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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. 

Abstract We provide a set of computational experiments based on ab initio calculations to elucidate whether a cuprate-like antiferromagnetic insulating state can be present in the phase diagram of the low-valence layered nickelate family (R $$_{n+1}$$ n + 1 Ni $$_n$$ n O $$_{2n+2}$$ 2 n + 2 , R= rare-earth, $$n=1-\infty$$ n = 1 - ∞ ) in proximity to half-filling. It is well established that at $$d^9$$ d 9 filling the infinite-layer ( $$n=\infty$$ n = ∞ ) nickelate is metallic, in contrast to cuprates wherein an antiferromagnetic insulator is expected. We show that for the Ruddlesden-Popper (RP) reduced phases of the series (finite n ) an antiferromagnetic insulating ground state can naturally be obtained instead at $$d^9$$ d 9 filling, due to the spacer RO $$_2$$ 2 fluorite slabs present in their structure that block the c -axis dispersion. In the $$n=\infty$$ n = ∞ nickelate, the same type of solution can be derived if the off-plane R-Ni coupling is suppressed. We show how this can be achieved if a structural element that cuts off the c -axis dispersion is introduced (i.e. vacuum in a monolayer of RNiO $$_2$$ 2 , or a blocking layer in multilayers formed by (RNiO $$_2$$ 2 ) $$_1$$ 1 /(RNaO $$_2$$ 2 ) $$_1$$ 1 ). 

The discovery of superconductivity in thin films (∼10 nm) of infinite-layer hole-doped NdNiO 2 has invigorated the field of high temperature superconductivity research, reviving the debate over contrasting views that nickelates that are isostructural with cuprates are either 1) sisters of the high temperature superconductors, or 2) that differences between nickel and copper at equal band filling should be the focus of attention. Each viewpoint has its merits, and each has its limitations, suggesting that such a simple picture must be superseded by a more holistic comparison of the two classes. Several recent studies have begun this generalization, raising a number of questions without suggesting any consensus. In this paper, we organize the findings of the electronic structures of n -layered NiO 2 materials ( n = 1 to ∞ ) to outline (ir)regularities and to make comparisons with cuprates, with the hope that important directions of future research will emerge.