Synthesis and physical properties of LaNiO2 crystals

Abstract

Infinite-layer (IL) nickelates are an emerging family of superconductors whose similarities and differences to cuprate superconductors are under intense debate. To date, the IL phase of nickelates can only be reached via topotactic oxygen reduction of the perovskite phase, using H2 gas or reducing agents such as CaH2. While the topotactic reduction method has been widely employed on thin film and polycrystalline powder samples, the reduction of La1-xCaxNiO3 single crystals with lateral dimensions up to 150 μm was achieved only recently, using an indirect contact method with CaH2. Here we report the topotactic transformation of much larger LaNiO3 crystals with lateral dimensions of more than one millimeter, via direct contact with CaH2. We characterize the crystalline, magnetic, and electronic properties of the obtained IL LaNiO2 crystals by powder and single-crystal x-ray diffraction (XRD), magnetometry, electrical transport, and x-ray photoelectron spectroscopy (XPS) measurements. The amount of incorporated topotactic hydrogen due to the reduction process is determined by a gas extraction method. In addition, we investigate the evolution of the lattice parameters under hydrostatic pressure up to 12 GPa, using high-resolution synchrotron XRD. Furthermore, we provide a direct comparison of several physical properties of the LaNiO2 crystals to their powder and thin film counterparts.