Sensitivity of the Shock Initiation Threshold of 1,3,5-Triamino-2,4,6-trinitrobenzene (TATB) to Nuclear Quantum Effects
BW Hamilton and MP Kroonblawd and MM Islam and A Strachan, JOURNAL OF PHYSICAL CHEMISTRY C, 123, 21969-21981 (2019).
Approximating the dynamics of atomic nuclei with classical equations of motion in molecular dynamics (MD) simulations causes an overprediction of the specific heat and omits zero-point energy which can have a significant effect on predictions of the response of materials under dynamical loading. We use quantum and classical thermostats in reactive MD simulations to characterize the effect of energy distribution on the initiation and decomposition of the explosive 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) under shock and thermal loading. Shock simulations using the multiscale shock technique (MSST) show that nuclear quantum effects not only increase the temperature rise during dynamical loading but also lower the shock temperature corresponding to the threshold for initiation of chemical reactions. The lower specific heat and presence of zero point energy contribute approximately equally to these effects. Thermal decomposition simulations show that nuclear quantum effects lower the activation barrier associated with reaction compared to classical simulations. Quite interestingly, comparing quantum and classical simulations as a function of average kinetic energy shows that classical baths result in faster kinetics as compared with quantum ones; we explore the molecular origins of this observation.
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