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Register a new userMagnetic order and spin-orbit coupled Mott state in double perovskite (La$_{1-x}$Sr$_x$)$_2$CuIrO$_6$
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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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The double-perovskite A$_2$BBO$_6$ with heavy transition metal ions on the ordered B sites is an important family of compounds to study the interplay between electron correlation and spin-orbit coupling (SOC). Here we prepared high-quality Sr$_2$MgReO$_6$ powder and single-crystal samples and performed non-resonant and resonant synchrotron x-ray diffraction experiments to investigate its magnetic ground state. By combining the magnetic susceptibility and heat capacity measurements, we conclude that Sr$_2$MgReO$_6$ exhibits a layered antiferromagnetic (AF) order at temperatures below $sim$ 55 K with a propagation vector q = (001), which contrasts the previously suspected spin glass state. Our works clarify the magnetic order in Sr$_2$MgReO$_6$ and demonstrate it as a candidate system to look for magnetic octupolar orders and exotic spin dynamics.
An anapole state that breaks inversion and time reversal symmetries with preserving translation symmetry of underlying lattice has aroused great interest as a new quantum state, but only a few candidate materials have been reported. Recently, in a spin-orbit coupled Mott insulator SIR, the emergence of a possible hidden order phase with broken inversion symmetry has been suggested at $T_{Omega}$ above the N{e}el temperature by optical second harmonic generation measurements. Moreover, polarized neutron diffraction measurements revealed the broken time reversal symmetry below $T_{Omega}$, which was supported by subsequent muon spin relaxation experiments. However, the nature of this mysterious phase remains largely elusive. Here, we investigate the hidden order phase through the combined measurements of the in-plane magnetic anisotropy with exceptionally high-precision magnetic torque and the nematic susceptibility with elastoresistance. A distinct two-fold in-plane magnetic anisotropy along the [110] Ir-O-Ir bond direction sets in below $sim T_{Omega}$, providing thermodynamic evidence for a nematic phase transition with broken $C_4$ rotational symmetry. However, in contrast to the even-parity nematic transition reported in other correlated electron systems, the nematic susceptibility exhibits no divergent behavior towards $T_{Omega}$. These results provide bulk evidence for an odd-parity order parameter with broken rotational symmetry in the hidden order state. We discuss the hidden order in terms of an anapole state, in which polar toroidal moment is induced by two current loops in each IrO$_6$ octahedron of opposite chirality. Contrary to the simplest loop-current pattern previously suggested, the present results are consistent with a pattern in which the intra-unit cell loop-current flows along only one of the diagonal directions in the IrO$_4$ square.
We have studied Ir spin and orbital magnetic moments in the double perovskites La$_{2-x}$Sr$_x$CoIrO$_6$ by x-ray magnetic circular dichroism. In La$_2$CoIrO$_6$, Ir$^{4+}$ couples antiferromagnetically to the weak ferromagnetic moment of the canted Co$^{2+}$ sublattice and shows an unusually large negative total magnetic moment (-0.38,$mu_{text B}$/f.u.) combined with strong spin-orbit interaction. In contrast, in Sr$_2$CoIrO$_6$, Ir$^{5+}$ has a paramagnetic moment with almost no orbital contribution. A simple kinetic-energy-driven mechanism including spin-orbit coupling explains why Ir is susceptible to the induction of substantial magnetic moments in the double perovskite structure.
We report the results of ac and dc magnetization (M) and heat-capacity (C) measurements on the solid solution, Sr$_3$Cu$_{1-x}$Zn$_x$IrO$_6$. While the Zn end member is known to form in a rhombohedral pseudo one-dimensional K$_4$CdCl$_6$ structure with an antiferromagnetic ordering temperature of (T$_N$ =) 19 K, the Cu end member has been reported to form in a monoclinically distorted form with a Curie temperature of (T$_C$ =) 19 K. The magnetism of the Zn compound is found to be robust to synthetic conditions and is broadly consistent with the behavior known in the literature. However, we find a lower magnetic ordering temperature (T$_o$) for our Cu compound (~ 13 K), thereby suggesting that T$_o$ is sensitive to synthetic conditions. The Cu sample appears to be in a spin-glass-like state at low temperatures, judged by a frequency dependence of ac magnetic susceptibility and a broadening of the C anomaly at the onset of magnetic ordering, in sharp contrast to earlier proposals. Small applications of magnetic field, however, drive this system to ferromagnetism as inferred from the M data. Small substitutions for Cu/Zn (x = 0.75 or 0.25) significantly depress magnetic ordering; in other words, T$_o$ varies non-monotonically with x (T$_o$ ~ 6, 3 and 4 K for x = 0.25, 0.5, and 0.67 respectively). The plot of inverse susceptibility versus temperature is non-linear in the paramagnetic state as if correlations within (or among) the magnetic chains continuously vary with temperature. The results establish
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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