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Register a new userDetection of multipolar orders in the spin-orbit-entangled 5d Mott insulator Ba2MgReO6
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In electronic solids with strong spin-orbit interactions (SOIs), the spin and orbital degrees of freedom of an electron are quantum mechanically entangled, which may result in an exotic multipolar order instead of a conventional dipolar order such as a magnetic order. Such a higher-degree order is called hidden order because of difficulties in experimental detection. Moreover, the number of candidate compounds is limited, especially rare in d electron systems, in which an interplay between SOIs and Coulomb interactions is expected to cause rich physics. Here, we employ state-of-the-art synchrotron X-ray diffraction techniques on a high-quality single crystal to probe subtle symmetry breaking induced by a multipolar order. We unequivocally demonstrate that the double-perovskite Ba2MgReO6 exhibits successive transitions to quadrupolar and then dipolar orders upon cooling, which is consistent with a theory considering SOIs. Our findings are a significant step towards understanding the intriguing physics of multipoles realized by spin-orbit-entangled 5d electrons.
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The intertwined charge, spin, orbital, and lattice degrees of freedom could endow 5d compounds with exotic properties. Current interest is focused on electromagnetic interactions in these materials, whereas the important role of lattice geometry remains to be fully recognized. For this sake, we investigate pressure-induced phase transitions in the spin-orbit Mott insulator Sr3Ir2O7 with Raman, electrical resistance, and x-ray diffraction measurements. We reveal an interesting magnetic transition coinciding with a structural transition at 14.4 GPa, but without a concurrent insulator-metal transition. The conventional correlation between magnetic and Mott insulating states is thereby absent. The observed softening of the one-magnon mode can be explained by a reduced tetragonal distortion, while the actual magnetic transition is associated with tilting of the IrO6 octahedra. This work highlights the critical role of lattice frustration in determining the high-pressure phases of Sr3Ir2O7. The ability to control electromagnetic properties via manipulating the crystal structure with pressure promises a new way to explore new quantum states in spin-orbit Mott insulators.
Using ab initio calculations, we have investigated an insulating tetragonally distorted perovskite BaCrO$_3$ with a formal $3d^2$ configuration, the volume of which is apparently substantially enhanced by a strain due to SrTiO$_3$ substrate. Inclusion of both correlation and spin-orbit coupling (SOC) effects leads to a metal-insulator transition and in-plane zigzag orbital-ordering (OO) of alternating singly filled $d_{xz}+id_{yz}$ and $d_{xz}-id_{yz}$ orbitals, which results in a large orbital moment $M_L$ ~ -0.78 $mu_B$ antialigned to the spin moment $M_S$ ~ $2|M_L|$ in Cr ions. Remarkably, this ordering also induces a considerable $M_L$ for apical oxygens. Our findings show metal-insulator and OO transitions, driven by an interplay among strain, correlation, and SOC, which is uncommon in 3d systems.
Correlated oxides can exhibit complex magnetic patterns, characterized by domains with vastly different size, shape and magnetic moment spanning the material. Understanding how magnetic domains form in the presence of chemical disorder and their robustness to temperature variations has been of particular interest, but atomic-scale insight into this problem has been limited. We use spin-polarized scanning tunneling microscopy to image the evolution of spin-resolved modulations originating from antiferromagnetic (AF) ordering in a spin-orbit Mott insulator Sr3Ir2O7 as a function of chemical composition and temperature. We find that replacing only several percent of La for Sr leaves behind nanometer-scale AF puddles clustering away from La substitutions preferentially located in the middle SrO layer within the unit cell. Thermal erasure and re-entry into the low-temperature ground state leads to a spatial reorganization of the AF modulations, indicating multiple stable AF configurations at low temperature. Interestingly, regardless of this rearrangement, the AF puddles maintain scale-invariant fractal geometry in each configuration. Our experiments reveal spatial fluctuations of the AF order in electron doped Sr3Ir2O7, and shed light on its sensitivity to different types of atomic-scale disorder.
Lacunar spinel GaTa$_4$Se$_8$ is a unique example of spin-orbit coupled Mott insulator described by molecular $j_{text{eff}}!=!3/2$ states. It becomes superconducting at T$_c$=5.8K under pressure without doping. In this work, we show, this pressure-induced superconductivity is a realization of a new type topological phase characterized by spin-2 Cooper pairs. Starting from first-principles density functional calculations and random phase approximation, we construct the microscopic model and perform the detailed analysis. Applying pressure is found to trigger the virtual interband tunneling processes assisted by strong Hund coupling, thereby stabilizing a particular $d$-wave quintet channel. Furthermore, we show that its Bogoliubov quasiparticles and their surface states exhibit novel topological nature. To verify our theory, we propose unique experimental signatures that can be measured by Josephson junction transport and scanning tunneling microscope. Our findings open up new directions searching for exotic superconductivity in spin-orbit coupled materials.
We investigate topological transport in a spin-orbit coupled bosonic Mott insulator. We show that interactions can lead to anomalous quasi-particle dynamics even when the spin-orbit coupling is abelian. To illustrate the latter, we consider the spin-orbit coupling realized in the experiment of Lin textit{et al}. [Nature (London) textbf{471}, 83 (2011)]. For this spin-orbit coupling, we compute the quasiparticle dispersions and spectral weights, the interaction-induced momentum space Berry curvature, and the momentum space distribution of spin density, and propose experimental signatures. Furthermore, we find that in our approximation for the single-particle propagator, the ground state can in principle support an integer Hall conductivity if the sum of the Chern numbers of the hole bands is nonzero.
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