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We examine the bulk electronic structure of ${\mathrm{Nd}}_3{\mathrm{Ni}}_2{\mathrm{O}}_7$using Ni $2p$core-level hard x-ray photoemission spectroscopy combined with density functional theory $+$dynamical mean-field theory. Our results reveal a large deviation of the Ni $3d$occupation from the formal ${\mathrm{Ni}}^{2.5+}$valency, highlighting the importance of the charge transfer from oxygen ligands. We find that the dominant $d^8$configuration is accompanied by nearly equal contributions from $d^7$and $d^9$states, exhibiting an unusual valence state among Ni-based oxides. Finally, we discuss the Ni $d_{x^2-y^2}$and $d_{z^2}$orbital-dependent hybridization, correlation and local spin dynamics. Published by the American Physical Society2025 

Abstract A key open question in the study of layered superconducting nickelate films is the role that hydrogen incorporation into the lattice plays in the appearance of the superconducting state. Due to the challenges of stabilizing highly crystalline square planar nickelate films, films are prepared by the deposition of a more stable parent compound which is then transformed into the target phaseviaa topotactic reaction with a strongly reducing agent such as CaH₂. Recent studies, both experimental and theoretical, have introduced the possibility that the incorporation of hydrogen from the reducing agent into the nickelate lattice may be critical for the superconductivity. In this work, we use secondary ion mass spectrometry to examine superconducting La_1−xX_xNiO₂/ SrTiO₃(X= Ca and Sr) and Nd₆Ni₅O₁₂/ NdGaO₃films, along with non-superconducting NdNiO₂/ SrTiO₃and (Nd,Sr)NiO₂/ SrTiO₃. We find no evidence for extensive hydrogen incorporation across a broad range of samples, including both superconducting and non-superconducting films. Theoretical calculations indicate that hydrogen incorporation is broadly energetically unfavorable in these systems, supporting our conclusion that extensive hydrogen incorporation is not generally required to achieve a superconducting state in layered square-planar nickelates. 

Abstract The layered square-planar nickelates, Nd n +1 Ni n O 2 n +2 , are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd 6 Ni 5 O 12 thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n  = 3 Ruddlesden-Popper compound, Nd 4 Ni 3 O 10 , and subsequent reduction to the square-planar phase, Nd 4 Ni 3 O 8 . We synthesize our highest quality Nd 4 Ni 3 O 10 films under compressive strain on LaAlO 3 (001), while Nd 4 Ni 3 O 10 on NdGaO 3 (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd 4 Ni 3 O 10 on SrTiO 3 (001). Films reduced on LaAlO 3 become insulating and form compressive strain-induced c -axis canting defects, while Nd 4 Ni 3 O 8 films on NdGaO 3 are metallic. This work provides a pathway to the synthesis of Nd n +1 Ni n O 2 n +2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy.