Direct detection of dimer orbitals in Ba${}_5$AlIr${}_2$O${}_{11}$

Abstract

The electronic states of many Mott insulators, including iridates, are often conceptualized in terms of localized atomic states such as the famous "$J_{\text{eff}}=1/2$ state". Although, orbital hybridization can strongly modify such states and dramatically change the electronic properties of materials, probing this process is highly challenging. In this work, we directly detect and quantify the formation of dimer orbitals in an iridate material Ba${}_5$AlIr${}_2$O${}_{11}$ using resonant inelastic x-ray scattering (RIXS). Sharp peaks corresponding to the excitations of dimer orbitals are observed and analyzed by a combination of density functional theory (DFT) calculations and theoretical simulations based on a Ir-Ir cluster model. Such partially delocalized dimer states lead to a re-definition of the angular momentum of the electrons and changes in the magnetic and electronic behaviors of the material. We use this to explain the reduction of the observed magnetic moment with respect to prediction based on atomic states. This study opens new directions to study dimerization in a large family of materials including solids, heterostructures, molecules and transient states.

arXiv comment7 pages, 3 figures

References in corpus (46)

• Wannier90: A Tool for Obtaining Maximally-Localised Wannier Functions
• Maximally localized Wannier functions: Theory and applications
• Novel Jeff = 1/2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr2IrO4
• Magnetic Pyrochlore Oxides
• Resonant Inelastic X-ray Scattering Studies of Elementary Excitations
• Kitaev-Heisenberg Model on Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides $A_2$IrO${}_3$
• Mott physics and band topology in materials with strong spin-orbit interaction
• Spin-Liquid State in the S = 1/2 Hyperkagome Antiferromagnet Na4Ir3O8
• Twisted Hubbard Model for Sr2IrO4: Magnetism and Possible High Temperature Superconductivity
• Quantum spin Hall effect in a transition metal oxide Na2IrO3
• Exotic phases induced by strong spin-orbit coupling in ordered double perovskites
• Excitonic Magnetism in Van Vleck-type d^4 Mott Insulators
• Crystal field splitting and correlation effect on the electronic structure of A2IrO3
• Na2IrO3 as a molecular orbital crystal
• Ultrafast energy and momentum resolved dynamics of magnetic correlations in photo-doped Mott insulator Sr${}_2$IrO${}_4$
• The Challenge of Spin-Orbit-Tuned Ground States in Iridates
• Spin-orbit coupling in $d^2$ ordered double perovskites
• Novel magnetism of Ir5+ ions in the double perovskite Sr2YIrO6
• Spin-orbit effects in Na${}_4$Ir${}_3$O${}_8$, a hyper-kagomé lattice antiferromagnet
• Spin excitations in a single La${}_2$CuO${}_4$ layer
• Gapless spin liquids on the three dimensional hyper-kagome lattice of Na${}_4$Ir${}_3$O${}_8$
• Continuous Transition between Antiferromagnetic Insulator and Paramagnetic Metal in the Pyrochlore Iridate Eu2Ir2O7
• Testing the validity of the strong spin-orbit-coupling limit for octahedrally coordinated iridates in a model system Sr${}_3$CuIrO${}_6$
• Covalent bonds against magnetism in transition metal compounds
• Structure and Magnetic Properties of the Pyrochlore Iridate Y2Ir2O7
• All-in all-out magnetic order and propagating spin-waves in Sm2Ir2O7
• Na4Ir3O8 as a 3D spin liquid with fermionic spinons
• Emergent excitation at the magnetic metal-insulator transition in the pyrochlore osmate Cd2Os2O7
• CaIrO3: a Spin-Orbit Mott Insulator Beyond the jeff = 1/2 Ground State
• Determination of Hund's coupling in 5d Oxides using Resonant Inelastic X-ray Scattering
• Tuning Magnetic Coupling in Sr${}_2$IrO${}_4$ Thin Films with Epitaxial Strain
• Origin of the insulating state in honeycomb iridates and rhodates
• Magnetic order and the electronic ground state in the pyrochlore iridate Nd2Ir2O7
• X-ray scattering study of pyrochlore iridates: crystal structure, electronic and magnetic excitations
• Resonant inelastic x-ray incarnation of Young's double-slit experiment
• Persistent low-temperature spin dynamics in the mixed-valence iridate Ba${}_3$InIr${}_2$O${}_9$
• Charge order at the frontier between the molecular and solid states in Ba3NaRu2O9
• Frustrated spin-1/2 molecular magnetism in the mixed-valence antiferromagnets Ba3MRu2O9 (M = In, Y, Lu)
• Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates
• Resonant inelastic x-ray scattering operators for $t_{2g}$ orbital systems
• Covalency-driven collapse of strong spin-orbit coupling in face-sharing iridium octahedra
• Suppression of magnetism in Ba5AlIr2O11: interplay of Hund's coupling, molecular orbitals and spin-orbit interaction
• Evolution of Magnetic Excitations Across the Metal-Insulator Transition in a Pyrochlore Iridate Eu${}_2$Ir${}_2$O${}_7$
• Analysis of resonant inelastic x-ray scattering from Sr${}_2$IrO${}_4$ in an itinerant-electron approach
• Electronic correlations and competing orders in multiorbital dimers: a cluster DMFT study
• Coexisting charge and magnetic orders in the dimer-chain iridate Ba5AlIr2O11

Cited by in corpus (15)

• Hexagonal Perovskites as Quantum Materials
• EDRIXS: An open source toolkit for simulating spectra of resonant inelastic x-ray scattering
• Hopping induced ground-state magnetism in 6H perovskite iridates
• Nearly itinerant electronic groundstate in the intercalated honeycomb iridate Ag${}_3$LiIr${}_2$O${}_6$
• Emergence of spinons in layered trimer iridate Ba4Ir3O10
• Quasimolecular electronic structure of the spin-liquid candidate Ba${}_3$InIr${}_2$O${}_9$
• RIXS interferometry and the role of disorder in the quantum magnet Ba${}_3$Ti${}_{3-x}$Ir${}_x$O${}_9$
• Charge ordering in Ir dimers in the ground state of Ba${}_5$AlIr${}_2$O${}_{11}$
• Spin-orbit excitons and electronic configuration of the $5d^4$ insulator Sr${}_3$Ir${}_2$O${}_7$F${}_2$
• Novel Block Excitonic Condensate at $n=3.5$ in a Spin-Orbit Coupled $t_{2g}$ Multiorbital Hubbard Model
• Interplay of broken symmetry and delocalized excitations in the insulating state of 1$T$-TaS${}_2$
• A Novel ground state in a new dimer iridate Ba13Ir6O30 with Ir6+(5d3) Ions
• Signatures of multiple charge excitations in RIXS spectra of metals
• Novel electronic state of honeycomb iridate Cu${}_2$IrO${}_3$ at high pressure
• Orbital-Selective Spin-Orbit Mott Insulator in Fractional Valence Iridate La${}_3$Ir${}_3$O${}_{11}$