Unraveling 5f correlated electronic states in paramagnetic PuSn3

Abstract

Plutonium-based compounds establish an ideal platform for exploring the interplay between long-standing itinerant-localized 5f states and strongly correlated electronic states. In this paper, we exhaustively investigate the 5f correlated electronic states of PuSn3 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 5f 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 5f states. It is predicted that a 5f localized to itinerant crossover is induced by temperature accompanied by the change in Fermi surface topology. Therefore itinerant 5f 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 PuSn3. Furthermore, the 5f electronic correlations are orbital selective, which 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.