Bandwidth-control orbital-selective delocalization of 4f electrons in epitaxial Ce films

Abstract

The 4f-electron delocalization plays a key role in the low-temperature properties of rare-earth metals and intermetallics, including heavy fermions and mix-valent compounds, and is normally realized by the many-body Kondo coupling between 4f and conduction electrons. Due to the large onsite Coulomb repulsion of 4f electrons, the bandwidth-control Mott-type delocalization, commonly observed in d-electron systems, is difficult in 4f-electron systems and remains elusive in spectroscopic experiments. Here we demonstrate that the bandwidth-control orbital-selective delocalization of 4f electrons can be realized in epitaxial Ce films by thermal annealing, which results in a metastable surface phase with a reduced layer spacing. The resulting quasiparticle bands exhibit large dispersion with exclusive 4f character near E_F and extend reasonably far below the Fermi energy, which can be explained from the Mott physics. The experimental quasiparticle dispersion agrees surprisingly well with density-functional theory calculation and also exhibits unusual temperature dependence, which could be a direct consequence of the delicate interplay between the bandwidth-control Mott physics and the coexisting Kondo hybridization. Our work therefore opens up the opportunity to study the interaction between two well-known localization-delocalization mechanisms in correlation physics, i.e., Kondo vs Mott, which can be important for a fundamental understanding of 4f-electron systems.