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

Area of Science:

• Condensed Matter Physics
• Materials Science
• Computational Chemistry

Background:

• Previous literature proposed coexisting localized and iterant 4f-electron cerium atoms in low-density liquid cerium.
• Direct experimental or classical simulation evidence for these distinct cerium atom types has been challenging to obtain.
• Understanding these states is crucial for revealing the unique properties of liquid cerium.

Purpose of the Study:

• To provide ab initio molecular dynamics (MD) simulation evidence for the coexistence of two cerium atom types in low-density liquid cerium.
• To investigate the structural behavior and ordering associated with each cerium atom type.
• To offer new insights into liquid cerium and related amorphous alloys.

Main Methods:

• Utilizing ab initio molecular dynamics (MD) simulations.
• Analyzing low-density liquid cerium at high pressure (13 GPa) and temperature (1900 K).
• Characterizing the 4f-electron localization and local atomic structures.

Main Results:

• Confirmed the coexistence of cerium atoms with localized and iterant 4f-electrons in low-density liquid cerium.
• Observed that cerium atoms with similar 4f-electron localization degrees tend to aggregate.
• Identified icosahedral short-range order (ISRO) around cerium atoms with iterant 4f-electrons, but not around those with highly localized 4f-electrons.

Conclusions:

• The study provides compelling simulation evidence for distinct cerium atom states in liquid cerium.
• The findings reveal unique structural ordering differences based on 4f-electron behavior.
• This work opens new avenues for understanding liquid cerium and developing novel amorphous Ce-based alloys.