Zr/Ba/Na fluoride glass molecular dynamics studies at atmospheric pressure and 4 GPa I: equilibration and the glass transition

A constant volume, atmospheric pressure Zr/Ba/Na fluoride glass has been simulated by molecular dynamics with the limitations of the Born-Mayer-Huggins potentials, used previously and resulting in high simulation pressures, having been overcome. The simulated structure of this glass as well as its activation energy for diffusion are in very good agreement with those experimentally observed. To highlight the changes brought on by the decrease in pressure, the simulation at atmospheric pressure has been compared with one at high pressure. The results show that structural energy (total and potential), specific heat and pressure derivative changes occur with the reduction in pressure. In addition, a greater structural relaxation rate and a glass with a lower configurational variation were also observed. The glass transition has also been studied and it was found, on moving from glass to liquid temperatures, to be caused by the breaking of structural and geometric constraints. As expected, a sharp increase in the MSD was observed after the glass transition