Density Functional Theory Study of the Entangled Crystal, Magnetic, and Electronic Structures of PuGa3

TL;DR

This study uses density functional theory to explore how crystal, magnetic, and electronic structures of PuGa3 are interconnected, emphasizing the importance of electronic correlation treatment for accurate structural predictions.

Contribution

It demonstrates the entanglement of structural and electronic properties in PuGa3 and highlights the role of magnetic structure and correlation effects in DFT modeling.

Findings

Magnetic structure influences energy more than crystal structure.

Correct structural ordering requires special treatment of 5f electron correlations.

Hubbard bands evolve differently with U for different crystal structures.

Abstract

Systematically studying the crystal, magnetic, and electronic structures of PuGa3 with density functional theory (DFT) reveals the entanglement of the three types of structure. Magnetic structure affects the energy more strongly than crystal structure. For DFT to correctly order the crystal structures in agreement with experiment requires special treatment of the electronic correlation in the 5f states, exemplified here by the GGA+U approach. The upper and lower Hubbard bands change with increasing U in very dissimilar ways for the two most different crystal structures. The results suggest the effectiveness of using magnetic structure to simulate correlation effects in the actinides depends on both the magnetic and the crystal structure.