Avoided metallicity in a hole-doped Mott insulator on a triangular lattice.

Doping of a Mott insulator gives rise to a wide variety of exotic emergent states, from high-temperature superconductivity to charge, spin, and orbital orders. The physics underpinning their evolution is, however, poorly understood. A major challenge is the chemical complexity associated with traditional routes to doping. Here, we study the Mott insulating CrO2 layer of the delafossite PdCrO2, where an intrinsic polar catastrophe provides a clean route to doping of the surface. From scanning tunnelling microscopy and angle-resolved photoemission, we find that the surface stays insulating accompanied by a short-range ordered state. From density functional theory, we demonstrate how the formation of charge disproportionation results in an insulating ground state of the surface that is disparate from the hidden Mott insulator in the bulk. We demonstrate that voltage pulses induce local modifications to this state which relax over tens of minutes, pointing to a glassy nature of the charge order.

Chemical Trends of the Bulk and Surface Termination-Dependent Electronic Structure of Metal-Intercalated Transition Metal Dichalcogenides.

The addition of metal intercalants into the van der Waals gaps of transition metal dichalcogenides has shown great promise as a method for controlling their functional properties. For example, chiral helimagnetic states, current-induced magnetization switching, and a giant valley-Zeeman effect have all been demonstrated, generating significant renewed interest in this materials family. Here, we present a combined photoemission and density-functional theory study of three such compounds: , , and , to investigate chemical trends of the intercalant species on their bulk and surface electronic structure. Our resonant photoemission measurements indicate increased hybridization with the itinerant NbS2-derived conduction states with increasing atomic number of the intercalant, leading to pronounced mixing of the nominally localized intercalant states at the Fermi level. Using spatially and angle-resolved photoemission spectroscopy, we show how this impacts surface-termination-dependent charge transfers and leads to the formation of new dispersive states of mixed intercalant-Nb character at the Fermi level for the intercalant-terminated surfaces. This provides an explanation for the origin of anomalous states previously reported in this family of compounds and paves the way for tuning the nature of the magnetic interactions in these systems via control of the hybridization of the magnetic ions with the itinerant states.

Hierarchy of Lifshitz Transitions in the Surface Electronic Structure of Sr_{2}RuO_{4} under Uniaxial Compression.

We report the evolution of the electronic structure at the surface of the layered perovskite Sr_{2}RuO_{4} under large in-plane uniaxial compression, leading to anisotropic B_{1g} strains of ϵ_{xx}-ϵ_{yy}=-0.9±0.1%. From angle-resolved photoemission, we show how this drives a sequence of Lifshitz transitions, reshaping the low-energy electronic structure and the rich spectrum of van Hove singularities that the surface layer of Sr_{2}RuO_{4} hosts. From comparison to tight-binding modeling, we find that the strain is accommodated predominantly by bond-length changes rather than modifications of octahedral tilt and rotation angles. Our study sheds new light on the nature of structural distortions at oxide surfaces, and how targeted control of these can be used to tune density of state singularities to the Fermi level, in turn paving the way to the possible realization of rich collective states at the Sr_{2}RuO_{4} surface.