Abstract
A thorough understanding of the kinetics and dynamics of combusting mixtures is of considerable interest, especially in regimes beyond the reach of current experimental validation. The ReaxFF reactive force field method has provided a way to simulate large-scale systems of hydrogen combustion via a parametrized potential that can simulate bond breaking. This modeling approach has been applied to hydrogen combustion, as well as myriad other reactive chemical systems. In this work, we benchmark the performance of several common parametrizations of this potential against higher-level quantum mechanical (QM) approaches. We demonstrate instances where these parametrizations of the ReaxFF potential fail both quantitatively and qualitatively to describe reactive events relevant for hydrogen combustion systems.
| Original language | English |
|---|---|
| Pages (from-to) | 5631-5645 |
| Number of pages | 15 |
| Journal | Journal of Physical Chemistry A |
| Volume | 124 |
| Issue number | 27 |
| DOIs | |
| State | Published - Jul 9 2020 |
| Externally published | Yes |
Funding
This work is supported by the U.S. Army Research Laboratory and U.S Army Research Office under Grant No. W911NF-14-1-0359. L.W.B. thanks the NSF for a NSF Graduate Research Fellowship, DGE-1106400. L.W.B. and M.H.-G. thank Allan Avila and Igor Mezić for useful discussions of the ReaxFF potential and Teresa Head-Gordon, Itai Leven, Akshaya Das, Christopher Stein, Matthias Loipersberger, Abdulrahman Aldossary, and Kevin Ikeda for useful discussions of molecular dynamics.