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

Abstract

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 proven remarkably difficult. Here, we report the topotactic reduction of La${}_{1-x}$Ca${}_x$NiO${}_3$ single-crystals to La${}_{1-x}$Ca${}_x$NiO${}_{2+\delta }$ using CaH${}_2$ as the reducing agent. The transformation from the three-dimensional perovskite to the quasi-two-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.

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• Short-range magnetic interactions and spin-glass behavior in the quasi-2D nickelate Pr4Ni3O8
• High pO2 Floating Zone Crystal Growth of the Perovskite Nickelate PrNiO3
• Magnetic excitations in infinite-layer nickelates

Cited by in corpus (29)

• Superconductivity in infinite-layer nickelate La${}_{1-x}$Ca${}_x$NiO${}_2$ thin films
• Superconductivity in infinite-layer nickelates
• Reconstructing the polar interface of infinite-layer nickelate thin films
• Magnetic correlations in infinite-layer nickelates: an experimental and theoretical multi-method study
• Dynamical Mean Field Studies of Infinite Layer Nickelates: Physics Results and Methodological Implications
• Infinite-layer nickelate superconductors: A current experimental perspective of the crystal and electronic structures
• Limits to the strain engineering of layered square-planar nickelate thin films
• Synthesis and physical properties of LaNiO${}_2$ crystals
• Geometric effects in the infinite-layer nickelates
• Investigation of hydrogen incorporations in bulk infinite-layer nickelates
• On the origin of topotactic reduction effect for superconductivity in infinite-layer nickelates
• Synthesis of thin film infinite-layer nickelates by atomic hydrogen reduction: clarifying the role of the capping layer
• Dynamical structural instability and its implication on the physical properties of infinite-layer nickelates
• Emergent flat-band physics in $d^{9-\delta }$ multilayer nickelates
• Phase formation in hole- and electron-doped rare-earth nickelate single crystals
• Synthesis and Properties of La${}_{1-x}$Sr${}_x$NiO${}_3$ and La${}_{1-x}$Sr${}_x$NiO${}_2$
• Structural instabilities of infinite-layer nickelates from first-principles simulations
• Signature of superconductivity in pressurized La4Ni3O10-x single crystals grown at ambient pressure
• Topotactically induced oxygen vacancy order in nickelate single crystals
• Investigation of spin excitations and charge order in bulk crystals of the infinite-layer nickelate LaNiO${}_2$
• Unraveling p-type and n-type interfaces in Superconducting Infinite-Layer Nickelate thin films
• Possible structural quantum criticality tuned by rare-earth ion substitution in infinite-layer nickelates
• Capping effects on spin and charge excitations in parent and superconducting Nd1-xSrxNiO2
• Damage of bilayer structure in La3Ni2O7-d induced by high pO2 annealing
• Lattice dynamics of the infinite-layer nickelate LaNiO${}_2$
• Superconducting phase diagram of multi-layer square-planar nickelates
• Floating zone growth at high oxygen pressures in Ruddlesden-Popper bilayer nickelate Y${}_y$Sr${}_{3-y}$Ni${}_{2-x}$Al${}_x$O${}_{7-\delta }$
• Superconducting PdTe Thin Film Via Topotactic Transformation, Toward Topological Superconductors
• Achieving superconductivity in infinite-layer nickelate thin films by aluminum sputtering deposition