Metal-insulator transition in CaVO${}_3$ thin films: interplay between epitaxial strain, dimensional confinement, and surface effects

Abstract

We use density functional theory plus dynamical mean-field theory (DFT+DMFT) to study multiple control parameters for tuning the metal-insulator transition (MIT) in CaVO${}_3$ thin films. We focus on separating the effects resulting from substrate-induced epitaxial strain from those related to the reduced thickness of the film. We show that tensile epitaxial strain of around 3-4% is sufficient to induce a transition to a paramagnetic Mott-insulating phase. This corresponds to the level of strain that could be achieved on a SrTiO${}_3$ substrate. Using free-standing slab models, we then demonstrate that reduced film thickness can also cause a MIT in CaVO${}_3$, however, only for thicknesses of less than 4 perovskite units. Our calculations indicate that the MIT in such ultra-thin films results mainly from a surface-induced crystal-field splitting between the $t_{2g}$-orbitals, favoring the formation of an orbitally-polarized Mott insulator. This surface-induced crystal-field splitting is of the same type as the one resulting from tensile epitaxial strain, and thus the two effects can also cooperate. Furthermore, our calculations confirm an enhancement of correlation effects at the film surface, resulting in a reduced quasiparticle spectral weight in the outermost layer, whereas bulk-like properties are recovered within only a few layers away from the surface.

10 pages, 9 figures

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• On the effect of charge self-consistency in DFT+DMFT calculations for complex transition metal oxides
• Strain Tuning of Plasma Frequency in Vanadate, Niobate, and Molybdate Perovskite Oxides
• Electronic Localization in CaVO3 Films via Bandwidth Control
• Wavefunctions, electronic localization and bonding properties for correlated materials beyond the Kohn-Sham formalism
• Anisotropy of electronic correlations: On the applicability of local theories to layered materials
• Quantum Confinement Induced Metal-Insulator Transition in Strongly Correlated Quantum Wells of SrVO${}_3$ Superlattice
• Multilayer engineering of CaVO${}_3$ thin films with SrTiO${}_3$ and LaAlO${}_3$ from DFT+DMFT
• Effect of Off-Diagonal Elements in Wannier Hamiltonian on DFT+DMFT for low-symmetry material: Study of Li${}_2$MnO${}_3$