Topotactic transformation of single crystals: From perovskite to infinite-layer nickelates.

Topotactic transformations between related crystal structures are a powerful emerging route for the synthesis of novel quantum materials. Whereas most such "soft chemistry" experiments have been carried out on polycrystalline powders or thin films, the topotactic modification of single crystals, the gold standard for physical property measurements on quantum materials, has been studied only sparsely. Here, we report the topotactic reduction of La1−xCaxNiO3 single crystals to La1−xCaxNiO2+δ using CaH2 as the reducing agent. The transformation from the three-dimensional perovskite to the quasi­two-dimensional infinite-layer phase was thoroughly characterized by x-ray diffraction, electron microscopy, Raman spectroscopy, magnetometry, and electrical transport measurements. Our work demonstrates that the infinite-layer structure can be realized as a bulk phase in crystals with micrometer-sized single domains. The electronic properties of these specimens resemble those of epitaxial thin films rather than powders with similar compositions.

Strain and vector magnetic field tuning of the anomalous phase in Sr3Ru2O7.

A major area of interest in condensed matter physics is the way electrons in correlated electron materials can self-organize into ordered states, and a particularly intriguing possibility is that they spontaneously choose a preferred direction of conduction. The correlated electron metal Sr3Ru2O7 has an anomalous phase at low temperatures that features strong susceptibility toward anisotropic transport. This susceptibility has been thought to indicate a spontaneous anisotropy, that is, electronic order that spontaneously breaks the point-group symmetry of the lattice, allowing weak external stimuli to select the orientation of the anisotropy. We investigate further by studying the response of Sr3Ru2O7 in the region of phase formation to two fields that lift the native tetragonal symmetry of the lattice: in-plane magnetic field and orthorhombic lattice distortion through uniaxial pressure. The response to uniaxial pressure is surprisingly strong: Compressing the lattice by ~0.1% induces an approximately 100% transport anisotropy. However, neither the in-plane field nor the pressure phase diagrams are qualitatively consistent with spontaneous symmetry reduction. Instead, both are consistent with a multicomponent order parameter that is likely to preserve the point-group symmetry of the lattice, but is highly susceptible to perturbation.

Persistent Paramagnons Deep in the Metallic Phase of Sr_{2-x}La_{x}IrO_{4}.

We have studied the magnetic excitations of electron-doped Sr_{2-x}La_{x}IrO_{4} (0≤x≤0.10) using resonant inelastic x-ray scattering at the Ir L_{3} edge. The long-range magnetic order is rapidly lost with increasing x, but two-dimensional short-range order (SRO) and dispersive magnon excitations with nearly undiminished spectral weight persist well into the metallic part of the phase diagram. The magnons in the SRO phase are heavily damped and exhibit anisotropic softening. Their dispersions are well described by a pseudospin-1/2 Heisenberg model with exchange interactions whose spatial range increases with doping. We also find a doping-independent high-energy magnetic continuum, which is not described by this model. The spin-orbit excitons arising from the pseudospin-3/2 manifold of the Ir ions broaden substantially in the SRO phase, but remain largely separated from the low-energy magnons. Pseudospin-1/2 models are therefore a good starting point for the theoretical description of the low-energy magnetic dynamics of doped iridates.

Strong increase of T(c) of Sr2RuO4 under both tensile and compressive strain.

A sensitive probe of unconventional order is its response to a symmetry-breaking field. To probe the proposed p(x) ± ip(y) topological superconducting state of Sr2RuO4, we have constructed an apparatus capable of applying both compressive and tensile strains of up to 0.23%. Strains applied along ⟨100⟩ crystallographic directions yield a strong, strain-symmetric increase in the superconducting transition temperature T(c). ⟨110⟩ strains give a much weaker, mostly antisymmetric response. As well as advancing the understanding of the superconductivity of Sr2RuO4, our technique has potential applicability to a wide range of problems in solid-state physics.