Temperature-Dependent Paracrystalline Nucleation in Atomically Disordered Diamonds.

Abstract

Atomically disordered diamonds with medium-range order realized in recent experiments extend our knowledge of atomic disorder in materials. However, the current understanding of amorphous carbons cannot answer why paracrystalline diamond (p-D) can be formed inherently different from other tetrahedral amorphous carbons (ta-Cs), and the emergence of p-D seems to be easily hindered by inappropriate temperatures. Herein, we performed atomistic-based simulations to shed light on temperature-dependent paracrystalline nucleation in atomically disordered diamonds. Using metadynamics and two carefully designed collective variables, reversible phase transitions among different ta-Cs can be presented under different temperatures, evidenced by corresponding local minima on the free energy surface and reaction path along the free energy gradient. We found that p-D is preferred in a narrow range of temperatures, which is comparable to real experimental temperatures under the Arrhenius framework. The insights and related methods should open up a perspective for investigating other amorphous carbons.