

The development of a reaction model is often a time-consuming process, especially if unknown reactions have to be found and quantified. To alleviate the reaction modeling process, automated procedures for reaction space exploration are highly desired. We present ChemTraYzer-TAD, a new reactive molecular dynamics acceleration technique aimed at efficient reaction space exploration. The new method is based on the basin confinement strategy known from the temperature-accelerated dynamics (TAD) acceleration method. Our method features integrated ChemTraYzer bond-order processing steps for the automatic and on-the-fly determination of the positions of virtual walls in configuration space that confine the system in a potential energy basin. We use the example of 1,3-dioxolane-4-hydroperoxide-2-yl radical oxidation to show that ChemTraYzer-TAD finds more than 100 different parallel reactions for the given set of reactants in less than 2 ns of simulation time. Among the many observed reactions, ChemTraYzer-TAD finds the expected typical low-temperature reactions despite the use of extremely high simulation temperatures up to 5000 K. Our method also finds a new concerted β-scission plus O 2 addition with a lower reaction barrier than the literature-known and so-far dominant β-scission.

Authors 6

1. Lukas Krep Aachen Institute of Technical Thermodynamics

   RWTH Aachen University

   Affiliation as printed

   Institute of Technical Thermodynamics, RWTH Aachen University, Aachen 52062, Germany

2. Indu Sekhar Roy Aachen Institute of Technical Thermodynamics

   RWTH Aachen University

   Affiliation as printed

   Institute of Technical Thermodynamics, RWTH Aachen University, Aachen 52062, Germany

3. Wassja A. Kopp Aachen Institute of Technical Thermodynamics

   RWTH Aachen University

   Affiliation as printed

   Institute of Technical Thermodynamics, RWTH Aachen University, Aachen 52062, Germany

4. Felix Schmalz Aachen Institute of Technical Thermodynamics

   RWTH Aachen University

   Affiliation as printed

   Institute of Technical Thermodynamics, RWTH Aachen University, Aachen 52062, Germany

5. Can Huang Aachen Institute of Technical Thermodynamics

   RWTH Aachen University

   Affiliation as printed

   Institute of Technical Thermodynamics, RWTH Aachen University, Aachen 52062, Germany

6. Kai O. Leonhard corresponding Aachen Institute of Technical Thermodynamics

   RWTH Aachen University

   Affiliation as printed

   Institute of Technical Thermodynamics, RWTH Aachen University, Aachen 52062, Germany