Electronic Structure of Heavy Fermion Uranium Compounds Studied by Core-Level Photoelectron Spectroscopy

TL;DR

This study uses high-resolution photoelectron spectroscopy to analyze the electronic structure and uranium valence states in various heavy Fermion uranium compounds, revealing differences in 5f electron hybridization and correlation effects.

Contribution

It provides detailed spectral analysis linking core-level line shapes to the degree of 5f electron hybridization and correlation in uranium compounds, highlighting distinctions among different materials.

Findings

U 5f electrons in some compounds are well hybridized with ligand states.

Spectral line shapes vary systematically with electronic structure.

U 5f electron count is close to three in some compounds and near two in UPt3.

Abstract

High-energy-resolution core-level and valence-band photoelectron spectroscopic studies were performed for the heavy Fermion uranium compounds UGe2, UCoGe, URhGe, URu2Si2, UNi2Al3, UPd2Al3, and UPt3 as well as typical localized and itinerant uranium compounds to understand the relationship between the uranium valence state and their core-level spectral line shapes. In addition to the main line and high-binding energy satellite structure recognized in the core-level spectra of uranium compounds, a shoulder structure on the lower binding energy side of the main lines of localized and nearly localized uranium compounds was also found. The spectral line shapes show a systematic variation depending on the U 5f electronic structure. The core-level spectra of UGe2, UCoGe, URhGe, URu2Si2, and UNi2Al3 are rather similar to those of itinerant compounds, suggesting that U 5f electrons in these compounds are well hybridized with ligand states. On the other hand, the core-level spectra of UPd2Al3 and UPt3 show considerably different spectral line shapes from those of the itinerant compounds, suggesting that U 5f electrons in UPd2Al3 and UPt3 are less hybridized with ligand states, leading to the correlated nature of U 5f electrons in these compounds. The dominant final state characters in their core-level spectra suggest that the numbers of 5f electrons in UGe2, UCoGe, URhGe, URu2Si2, UNi2Al3, and UPd2Al3 are close to but less than three, while that of UPt3 is close to two rather than to three.