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Register a new userOptical Signature of a Crossover from Mott- to Slater-type Gap in Sr$_2$Ir$_{1-x}$Rh$_{x}$O$_{4}$
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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.
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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.
Hidden magnetic order of Sr$_2$Ir$_{1-x}$Rh$_x$O$_4$, $x = 0.05$ and 0.1, has been studied using muon spin relaxation spectroscopy. In zero applied field and weak longitudinal fields ($mu_0H_L lesssim 2$~mT), muon spin relaxation data can be well described by exponentially-damped static Lorentzian Kubo-Toyabe functions, indicating that static and dynamic local fields coexist at each muon site. For $mu_0H_L gtrsim 2$~mT, the static rate is completely decoupled, and the exponential decay is due to dynamic spin fluctuations. In both zero field and $mu_0H_L = 1$--2~mT, the temperature dependencies of the exponential muon spin relaxation rate exhibit maxima at 215~K for $x = 0.05$ and 175~K for $x = 0.1$, suggesting critical slowing down of electronic spin fluctuations. The field dependencies of the dynamic spin fluctuation rates can be well described by the Redfield relation. The correlation time of this electronic spin fluctuation is in the range of~2--5~ns for Sr$_2$Ir$_{0.9}$Rh$_{0.1}$O$_4$, and shorter than 2~ns for Sr$_2$Ir$_{0.95}$Rh$_{0.05}$O$_4$. The rms fluctuating field is on the order of 1 mT, which is consistent with the polarized neutron diffraction cross-section.
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.
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.
Layered 5$d$ transition iridium oxides, Sr$_2$(Ir,Rh)O$_4$, are described as unconventional Mott insulators with strong spin-orbit coupling. The undoped compound, Sr$_2$IrO$_4$, is a nearly ideal two-dimensional pseudospin-$1/2$ Heisenberg antiferromagnet, similarly to the insulating parent compound of high-temperature superconducting copper oxides. Using polarized neutron diffraction, we here report a hidden magnetic order in pure and doped Sr$_2$(Ir,Rh)O$_4$, distinct from the usual antiferromagnetic pseudo-spin ordering. We find that time-reversal symmetry is broken while the lattice translation invariance is preserved in the hidden order phase. The onset temperature matches that of the odd-parity hidden order recently highlighted using optical second harmonic generation experiments. The novel magnetic order and broken symmetries can be explained by the loop-current model, previously predicted for the copper oxide superconductors.
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