Electron and hole doping in the relativistic Mott insulator Sr${}_2$IrO${}_4$: a first-principles study using band unfolding technique

Abstract

We study the effects of dilute La and Rh doping on the electronic structure of the relativistic Mott insulator Sr${}_2$IrO${}_4$ using fully relativistic and magnetically non-collinear density functional theory with the inclusion of an on-site Hubbard $U$. To model doping effects, we have adopted the supercell approach that allows for a realistic treatment of structural relaxations and electronic effects beyond a purely rigid band approach. By means of the band unfolding technique we have computed the spectral function and constructed the effective band structure and Fermi surface (FS), which are readily comparable with available experimental data. Our calculations clearly indicate that La and Rh doping can be interpreted as effective electron and (fractional) hole doping, respectively. In Sr${}_{2-x}$La${}_x$IrO${}_4$ the IMT is accompanied by a moderate renormalization of the electronic correlation substantiated by a reduction of the effective on-site Coulomb repulsion $U-J$ from 1.6 eV ($x=0$) to 1.4 eV (metallic regime $x=12.5\%$). The progressive closing of the relativistic Mott gap leads to the emergence of connected elliptical electron pockets at ($\pi$/2,$\pi$/2) and less intense features at $X$ in the FS. The substitution of Ir with the nominally isovalent Rh is accompanied by a substantial hole transfer from the Rh site to the nearest neighbor Ir sites. This shifts down the chemical potential, creates almost circular disconnected hole pockets in the FS and establishes the emergence of a two-dimensional metallic state formed by conducting Rh-planes intercalated by insulating Ir-planes. Finally, our data indicate that hole doping causes a flipping of the in-plane net ferromagnetic moment in the Rh plane and induces a magnetic transition from the AF-I to the AF-II ordering.

References in corpus (19)

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• Twisted Hubbard Model for Sr2IrO4: Magnetism and Possible High Temperature Superconductivity
• Fermi Arcs in a Doped Pseudospin-1/2 Heisenberg Antiferromagnet
• Observation of a $d$-wave gap in electron-doped Sr${}_2$IrO${}_4$
• Monte Carlo study of an unconventional superconducting phase in Ir-oxide J_{eff}=1/2 Mott insulators induced by carrier doping
• Collapse of the Mott gap and emergence of a nodal liquid in lightly doped Sr${}_2$IrO${}_4$
• Signature of high temperature superconductivity in electron doped Sr2IrO4
• Excitonic quasiparticles in a spin-orbit Mott insulator
• Dimensionality Driven Spin-Flop Transition in Layered Iridates
• Spin-orbit tuned metal-insulator transitions in single-crystal Sr2Ir1-xRhxO4 (0\leqx\leq1)
• The influence of electron-doping on the ground state of (Sr{1-x}La{x})2IrO4
• Electronic structures of layered perovskite Sr2MO4 (M=Ru, Rh, and Ir)
• Anisotropic Magnetic Couplings and Structure-Driven Canted to Collinear Transitions in Spin-orbit Coupled Sr2IrO4
• Transfer of spectral weight across the gap of Sr2IrO4 induced by La doping
• Structure symmetry determination and magnetic evolution in $\mathrm{S}{\mathrm{r}}_2\mathrm{I}{\mathrm{r}}_{1-\mathrm{x}}\mathrm{R}{\mathrm{h}}_{\mathrm{x}}{\mathrm{O}}_4$
• Evolution of competing magnetic order in the Jeff=1/2 insulating state of Sr2Ir1-xRuxO4
• Unveiling the Origin of the Basal-plane Antiferromagnetism in the Jeff=1/2 Mott Insulator Ba2IrO4: A Density Functional and Model Hamiltonian Study
• Doping-dependent bandwidth renormalization and spin-orbit coupling in (Sr${}_{1-x}$La${}_x$)${}_2$RhO${}_4$

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• The Jeff=1/2 antiferromagnet Sr2IrO4: A golden avenue toward new physics and functions
• Correlation effects and hidden spin-orbit entangled electronic order in parent and electron-doped iridates Sr${}_2$IrO${}_4$
• Conditions for electronic hybridization between transition-metal dichalcogenide monolayers and physisorbed carbon-conjugated molecules
• Electronic state unfolding for plane waves: energy bands, Fermi surfaces and spectral functions
• Formation of an incoherent metallic state in Rh-doped Sr${}_2$IrO${}_4$
• Comparative ab initio study of the structural, electronic, magnetic, and dynamical properties of LiOsO${}_3$ and NaOsO${}_3$
• Evolution of remnant Fermi surface state in lightly-doped correlated spin-orbit insulator Sr${}_{2-x}$La${}_x$IrO${}_4$
• Magnetic properties of bilayer Sr${}_3$Ir${}_2$O${}_7$: role of epitaxial strain and oxygen vacancies
• Non-local Coulomb correlations in pure and electron-doped ${\mathrm{Sr}}_2{\mathrm{IrO}}_4$: spectral functions, Fermi surface and pseudogap-like spectral weight distributions from oriented cluster dynamical mean field theory
• Persistent large anisotropic magnetoresistance and insulator to metal transition in spin-orbit coupled antiferromagnets Sr2(Ir1-xGax)O4
• Two-dimensional Peierls instability via zone boundary Dirac line nodes in layered perovskite oxides
• Origin of the different electronic structure of Rh- and Ru-doped Sr2IrO4
• Tuning Dirac nodes with correlated d-electrons in BaCo_{1-x}Ni_{x}S_{2}
• Nonsymmorphic Dirac semimetal and carrier dynamics in doped spin-orbit-coupled Mott insulator Sr${}_2$IrO${}_4$
• Doping-induced insulator-metal transition in the Lifshitz magnetic insulator NaOsO3
• Low-energy electrodynamics of Dirac semimetal phases in the doped Mott insulator Sr${}_2$IrO${}_4$
• The "dark phase'' in Sr${}_2$Ir${}_{1-x}$Rh${}_x$O${}_4$ revealed by Seebeck and Hall measurements