Interplay of broken symmetry and delocalized excitations in the insulating state of 1 T –TaS 2
Coexistence of localized and extended excitations is central to the macroscopic properties of correlated materials. For 5d transition-metal compounds, electron correlations alone generally do not lead to a metal-insulator (Mott) transition, with insulating behavior usually resulting from their coupling with magnetic ordering and/or structural distortions. 1T–TaS 2 is a prototypical example of such correlated insulating behavior, with a high-symmetry metallic phase transforming into a distorted, charge-density wave (CDW) insulating state at low temperatures. The nature of the insulating phase as well as the existence and relevance of the localized electron physics remains debated. We resolve this standing controversy in 1T–TaS 2 combining resonant inelastic x-ray spectroscopy and first-principles calculations. We observe five electronic excitations arising from the interband transitions of the Ta 5d orbitals and the S 3p ligand state, with none of the excitations on the order of the Mott gap. These excitations cannot be explained within the framework of standard multiplet calculations that assume a localized wave function, but instead, are captured by a band-theory framework accounting for the low symmetry of the crystal field in the CDW state. Our findings suggest that the electronic properties of 1T–TaS 2 are dominated in the visible by both plasmonic quasiparticles and interband transitions, with no resonance associated with a putative Mott transition observed in the 0–3 eV energy range. Finally, our discovery provides insights into the electron localization and the Mott vs band-insulator debate in 1T–TaS 2 and other transition-metal materials.