Electronic structure of bulk manganese oxide and nickel oxide from coupled cluster theory

Abstract

We describe the ground- and excited-state electronic structure of bulk MnO and NiO, two prototypical correlated electron materials, using coupled cluster theory with single and double excitations (CCSD). As a corollary, this work also reports the first implementation of unrestricted periodic ab initio equation-of motion CCSD. Starting from a Hartree-Fock reference, we find fundamental gaps of 3.46 eV and 4.83 eV for MnO and NiO respectively for the 16 unit supercell, slightly overestimated compared to experiment, although finite-size scaling suggests that the gap is more severely overestimated in the thermodynamic limit. From the character of the correlated electronic bands we find both MnO and NiO to lie in the intermediate Mott/charge-transfer insulator regime, although NiO appears as a charge transfer insulator when only the fundamental gap is considered. While the lowest quasiparticle excitations are of metal 3d and O 2p character in most of the Brillouin zone, near the Γ point, the lowest conduction band quasiparticles are of s character. Our study supports the potential of coupled cluster theory to provide high level many-body insights into correlated solids.

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Cited by in corpus (23)

• Efficient Implementation of Ab Initio Quantum Embedding in Periodic Systems: Density Matrix Embedding Theory
• Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory
• Ab Initio Full Cell GW+DMFT for Correlated Materials
• A periodic equation-of-motion coupled-cluster implementation applied to $F$-centers in alkaline earth oxides
• Towards efficient and accurate \emph{ab initio} solutions to periodic systems via transcorrelation and coupled cluster theory
• Emergence of quantum critical charge and spin-state fluctuations near the pressure-induced Mott transition in MnO, FeO, CoO, and NiO
• A coupled cluster framework for electrons and phonons
• Exchange-striction driven ultrafast nonthermal lattice dynamics in NiO
• Ultrafast manipulation of the NiO antiferromagnetic order via sub-gap optical excitation
• Dynamical correlation energy of metals in large basis sets from downfolding and composite approaches
• Optimization strategies developed on NiO for Heisenberg exchange coupling calculations using projector augmented wave based first-principles DFT+U+J
• Periodic Coupled-Cluster Green's Function for Photoemission Spectra of Realistic Solids
• Non-Dyson Algebraic Diagrammatic Construction Theory for Charged Excitations in Solids
• Inverse Volume Scaling of Finite-Size Error in Periodic Coupled Cluster Theory
• The role of electron correlations in the electronic structure of putative Chern magnet TbMn${}_6$Sn${}_6$
• Finite-size Effects in periodic EOM-CCSD for Ionization Energies and Electron Affinities: Convergence Rate and Extrapolation to the Thermodynamic Limit
• Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2
• Equation of state of atomic solid hydrogen by stochastic many-body wave function methods
• Intriguing electronic and optical prospects of FCC bimetallic two-dimensional heterostructures: epsilon near-zero behaviour in UV-vis range
• Core-Ionized States and X-ray Photoelectron Spectra of Solids From Periodic Algebraic Diagrammatic Construction Theory
• Quantum phase estimation based filtering: performance analysis and application to low-energy spectral calculation
• 1D Transition Metal Oxide Chains as a Challenging Model for Ab Initio Calculations
• Resolving Finite-Size Errors in EOM-CCSD Band Gaps of Solids with Interacting-Bath Dynamical Embedding Theory