Intercalation-Induced Exfoliation and Thickness-Modulated Electronic Structure of a Layered Ternary Vanadium Oxide

Solid-state compounds wherein electrons cannot be described as noninteracting particles and instead show strongly correlated behavior are of interest both as systems manifesting novel quantum chemical phenomena as well as for electronic device applications. In the absence of predictive theoretical descriptors, modulation of the properties of these compounds tends to be challenging, and generalizable strategies for modulating closely coupled lattice, orbital, and spin degrees of freedom are exceedingly sparse. Here, it is shown that exfoliation mediated by cation intercalation can serve as a powerful means of modulating the electronic structure of layered correlated materials. Using a strongly correlated and charge-ordered layered compound, δ-Sr0.50V2O5, as a model system, it is shown that the band gap can be drastically altered from ca. 1.07 to 2.32 eV and the electron correlation strength can be greatly modified by intercalation-driven exfoliation to 2D nanosheets upon elimination of structural coherence along one dimension. These findings suggest that intercalation chemistry and solution-phase exfoliation provide a versatile strategy for modulating the electronic structure of quantum materials with potential for realizing Mott and neuromorphic circuitry.