Efficient Reaction Space Exploration with ChemTraYzer-TAD

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 beta-scission plus O-2 addition with a lower reaction barrier than the literature-known and so-far dominant beta-scission.

Automated summary

Developing a reaction model can be time-consuming, so automated procedures for reaction space exploration are desired. We present ChemTraYzer-TAD, a new reactive molecular dynamics acceleration technique that efficiently explores reaction space. Our method finds over 100 different parallel reactions and identifies a new reaction pathway.