Quantum driven proton diffusion in brucite-like minerals under high pressure

2020 
We investigate the elementary steps at the microscopic level for proton diffusion in brucite under high pressure, which results from a complex interplay between two processes: the O-H reorientations motion around the $\mathbf c$ axis and O-H covalent bond dissociations. First-principle path-integral molecular dynamics simulations reveal that the increasing pressure tends to lock the former motion, while, in contrast, it activates the latter which is mainly triggered by nuclear quantum effects. These two competing effects therefore give rise to a pressure sweet spot for proton diffusion within the mineral. In brucite \ce{Mg(OH)2}, proton diffusion reaches a maximum for pressures close to 70GPa, while the structurally similar portlandite \ce{Ca(OH)2} never shows proton diffusion within the pressure range and time scale that we explored. We analyze the different behaviors of brucite and portlandite, which might constitute two prototypes for other minerals with the same structure.
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