Dynamical structural instability and its implication on the physical properties of infinite-layer nickelates

Abstract

We use first-principles calculations to find that in infinite-layer nickelates $R$NiO${}_2$, the widely studied tetragonal $P4/mmm$ structure is only dynamically stable for early lanthanide elements $R$ = La-Sm. For late lanthanide elements $R$ = Eu-Lu, an imaginary phonon frequency appears at $A=(\pi ,\pi ,\pi )$ point. For those infinite-layer nickelates, condensation of this phonon mode into the $P4/mmm$ structure leads to a more energetically favorable $I4/mcm$ structure that is characterized by an out-of-phase rotation of "NiO${}_4$ square". Special attention is given to two borderline cases: PmNiO${}_2$ and SmNiO${}_2$, in which both the $P4/mmm$ structure and the $I4/mcm$ structure are local minima and the energy difference between the two structures can be fine-tuned by epitaxial strain. Compared to the $P4/mmm$ structure, $R$NiO${}_2$ in the $I4/mcm$ structure has a substantially reduced Ni $d_{x^2-y^2}$ bandwidth, a smaller Ni $d$ occupancy, a "cleaner" Fermi surface with a lanthanide-$d$-derived electron pocket suppressed at $\Gamma$ point, and a decreased critical $U_{\text{Ni}}$ to stabilize long-range antiferromagnetic ordering. All these features imply enhanced correlation effects and favor Mott physics. Our work reveals the importance of structure-property relation in infinite-layer nickelates, in particular, the spontaneous "NiO${}_4$ square" rotation provides a tuning knob to render $R$NiO${}_2$ in the $I4/mcm$ structure a closer analogy to superconducting infinite-layer cuprates.

26 pages and 6 figures

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Cited by in corpus (9)

• Sensitive dependence of pairing symmetry on Ni-$e_g$ crystal field splitting in the nickelate superconductor La${}_3$Ni${}_2$O${}_7$
• Optimizing superconductivity: from cuprates via nickelates to palladates
• Geometric effects in the infinite-layer nickelates
• Ruddlesden-Popper and perovskite phases as a material platform for altermagnetism
• An electronic origin of charge order in infinite-layer nickelates
• Structural instabilities of infinite-layer nickelates from first-principles simulations
• Possible structural quantum criticality tuned by rare-earth ion substitution in infinite-layer nickelates
• Pressure effects on the electronic structure and magnetic properties of infinite-layer nickelates
• Lattice dynamics of the infinite-layer nickelate LaNiO${}_2$