Machine Learning-Assisted Hybrid ReaxFF Simulations

Dundar E. Yilmaz, William Hunter Woodward, Adri C.T. Van Duin

Research output: Contribution to journalArticlepeer-review

6 Scopus citations


We have developed a machine learning (ML)-assisted Hybrid ReaxFF simulation method ("Hybrid/Reax"), which alternates reactive and non-reactive molecular dynamics simulations with the assistance of ML models to simulate phenomena that require longer time scales and/or larger systems than are typically accessible to ReaxFF. Hybrid/Reax uses a specialized tracking tool during the reactive simulations to further accelerate chemical reactions. Non-reactive simulations are used to equilibrate the system after the reactive simulation stage. ML models are used between reactive and non-reactive stages to predict non-reactive force field parameters of the system based on the updated bond topology. Hybrid/Reax simulation cycles can be continued until the desired chemical reactions are observed. As a case study, this method was used to study the cross-linking of a polyethylene (PE) matrix analogue (decane) with the cross-linking agent dicumyl peroxide (DCP). We were able to run relatively long simulations [>20 million molecular dynamics (MD) steps] on a small test system (4660 atoms) to simulate cross-linking reactions of PE in the presence of DCP. Starting with 80 PE molecules, more than half of them cross-linked by the end of the Hybrid/Reax cycles on a single Xeon processor in under 48 h. This simulation would take approximately 1 month if run with pure ReaxFF MD on the same machine.

Original languageEnglish (US)
Pages (from-to)6705-6712
Number of pages8
JournalJournal of Chemical Theory and Computation
Issue number11
StatePublished - Nov 9 2021

All Science Journal Classification (ASJC) codes

  • Computer Science Applications
  • Physical and Theoretical Chemistry


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