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Register a new userDoping induced Mott collapse and the density wave instabilities in (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$
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The path from a Mott insulating phase to high temperature superconductivity encounters a rich set of unconventional phenomena involving the insulator-to-metal transition (IMT) such as emergent electronic orders and pseudogaps that ultimately affect the condensation of Cooper pairs. A huge hindrance to understanding the origin of these phenomena in the curates is the difficulty in accessing doping levels near the parent state. Recently, the J$_{eff}$=1/2 Mott state of the perovskite strontium iridates has revealed intriguing parallels to the cuprates, with the advantage that it provides unique access to the Mott transition. Here, we exploit this accessibility to study the IMT and the possible nearby electronic orders in the electron-doped bilayer iridate (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$. Using spectroscopic imaging scanning tunneling microscopy, we image the La dopants in the top as well as the interlayer SrO planes. Surprisingly, we find a disproportionate distribution of La in these layers with the interlayer La being primarily responsible for the IMT, thereby revealing the distinct site-dependent effects of dopants on the electronic properties of bilayer systems. Furthermore, we discover the coexistence of two electronic orders generated by electron doping: a unidirectional electronic order with a concomitant structural distortion; and local resonant states forming a checkerboard-like pattern trapped by La. This provides evidence that multiple charge orders may exist simultaneously in Mott systems, even with only one band crossing the Fermi energy.
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We use resonant elastic and inelastic X-ray scattering at the Ir-$L_3$ edge to study the doping-dependent magnetic order, magnetic excitations and spin-orbit excitons in the electron-doped bilayer iridate (Sr$_{1-x}$La$_{x}$)$_3$Ir$_2$O$_7$ ($0 leq x leq 0.065$). With increasing doping $x$, the three-dimensional long range antiferromagnetic order is gradually suppressed and evolves into a three-dimensional short range order from $x = 0$ to $0.05$, followed by a transition to two-dimensional short range order between $x = 0.05$ and $0.065$. Following the evolution of the antiferromagnetic order, the magnetic excitations undergo damping, anisotropic softening and gap collapse, accompanied by weakly doping-dependent spin-orbit excitons. Therefore, we conclude that electron doping suppresses the magnetic anisotropy and interlayer couplings and drives (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$ into a correlated metallic state hosting two-dimensional short range antiferromagnetic order and strong antiferromagnetic fluctuations of $J_{text{eff}} = frac{1}{2}$ moments, with the magnon gap strongly suppressed.
X-ray magnetic critical scattering measurements and specific heat measurements were performed on the perovskite iridate Sr$_3$Ir$_2$O$_7$. We find that the magnetic interactions close to the N{e}el temperature $T_N$ = 283.4(2) K are three-dimensional. This contrasts with previous studies which suggest two-dimensional behaviour like Sr$_2$IrO$_4$. Violation of the Harris criterion ($d u>2$) means that weak disorder becomes relevant. This leads a rounding of the antiferromagnetic phase transition at $T_N$, and modifies the critical exponents relative to the clean system. Specifically, we determine that the critical behaviour of Sr$_3$Ir$_2$O$_7$ is representative of the diluted 3D Ising universality class.
Oxides containing iridium ions display a range of magnetic and conducting properties that depend on the delicate balance between interactions and are controlled, at least in part, by the details of the crystal architecture. We have used muon-spin rotation ($mu$SR) to study the local field in four iridium oxides, Ca$_4$IrO$_6$, Ca$_5$Ir$_3$O$_{12}$, Sr$_3$Ir$_2$O$_7$ and Sr$_2$IrO$_4$, which show contrasting behavior. Our $mu$SR data on Ca$_4$IrO$_6$ and Ca$_5$Ir$_3$O$_{12}$ are consistent with conventional antiferromagnetism where quasistatic magnetic order develops below $T_{rm N}=13.85(6)$ K and 7.84(7) K respectively. A lower internal field is observed for Ca$_5$Ir$_3$O$_{12}$, as compared to Ca$_4$IrO$_6$ reflecting the presence of both Ir$^{4+}$ and Ir$^{5+}$ ions, resulting in a more magnetically dilute structure. Muon precession is only observed over a restricted range of temperature in Sr$_3$Ir$_2$O$_7$, while the Mott insulator Sr$_2$IrO$_4$ displays more complex behavior, with the $mu$SR signal containing a single, well-resolved precession signal below $T_{rm N}=230$,K, which splits into two precession signals at low temperature following a reorientation of the spins in the ordered state.
The topochemical transformation of single crystals of Sr$_3$Ir$_2$O$_7$ into Sr$_3$Ir$_2$O$_7$F$_2$ is reported via fluorine insertion. Characterization of the newly formed Sr$_3$Ir$_2$O$_7$F$_2$ phase shows a nearly complete oxidation of Ir$^{4+}$ cations into Ir$^{5+}$ that in turn drives the system from an antiferromagnetic Mott insulator with a half-filled J$_{eff}=1/2$ band into a nonmagnetic $J=0$ band insulator. First principles calculations reveal a remarkably flat insertion energy that locally drives the fluorination process to completion. Band structure calculations support the formation of a band insulator whose charge gap relies on the strong spin-orbit coupling inherent to the Ir metal ions of this compound.
Double-perovskite oxides that contain both 3d and 5d transition metal elements have attracted growing interest as they provide a model system to study the interplay of strong electron interaction and large spin-orbit coupling (SOC). Here, we report on experimental and theoretical studies of the magnetic and electronic properties of double-perovskites (La$_{1-x}$Sr$_x$)$_2$CuIrO$_6$ ($x$ = 0.0, 0.1, 0.2, and 0.3). The undoped La$_2$CuIrO$_6$ undergoes a magnetic phase transition from paramagnetism to antiferromagnetism at T$_N$ $sim$ 74 K and exhibits a weak ferromagnetic behavior below $T_C$ $sim$ 52 K. Two-dimensional magnetism that was observed in many other Cu-based double-perovskites is absent in our samples, which may be due to the existence of weak Cu-Ir exchange interaction. First-principle density-functional theory (DFT) calculations show canted antiferromagnetic (AFM) order in both Cu$^{2+}$ and Ir$^{4+}$ sublattices, which gives rise to weak ferromagnetism. Electronic structure calculations suggest that La$_2$CuIrO$_6$ is an SOC-driven Mott insulator with an energy gap of $sim$ 0.3 eV. Sr-doping decreases the magnetic ordering temperatures ($T_N$ and $T_C$) and suppresses the electrical resistivity. The high temperatures resistivity can be fitted using a variable-range-hopping model, consistent with the existence of disorders in these double-pervoskite compounds.
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