An \emph{ab initio} study of structural phase transitions of crystalline aluminum under ultrahigh pressures based on ensemble theory

Abstract

It is a long-time pursuit of computations with \emph{ab initio} precision of thermal contributions to phase behaviors of condensed matters under extreme conditions. In this work, the pressure induced structural phase transitions of crystalline aluminum up to $600$ GPa at room temperature are investigated based on the criterion of Gibbs free energy derived directly from the partition function that formulated in the ensemble theory with the interatomic interactions characterized by density functional theory computations. The transition pressures of the FCC$\rightarrow$HCP$\rightarrow$BCC phase transitions are determined at $194$ and $361$ GPa, the axial ratio of the stable HCP structure is found to be equal to $1.62$ and the discontinuities in the equations of states are confirmed to be associated with $-0.67\%$ and $-0.90\%$ volume changes, which are all in an excellent agreement with the measurements by one of the recent experiments but differ from other experimental observations. Compared with the results obtained by the criterion of enthalpy at $0$K, this work further shows the nontrivial thermal impacts on the structural stability of aluminum under ultrahigh-pressure circumstances even at room temperature.