Exploring the Magnetic Landscape of Easily Exfoliable Two-Dimensional Materials

Area of Science:

• Condensed Matter Physics
• Materials Science
• Computational Materials Science

Background:

• Magnetic materials possess complex energy landscapes with multiple local minima, making global minimum identification difficult.
• Traditional heuristic methods for finding ground-state magnetic order are not always reliable or exhaustive.

Purpose of the Study:

• To systematically explore the energy landscape of 194 magnetic monolayers.
• To determine the ground-state magnetic order of these materials using a novel automated workflow.
• To identify promising magnetic materials for spintronics applications.

Main Methods:

• Application of a recently developed automated workflow for energy landscape exploration.
• Systematic sampling of orbital occupation matrices for rapid local minima identification.
• Utilizing first-principles calculations with Hubbard U corrections (computed via linear-response theory) to refine energy functionals.

Main Results:

• Identification of a diverse range of self-consistent collinear metastable magnetic states.
• Discovery of 109 ferromagnetic, 83 antiferromagnetic, and 2 altermagnetic monolayers.
• Unveiling of 12 novel ferromagnetic half-metals with significant potential for spintronics.

Conclusions:

• The automated workflow provides effective control and sampling for identifying magnetic ground states.
• Hubbard-corrected energy functionals enhance the accuracy of magnetic ordering predictions.
• The identified novel half-metals represent valuable candidates for future spintronics device development.