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Register a new userTwo-dimensional ${J}_{rm eff}$ = 1/2 antiferromagnetic insulator unraveled from interlayer exchange coupling in artificial perovskite iridate superlattices
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We report an experimental investigation of the two-dimensional ${J}_{rm eff}$ = 1/2 antiferromagnetic Mott insulator by varying the interlayer exchange coupling in [(SrIrO$_3$)$_1$, (SrTiO$_3$)$_m$] ($m$ = 1, 2 and 3) superlattices. Although all samples exhibited an insulating ground state with long-range magnetic order, temperature-dependent resistivity measurements showed a stronger insulating behavior in the $m$ = 2 and $m$ = 3 samples than the $m$ = 1 sample which displayed a clear kink at the magnetic transition. This difference indicates that the blocking effect of the excessive SrTiO$_3$ layer enhances the effective electron-electron correlation and strengthens the Mott phase. The significant reduction of the Neel temperature from 150 K for $m$ = 1 to 40 K for $m$ = 2 demonstrates that the long-range order stability in the former is boosted by a substantial interlayer exchange coupling. Resonant x-ray magnetic scattering revealed that the interlayer exchange coupling has a switchable sign, depending on the SrTiO$_3$ layer number $m$, for maintaining canting-induced weak ferromagnetism. The nearly unaltered transition temperature between the $m$ = 2 and the $m$ = 3 demonstrated that we have realized a two-dimensional antiferromagnet at finite temperatures with diminishing interlayer exchange coupling.
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We use neutron reflectometry to investigate the interlayer exchange coupling between Ga$_{0.97}$Mn$_{0.03}$As ferromagnetic semiconductor layers separated by non-magnetic Be-doped GaAs spacers. Polarized neutron reflectivity measured below the Curie temperature of Ga$_{0.97}$Mn$_{0.03}$As reveals a characteristic splitting at the wave vector corresponding to twice the multilayer period, indicating that the coupling between the ferromagnetic layers are antiferromagnetic (AFM). When the applied field is increased to above the saturation field, this AFM coupling is suppressed. This behavior is not observed when the spacers are undoped, suggesting that the observed AFM coupling is mediated by charge carriers introduced via Be doping. The behavior of magnetization of the multilayers measured by DC magnetometry is consistent with the neutron reflectometry results.
Heavy transition metal magnets with $J_{rm eff}$ $=$ 1/2 electronic ground states have attracted recent interest due to their penchant for hosting new classes of quantum spin liquids and superconductors. Unfortunately, model systems with ideal $J_{rm eff}$ $=$ 1/2 states are scarce due to the importance of non-cubic local distortions in most candidate materials. In this work, we identify a family of iridium halide systems [i.e. K$_2$IrCl$_6$, K$_2$IrBr$_6$, (NH$_4$)$_2$IrCl$_6$, and Na$_2$IrCl$_6 cdotp $ 6(H$_2$O)] with Ir$^{4+}$ electronic ground states in extremely close proximity to the ideal $J_{rm eff}$ $=$ 1/2 limit, despite a variation in the low-temperature global crystal structures. We also find ordered magnetic ground states for the three anhydrous systems, with single crystal neutron diffraction on K$_2$IrBr$_6$ revealing Type-I antiferromagnetism. This spin configuration is consistent with expectations for significant Kitaev exchange in a face-centered-cubic magnet.
Antiferromagnetic coupling between ferromagnetic layers has been observed for the first time in all-semiconductor superlattice structure EuS/PbS(001), by neutron scattering and magnetization measurements. Spin-dependent superlattice band structure effects are invoked to explain the possible origin and the strength of the observed coupling.
We have performed inelastic neutron scattering (INS) experiments to investigate the magnetic excitations in the weakly distorted face-centered-cubic (fcc) iridate double perovskites La$_2$ZnIrO$_6$ and La$_2$MgIrO$_6$, which are characterized by A-type antiferromagnetic ground states. The powder inelastic neutron scattering data on these geometrically frustrated $j_{rm eff}=1/2$ Mott insulators provide clear evidence for gapped spin wave excitations with very weak dispersion. The INS results and thermodynamic data on these materials can be reproduced by conventional Heisenberg-Ising models with significant uniaxial Ising anisotropy and sizeable second-neighbor ferromagnetic interactions. Such a uniaxial Ising exchange interaction is symmetry-forbidden on the ideal fcc lattice, so that it can only arise from the weak crystal distortions away from the ideal fcc limit. This may suggest that even weak distortions in $j_{rm eff}=1/2$ Mott insulators might lead to strong exchange anisotropies. More tantalizingly, however, we find an alternative viable explanation of the INS results in terms of spin models with a dominant Kitaev interaction. In contrast to the uniaxial Ising exchange, the highly-directional Kitaev interaction is a type of exchange anisotropy which is symmetry-allowed even on the ideal fcc lattice. The Kitaev model has a magnon gap induced by quantum order-by-disorder, while weak anisotropies of the Kitaev couplings generated by the symmetry-lowering due to lattice distortions, can pin the order and enhance the magnon gap. Our findings highlight how even conventional magnetic orders in heavy transition metal oxides may be driven by highly-directional exchange interactions rooted in strong spin-orbit coupling.
The perovskite SrIrO3 is an exotic narrow-band metal owing to a confluence of the strengths of the spin-orbit coupling (SOC) and the electron-electron correlations. It has been proposed that topological and magnetic insulating phases can be achieved by tuning the SOC, Hubbard interactions, and/or lattice symmetry. Here, we report that the substitution of nonmagnetic, isovalent Sn4+ for Ir4+ in the SrIr1-xSnxO3 perovskites synthesized under high pressure leads to a metal-insulator transition to an antiferromagnetic (AF) phase at TN > 225 K. The continuous change of the cell volume as detected by x-ray diffraction and the lamda-shape transition of the specific heat on cooling through TN demonstrate that the metal-insulator transition is of second-order. Neutron powder diffraction results indicate that the Sn substitution enlarges an octahedral-site distortion that reduces the SOC relative to the spin-spin exchange interaction and results in the type-G AF spin ordering below TN. Measurement of high-temperature magnetic susceptibility shows the evolution of magnetic coupling in the paramagnetic phase typical of weak itinerant-electron magnetism in the Sn-substituted samples. A reduced structural symmetry in the magnetically ordered phase leads to an electron gap opening at the Brillouin zone boundary below TN in the same way as proposed by Slater.
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