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We report the observation of an electronic reconstruction in dimensionally controlled ruthenate heterostructures synthesized by pulsed laser deposition. High structural and electronic quality of superlattices comprised of a single SrRuO3 layer inter-spaced with varying thicknesses of insulating SrTiO3 layers was verified by reflection high energy electron diffraction, atomic force microscopy, x-ray diffraction, reciprocal space mapping, and x-ray absorption spectroscopy. X-ray absorption spectroscopy evidences a confinement-driven evolution of the Ru electronic configuration from the d5L to the d4 state. Significant increases of the spin-orbit coupling are observed in connection with the configuration changes supporting recent works identifying large enhancement of the magnetic anisotropy. The growth of high quality two-dimensional confined ruthenate layers under precisely controlled environments highlights the potential to directly manipulate interlayer coupling and selectively perturb the electronic state in ruthenates in analogy to superconducting Sr2RuO4. 

Abstract The search for Kitaev’s quantum spin liquid in real materials has recently expanded with the prediction that honeycomb lattices of divalent, high-spin cobalt ions could host the dominant bond-dependent exchange interactions required to stabilize the elusive entangled quantum state. The layered honeycomb Na₃Co₂SbO₆has been singled out as a leading candidate provided that the trigonal crystal field acting on Co 3dorbitals, which enhances non-Kitaev exchange interactions between$${J}_{{{\rm{eff}}}}=\frac{1}{2}$$ $J_{\mathrm{eff}}=\frac{1}{2}$ spin-orbital pseudospins, is reduced. Here we show that applied pressure leads to anisotropic compression of the layered structure, significantly reducing the trigonal distortion of CoO₆octahedra. Ferromagnetic correlations between pseudospins are enhanced in the spin-polarized (3 Tesla) phase up to about 60 GPa. Higher pressures drive a high-spin to low-spin transition destroying the$${J}_{{{\rm{eff}}}}=\frac{1}{2}$$ $J_{\mathrm{eff}}=\frac{1}{2}$ moments required to map the spin Hamiltonian into Kitaev’s model. The spin transition strongly suppresses the low-temperature magnetic susceptibility and appears to stabilize a paramagnetic phase driven by frustration. The possible emergence of frustrated magnetism of localized$$S=\frac{1}{2}$$ $S=\frac{1}{2}$ moments opens the door for exploration of novel magnetic quantum states in compressed honeycomb lattices of divalent cobaltates. 

Abstract Understanding the interplay between the inherent disorder and the correlated fluctuating-spin ground state is a key element in the search for quantum spin liquids. H₃LiIr₂O₆is considered to be a spin liquid that is proximate to the Kitaev-limit quantum spin liquid. Its ground state shows no magnetic order or spin freezing as expected for the spin liquid state. However, hydrogen zero-point motion and stacking faults are known to be present. The resulting bond disorder has been invoked to explain the existence of unexpected low-energy spin excitations, although data interpretation remains challenging. Here, we use resonant X-ray spectroscopies to map the collective excitations in H₃LiIr₂O₆and characterize its magnetic state. In the low-temperature correlated state, we reveal a broad bandwidth of magnetic excitations. The central energy and the high-energy tail of the continuum are consistent with expectations for dominant ferromagnetic Kitaev interactions between dynamically fluctuating spins. Furthermore, the absence of a momentum dependence to these excitations are consistent with disorder-induced broken translational invariance. Our low-energy data and the energy and width of the crystal field excitations support an interpretation of H₃LiIr₂O₆as a disordered topological spin liquid in close proximity to bond-disordered versions of the Kitaev quantum spin liquid. 

The recent prediction that honeycomb lattices of Co2+ (3d7) ions could host dominant Kitaev interactions provides an exciting direction for exploration of new routes to stabilizing Kitaev’s quantum spin liquid in real materials. Na3Co2SbO6 has been singled out as a potential material candidate provided that spin and orbital moments couple into a Jeff = 1/2 ground state, and that the relative strength of trigonal crystal field and spin-orbit coupling acting on Co ions can be tailored. Using x-ray linear dichroism (XLD) and x-ray magnetic circular dichroism (XMCD) experiments, alongside configuration interaction calculations, we confirm the counterintuitive positive sign of the trigonal crystal field acting on Co2+ ions and test the validity of the Jeff = 1/2 description of the electronic ground state. The results lend experimental support to recent theoretical predictions that a compression (elongation) of CoO6 octahedra along (perpendicular to) the trigonal axis would drive this cobaltate toward the Kitaev limit, assuming the Jeff = 1/2 character of the electronic ground state is preserved. 

Abstract Excitonic insulators are usually considered to form via the condensation of a soft charge mode of bound electron-hole pairs. This, however, presumes that the soft exciton is of spin-singlet character. Early theoretical considerations have also predicted a very distinct scenario, in which the condensation of magnetic excitons results in an antiferromagnetic excitonic insulator state. Here we report resonant inelastic x-ray scattering (RIXS) measurements of Sr 3 Ir 2 O 7 . By isolating the longitudinal component of the spectra, we identify a magnetic mode that is well-defined at the magnetic and structural Brillouin zone centers, but which merges with the electronic continuum in between these high symmetry points and which decays upon heating concurrent with a decrease in the material’s resistivity. We show that a bilayer Hubbard model, in which electron-hole pairs are bound by exchange interactions, consistently explains all the electronic and magnetic properties of Sr 3 Ir 2 O 7 indicating that this material is a realization of the long-predicted antiferromagnetic excitonic insulator phase.