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Register a new userBond Directional Anapole Order in a Spin-Orbit Coupled Mott Insulator Sr$_2$(Ir$_{1-x}$Rh$_x$)O$_{4}$
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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.
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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.
With optical spectroscopy we provide evidence that the insulator-metal transition in Sr$_2$Ir$_{1-x}$Rh$_{x}$O$_{4}$ occurs close to a crossover from the Mott- to the Slater-type. The Mott-gap at $x = 0$ persists to high temperature and evolves without an anomaly across the N{e}el temperature, $T_N$. Upon Rh-doping, it collapses rather rapidly and vanishes around $x = 0.055$. Notably, just as the Mott-gap vanishes yet another gap appears that is of the Slater-type and develops right below $T_N$. This Slater-gap is only partial and is accompanied by a reduced scattering rate of the remaining free carriers, similar as in the parent compounds of the iron arsenide superconductors.
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.
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.
It was found that, although isovalent, Rh substituted for Ir in Sr$_2$IrO$_4$ may trap one electron inducing effective hole doping of Ir sites. Transport and thermoelectric measurements on Sr$_2$Ir$_{1-x}$Rh$_x$O$_4$ single crystals presented here reveal the existence of an electron-like contribution to transport, in addition to the hole-doped one. As no electron band shows up in ARPES measurements, this points to the possibility that this hidden electron may delocalize in disordered clusters.
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