Unraveling the 4f electronic structures of cerium monopnictides

TL;DR

This study uses advanced first-principles calculations to explore the 4f electronic structures in cerium monopnictides, revealing a crossover from itinerant to localized electrons and orbital-selective correlations across different compounds.

Contribution

It introduces a detailed theoretical analysis of 4f electron behavior in CeX compounds using combined DFT and DMFT methods, highlighting the crossover and orbital selectivity.

Findings

CeN exhibits highly itinerant and mixed-valence 4f electrons.

CeBi shows well-localized 4f electrons with weak valence fluctuations.

A 4f itinerant-localized crossover occurs from CeN to CeBi.

Abstract

In order to unveil the 4f electronic structures in cerium monopnictides (CeX, where X = N, P, As, Sb, and Bi), we employed a state-of-the-art first-principles many-body approach, namely the density functional theory in combination with the single-site dynamical mean-field theory, to make detailed calculations. We find that the 4f electrons in CeN are highly itinerant and mixed-valence, showing a prominent quasi-particle peak near the Fermi level. On the contrary, they become well localized and display weak valence fluctuation in CeBi. It means that a 4f itinerant-localized crossover could emerge upon changing the X atom from N to Bi. Moreover, according to the low-energy behaviors of 4f self-energy functions, we could conclude that the 4f electrons in CeX also demonstrate interesting orbital-selective electronic correlations, which are similar to the other cerium-based heavy fermion compounds.