High photon energy spectroscopy of NiO: experiment and theory

Abstract

We have revisited the valence band electronic structure of NiO by means of hard x-ray photoemission spectroscopy (HAXPES) together with theoretical calculations using both the GW method and the local density approximation + dynamical mean-field theory (LDA+DMFT) approaches. The effective impurity problem in DMFT is solved through the exact diagonalization (ED) method. We show that the LDA+DMFT method alone cannot explain all the observed structures in the HAXPES spectra. GW corrections are required for the O bands and Ni-s and p derived states to properly position their binding energies. Our results establish that a combination of the GW and DMFT methods is necessary for correctly describing the electronic structure of NiO in a proper ab-initio framework. We also demonstrate that the inclusion of photoionization cross section is crucial to interpret the HAXPES spectra of NiO.We argue that our conclusions are general and that the here suggested approach is appropriate for any complex transition metal oxide.

16 pages, 5 figures

References in corpus (21)

• Quasiparticle Self-Consistent GW Theory
• Ab initio calculations of quasiparticle band structure in correlated systems: LDA++ approach
• Implementation of the Projector Augmented Wave LDA+U Method: Application to the Electronic Structure of NiO
• All-electron self-consistent GW approximation: Application to Si, MnO, and NiO
• Quasiparticle self-consistent $GW$ method; a basis for the independent-particle approximation
• First principles approach to the electronic structure of strongly correlated systems: combining GW and DMFT
• Theory of quasiparticle spectra for Fe, Co, and Ni: bulk and surface
• NiO: Correlated Bandstructure of a Charge-Transfer Insulator
• Revisiting the valence-band and core-level photoemission spectra of NiO
• LDA+DMFT computation of the electronic spectrum of NiO
• Charge self-consistent dynamical mean-field theory based on the full-potential linear muffin-tin orbital method: methodology and applications
• Combined GW and dynamical mean field theory: Dynamical screening effects in transition metal oxides
• Computing total energies in complex materials using charge self-consistent DFT+DMFT
• Correlation effects in total energy of transition metals and related properties
• Covalency, double-counting and the metal-insulator phase diagram in transition metal oxides
• Electronic entanglement in late transition metal oxides
• Spin wave dispersion based on the quasiparticle self-consistent $GW$ method: NiO, MnO and $\alpha$-MnAs
• Density functional plus dynamical mean field theory of the metal-insulator transition in early transition metal oxides
• GW approximation with LSDA+U method and applications to NiO, MnO, and V${}_2$O${}_3$
• Covalency and the metal-insulator transition in titanate and vanadate perovskites
• Convergence of quasiparticle self-consistent GW calculations of transition metal monoxides

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