Critical role of electronic correlations in determining crystal structure of transition metal compounds

Abstract

The choice that a solid system "makes" when adopting a crystal structure (stable or metastable) is ultimately governed by the interactions between electrons forming chemical bonds. By analyzing 6 prototypical binary transition-metal compounds we demonstrate here that the orbitally-selective strong $d$-electron correlations influence dramatically the behavior of the energy as a function of the spatial arrangements of the atoms. Remarkably, we find that the main qualitative features of this complex behavior can be traced back to simple electrostatics, i.e., to the fact that the strong $d$-electron correlations influence substantially the charge transfer mechanism, which, in turn, controls the electrostatic interactions. This result advances our understanding of the influence of strong correlations on the crystal structure, opens a new avenue for extending structure prediction methodologies to strongly correlated materials, and paves the way for predicting and studying metastability and polymorphism in these systems.

Main text: 8 pages, 4 figures, 1 table; Supplemental material: 2 pages, 1 figure, 2 tables

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Cited by in corpus (15)

• Systematic beyond-DFT study of binary transition metal oxides
• Gutzwiller Hybrid Quantum-Classical Computing Approach for Correlated Materials
• Emergence of quantum critical charge and spin-state fluctuations near the pressure-induced Mott transition in MnO, FeO, CoO, and NiO
• Electronic correlations at paramagnetic $(001)$ and $(110)$ NiO surfaces: Charge-transfer and Mott-Hubbard-type gaps at the surface and subsurface of $(110)$ NiO
• Quantum-embedding description of the Anderson lattice model with the ghost Gutzwiller Approximation
• LDA+Usc calculations of phase relations in FeO
• Bypassing the computational bottleneck of quantum-embedding theories for strong electron correlations with machine learning
• Accuracy of ghost-rotationally-invariant slave-boson theory for multiorbital Hubbard models and realistic materials
• Operatorial formulation of the ghost rotationally-invariant slave-Boson theory
• Optical signature for distinguishing between Mott-Hubbard, intermediate and charge-transfer insulators
• Electronic correlations and long-range magnetic ordering in NiO tuned by pressure
• Intermediate spin state and the B1-B2 transition in ferropericlase at tera-Pascal pressures
• Charge self-consistent density functional theory plus ghost rotationally-invariant slave-boson theory for correlated materials
• Efficient slave-boson approach for multiorbital two-particle response functions and superconductivity
• Linear Foundation Model for Quantum Embedding: Data-Driven Compression of the Ghost Gutzwiller Variational Space