Parallel replica dynamics simulations of reactions in shock compressed liquid benzene

E Martinez and R Perriot and EM Kober and P Bowlan and M Powell and S McGrane and MJ Cawkwell, JOURNAL OF CHEMICAL PHYSICS, 150, 244108 (2019).

DOI: 10.1063/1.5092209

The study of the long-term evolution of slow chemical reactions is challenging because quantum-based reactive molecular dynamics simulation times are typically limited to hundreds of picoseconds. Here, the extended Lagrangian Born-Oppenheimer molecular dynamics formalism is used in conjunction with parallel replica dynamics to obtain an accurate tool to describe the long-term chemical dynamics of shock-compressed benzene. Langevin dynamics has been employed at different temperatures to calculate the first reaction times in liquid benzene at pressures and temperatures consistent with its unreacted Hugoniot. Our coupled engine runs for times on the order of nanoseconds (one to two orders of magnitude longer than traditional techniques) and is capable of detecting reactions that are characterized by rates significantly slower than we could study before. At lower pressures and temperatures, we mainly observe Diels-Alder metastable reactions, whereas at higher pressures and temperatures we observe stable polymerization reactions. Published under license by AIP Publishing.

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