Correlation between the electronic structure, topologic structure and dynamic properties of liquid cerium

Abstract

In literature, two different kinds of cerium atoms, namely Ce atoms with a localized 4f-electron and an iterant 4f-electron, have been suggested to coexist in low-density liquid cerium (A. Cadien et al., Phys. Rev. Lett., 2013, 110, 125503). However, direct evidence of this phenomenon is hard to be detected in the laboratory or classical MD simulations. Thus, the amazing properties of liquid cerium cannot be revealed. Herein, we have shown an ab initio MD simulation evidence that both kinds of cerium atoms can be detected in low-density liquid cerium at 13 GPa and 1900 K. Ce atoms with a similar degree of 4f-electron locality tend to aggregate with each other. An icosahedral short-range order (ISRO) appears for the local structures around the Ce atoms with an iterant 4f electron, whereas it does not appear around the Ce atoms with highly localized 4f electrons. Our study also offers a new perspective and approach to deeply understand liquid Ce and related amorphous Ce-based alloys.