Magnetic state and electronic structure of plutonium from ``first principles'' calculations

TL;DR

This paper reviews the challenges and methods for accurately modeling plutonium's complex electronic structure using first-principles calculations, focusing on the partial localization of 5f-electrons.

Contribution

It provides a comprehensive review of computational approaches to describe plutonium's electronic states, highlighting the difficulties due to its intermediate 5f-electron localization.

Findings

Standard DFT works for early actinides with itinerant 5f-electrons.

Localized 5f-electrons models suit late actinides like Am and Cm.

Plutonium's partial localization requires specialized methods.

Abstract

The goal to describe plutonium phases from ``first principles'' calculation methods is complicated by the problem of 5f-electrons localization. While for early actinides (Th, U,Np) standard DFT (Density Functional Theory) description with itinerant 5f-electrons works well for late actinides (Am, Cm) DFT calculations with completely localized (pseudocore) 5f-electrons give satisfactory results. However plutonium presents a border case of partial localization and both limits (itinerant and completely localized) are not valid. We present a review of the methods used to solve this problem and discuss what could be the reasons for their successes and failures.