Unraveling exotic 5$f$ states and paramagnetic phase of PuSn$_3$

TL;DR

This study uses advanced theoretical methods to explore the temperature-dependent electronic states of PuSn₃, revealing a transition from localized to itinerant 5f electrons, hybridization effects, and implications for its paramagnetic behavior.

Contribution

It provides a comprehensive analysis of the correlated 5f electronic states in PuSn₃, highlighting temperature-induced crossover and orbital selectivity using combined density functional and dynamical mean-field theories.

Findings

Growth of narrow 5f spectral weight at low temperature

Observation of quasiparticle multiplets near the Fermi level

Temperature-induced crossover from localized to itinerant 5f states

Abstract

Plutonium-based compounds establish an ideal platform for exploring the interplay between long-standing itinerant-localized 5$f$ states and strongly correlated electronic states. In this paper, we exhaustively investigate the correlated 5$f$ electronic states of PuSn$_3$ dependence on temperature by means of a combination of the density functional theory and the embedded dynamical mean-field theory. It is found that the spectral weight of narrow 5$f$ band grows significantly and remarkable quasiparticle multiplets appear around the Fermi level at low temperature. A striking $c-f$ hybridization and prominent valence state fluctuations indicate the advent of coherence and itinerancy of 5$f$ states. It is predicted that a 5$f$ localized to itinerant crossover is induced by temperature accompanied by the change in Fermi surface topology. Therefore itinerant 5$f$ states are inclined to take in active chemical bonding, suppressing the formation of local magnetic moment of Pu atoms, which partly elucidates the intrinsic feature of paramagnetic ground state of PuSn$_3$. Furthermore, the 5$f$ electronic correlations are orbital selective manifested themselves in differentiated band renormalizations and electron effective masses. Consequently, the convincing results remain crucial to our understanding of plutonium-based compounds and promote ongoing research.