First-principles study of electron and hole doping in perovskite nickelates

Abstract

Rare-earth nickelates R${}^{3+}$Ni${}^{3+}$O${}_3$ (R=Lu-Pr, Y) show a striking metal-insulator transition in their bulk phase whose temperature can be tuned by the rare-earth radius. These compounds are also the parent phases of the newly identified infinite layer RNiO2 superconductors. Although intensive theoretical works have been devoted to understand the origin of the metal-insulator transition in the bulk, there have only been a few studies on the role of hole and electron doping by rare-earth substitutions in RNiO${}_3$ materials. Using first-principles calculations based on density functional theory (DFT) we study the effect of hole and electron doping in a prototypical nickelate SmNiO3. We perform calculations without Hubbard-like U potential on Ni 3d levels but with a meta-GGA better amending self-interaction errors. We find that at low doping, polarons form with intermediate localized states in the band gap resulting in a semiconducting behavior. At larger doping, the intermediate states spread more and more in the band gap until they merge either with the valence (hole doping) or the conduction (electron doping) band, ultimately resulting in a metallic state at 25% of R cation substitution. These results are reminiscent of experimental data available in the literature and demonstrate that DFT simulations without any empirical parameter are qualified for studying doping effects in correlated oxides and to explore the mechanisms underlying the superconducting phase of rare-earth nickelates.

References in corpus (25)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Understanding Band Gaps of Solids in Generalized Kohn-Sham Theory
• Orbital order and possible superconductivity in LaNiO3/LaMO3 superlattices
• Phase diagram and superconducting dome of infinite-layer $\mathrm{N}{\mathrm{d}}_{1-\mathrm{x}}\mathrm{S}{\mathrm{r}}_{\mathrm{x}}\mathrm{Ni}{\mathrm{O}}_2$ thin films
• Site-selective Mott transition in rare earth nickelates
• Photoferroelectric oxides
• Ground state oxygen holes and the metal-insulator transition in the negative charge transfer rare-earth nickelates
• A superconducting praseodymium nickelate with infinite layer structure
• Origin of band gaps in 3d perovskite oxides
• Structurally Triggered Metal-Insulator Transition in Rare-Earth Nickelates
• Reconciling the ionic and covalent pictures in rare-earth nickelates
• Low-energy description of the metal-insulator transition in the rare-earth nickelates
• Multiferroicity in rare-earth nickelates RNiO3
• Antiferromagnetic Ground State of La${}_2$CuO${}_4$: A Parameter-free Ab Initio Description
• Mott gapping in 3d ABO3 perovskites without Mott-Hubbard interelectronic U
• Electronic Transitions in Strained SmNiO_3 Thin Films
• Coupling and Electrical Control of Structural, Orbital and Magnetic Orders in Perovskites
• $f$-electron and magnetic ordering effects in nickelates LaNiO${}_2$ and NdNiO${}_2$: remarkable role of the cuprate-like $3d_{x^2-y^2}$ band
• Nickelate superconductors: an ongoing dialog between theory and experiments
• Anti-doping in Insulators and Semiconductors having Intermediate Bands with Trapped Carriers
• Origin of the orbital and spin orderings in rare-earth titanates
• High-density electron doping of SmNiO${}_3$ from first principles
• Landscape of coexisting excitonic states in the insulating single-layer cuprates and nickelates
• Optical spectra of rare-earth nickelates

Cited by in corpus (3)

• Phase formation in hole- and electron-doped rare-earth nickelate single crystals
• Structural instabilities of infinite-layer nickelates from first-principles simulations
• Charge ordering as the driving mechanism for superconductivity in rare-earth nickel oxides