Efficient Reaction Space Exploration with ChemTraYzer-TAD

L Krep and IS Roy and W Kopp and F Schmalz and C Huang and K Leonhard, JOURNAL OF CHEMICAL INFORMATION AND MODELING, 62, 1-13 (2022).

DOI: 10.1021/acs.jcim.1c01197

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.

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