ChemRxiv
These are preliminary reports that have not been peer-reviewed. They should not be regarded as conclusive, guide clinical practice/health-related behavior, or be reported in news media as established information. For more information, please see our FAQs.
1/1
0/0

Development of the ChIMES Force Field for Reactive Molecular Systems: Carbon Monoxide at Extreme Conditions

preprint
revised on 29.08.2019 and posted on 30.08.2019 by Rebecca Lindsey, Nir Goldman, Laurence E. Fried, Sorin Bastea

We have developed a transferable reactive force field for C/O systems under extreme temperature and pressure conditions based on the many-body Chebyshev Interaction Model for Efficient Simulation (ChIMES). The resulting model is shown to recover much of the accuracy of DFT for prediction of structure, dynamics and chemistry when applied to dissociative systems at 1:1 and 1:2 C:O ratios, as well as molten carbon. Our C/O modeling approach exhibits a 104 increase in efficiency and linear system size scalability over standard quantum molecular dynamics methods, allowing simulation of significantly larger systems than previously possible. Furthermore, we show that system sizes of at least 500 atoms are required to observe the formation of experimentally predicted molten carbon condensates under oxygen-deficient conditions, indicative of possible system size effects in quantum simulations of these types of systems. Overall, we find the present ChIMES model to be well suited for modeling chemical processes and cluster formation at pressures and temperatures typical of shock waves. We expect that the present C/O modeling paradigm can serve as a template for the development of a high pressure --high temperature organic chemistry force-field.

Funding

17-ERD-011

History

Email Address of Submitting Author

lindsey11@llnl.gov

Institution

Lawrence Livermore National Laboratory

Country

United States of America

ORCID For Submitting Author

0000-0002-3438-9064

Declaration of Conflict of Interest

The authors declare no competing financial interest.

Exports

Logo branding

Exports