Energetics of the coupled electronic-structural transition in the rare-earth nickelates

Abstract

Rare-earth nickelates exhibit a metal-insulator transition accompanied by a structural distortion that breaks the symmetry between formerly equivalent Ni sites. The quantitative theoretical description of this coupled electronic-structural instability is extremely challenging. Here, we address this issue by simultaneously taking into account both structural and electronic degrees of freedom using a charge self-consistent combination of density functional theory and dynamical mean-field theory, together with screened interaction parameters obtained from the constrained random phase approximation. Our total energy calculations show that the coupling to an electronic instability towards a charge disproportionated insulating state is crucial to stabilize the structural distortion, leading to a clear first order character of the coupled transition. The decreasing octahedral rotations across the series suppress this electronic instability and simultaneously increase the screening of the effective Coulomb interaction, thus weakening the correlation effects responsible for the metal-insulator transition. Our approach allows to obtain accurate values for the structural distortion and thus facilitates a comprehensive understanding, both qualitatively and quantitatively, of the complex interplay between structural properties and electronic correlation effects across the nickelate series.

9 pages, 5 figures

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Cited by in corpus (20)

• Mott gapping in 3d ABO3 perovskites without Mott-Hubbard interelectronic U
• Mechanism and Control Parameters of the Coupled Structural and Metal-Insulator Transition in Nickelates
• Comparative Many-Body Study of Pr${}_4$Ni${}_3$O${}_8$ and NdNiO${}_2$
• High-density electron doping of SmNiO${}_3$ from first principles
• Distortion mode anomalies in bulk PrNiO${}_3$ illustrating the potential of symmetry-adapted distortion mode analysis for the study of phase transitions
• Oxygen vacancy induced site-selective mott transition in lanio3
• Improved Description of Perovskite Oxide Crystal Structure and Electronic Properties using Self-Consistent Hubbard $U$ Corrections from ACBN0
• On the effect of charge self-consistency in DFT+DMFT calculations for complex transition metal oxides
• Raman spectroscopic evidence for multiferroicity in rare earth nickelate single crystals
• Dependence of band gaps in d-electron perovskite oxides on magnetism
• Unusual Mott transition associated with charge-order melting in BiNiO${}_3$ under pressure
• Metal-insulator transition and local-moment collapse in negative charge-transfer CaFeO${}_3$ under pressure
• Interplay between breathing-mode distortions and magnetic order in rare-earth nickelates from $ab$ $initio$ magnetic models
• Calculation of screened Coulomb interaction parameters for the charge-disproportionated insulator CaFeO${}_3$
• Optical spectra of rare-earth nickelates
• Interplay between electron correlations, magnetic state, and structural confinement in LaNiO3 ultrathin films
• First-principles study of the electronic, magnetic, and crystal structure of perovskite molybdates
• Influence of $f$ Electrons on the Electronic Band Structure of Rare-Earth Nickelates
• Electronic correlations and spin-charge-density stripes in double-layer La${}_3$Ni${}_2$O${}_7$
• Constrained Random Phase Approximation: the spectral method