Evolution of 4f-Electron States in the Metal-Insulator Transition of PrRu$_4$P$_{12}$

TL;DR

This study investigates how 4f-electron states in PrRu4P12 evolve from localized to hybridized states across the metal-insulator transition, revealing the role of p-f mixing in driving the transition.

Contribution

It provides experimental evidence of the evolution of 4f-electron states and the hybridization process associated with the metal-insulator transition in PrRu4P12.

Findings

Crystal-field excitations broaden and shift near TM-I.

4f-electron states evolve from localized to hybridized.

p-f hybridization drives the metal-insulator transition.

Abstract

Magnetic excitations of the filled skutterudite PrRu4P12 exhibiting a metal-insulator (M-I) transition at TM-I= 63 K were studied by inelastic neutron scattering experiment. The spectra at temperatures much lower than TM-I are described as well-defined crystal-field excitations. With approaching TM-I, the excitation peaks broaden and shift considerably together with the temperature variation of the carrier number and the atomic displacement in the transition. The 4f-electron state evolve from the well localized state in the insulator phase to the strongly hybridized itinerant state by p-f mixing near TM-I. The hybridization is responsible for the M-I transition of PrRu4P12.