Orbital-selective Mott and Peierls transition in HxVO2

Abstract

AbstractMaterials displaying metal-insulator transitions (MITs) as a function of external parameters such as temperature, pressure, or composition are most intriguing from the fundamental point of view and also hold high promise for applications. Vanadium dioxide (VO2) is one of the most prominent examples of MIT having prospective applications ranging from intelligent coatings, infrared sensing, or imaging, to Mott memory and neuromorphic devices. The key aspects conditioning possible applications are the controllability and reversibility of the transition. Here we present an intriguing MIT in hydrogenated vanadium dioxide, HxVO2. The transition relies on an increase of the electron occupancy through hydrogenation on the transition metal vanadium, driving the system insulating by a hybrid of two distinct MIT mechanisms. The insulating phase observed in HVO2 with a nominal d2 electronic configuration contrasts with other rutile d2 systems, most of which are metallic. Using spectroscopic tools and state-of-the-art many-body electronic structure calculations, our investigation reveals a correlation-enhanced Peierls and a Mott transition taking place in an orbital-selective manner cooperate to stabilize an insulating phase. The identification of the hybrid mechanism for MIT controlled by hydrogenation opens the way to radically design strategies for future correlated oxide devices by controlling phase reversibly while maintaining high crystallinity.