Temperature-driven hidden 5f itinerant-localized crossover in heavy-fermion compound PuIn3

TL;DR

This study uses advanced theoretical methods to explore how 5f electrons in PuIn3 transition between itinerant and localized states with temperature, revealing a hidden crossover and potential electronic and magnetic phase changes.

Contribution

It introduces a combined DFT+DMFT approach to identify a hidden temperature-driven 5f electron crossover in PuIn3, advancing understanding of its electronic structure.

Findings

Correctly reproduces experimental photoemission spectra

Identifies a hidden 5f itinerant-localized crossover

Suggests a possible Lifshitz transition and magnetic order onset

Abstract

The temperature-dependent evolution pattern of 5f electrons helps to elucidate the long-standing itinerant-localized dual nature in plutonium-based compounds. In this work, we investigate the correlated electronic states of PuIn3 dependence on temperature by using a combination of the density functional theory and the dynamical mean-field theory. Not only the experimental photoemission spectroscopy is correctly reproduced, but also a possible hidden 5f itinerant-localized crossover is identified. Moreover, it is found that the quasiparticle multiplets from the many-body transitions gradually enhance with decreasing temperature, accompanied by the hybridizations with 5f electrons and conduction bands. The temperature-induced variation of Fermi surface topology suggests a possible electronic Lifshitz transition and the onset of magnetic order at low temperature. Finally, the ubiquitous existence orbital selective 5f electron correlation is also discovered in PuIn3. These illuminating results shall enrich the understanding on Pu-based compounds and serve as critical predictions for ongoing experimental research.