In recent decades, ab initio molecular dynamics (AIMD) simulations have been applied to gain atomic insights into HE materials . In an AIMD simulation, an HE material is represented by an atomic model with interatomic forces determined by electronic structure calculations, and the Newtonian equations of motion are solved to obtain the dynamic trajectories. Thus, AIMD allows chemical reactions (i.e. bond breaking and forming events) to occur and accounts for electronic polarization effects.