Pressure and doping effects on the electronic structure and magnetism of the single-layer nickelate <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:msub> <mml:mi>La</mml:mi> <mml:mn>2</mml:mn> </mml:msub> <mml:msub> <mml:mi>

${\mathrm{La}}_{2}{\mathrm{NiO}}_{4}$ is a prototypical member of the Ruddlesden-Popper nickelate series that offers a valuable reference point for elucidating the key ingredients behind the intriguing properties of these systems. However, the structural and electronic properties of ${\mathrm{La}}_{2}{\mathrm{NiO}}_{4}$ under pressure and doping remain surprisingly underexplored. Here, we investigate these properties using density-functional-theory calculations. We find that its tetragonal $I4/mmm$ structure can be stabilized, not only under pressure, but also at ambient pressure via the partial substitution of La with Ba. In both cases, we find a pronounced magnetostructural interplay that manifests, in particular, as anomalies in the lattice-parameter evolution with composition, deviating from Vegard's law. Moreover, we show that the combined effects of Ba substitution and pressure leads to qualitative changes in the electronic structure toward the formal ${d}^{7.5}$ configuration of the superconducting bilayer nickelates. Further, while ${\mathrm{La}}_{2}{\mathrm{NiO}}_{4}$ can undergo an insulator-metal transition with pressure retaining G-type antiferromagnetic order, ${\mathrm{La}}_{1.5}{\mathrm{Ba}}_{0.5}{\mathrm{NiO}}_{4}$ exhibits metallic behavior with an enhanced competition between different magnetic states. Our results thus offer additional insights into the interplay of structure, doping, and magnetism across the Ruddlesden-Popper nickelate series.

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Journal
Physical Review Materials
Published
2025-11-24
DOI
https://doi.org/10.1103/94sd-ssbw
Primary Topic
Magnetic and transport properties of perovskites and related materials
Type
article
Field-Weighted Citation Impact
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article

Pressure and doping effects on the electronic structure and magnetism of the single-layer nickelate <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:msub> <mml:mi>La</mml:mi> <mml:mn>2</mml:mn> </mml:msub> <mml:msub> <mml:mi>

A. Cano, Fabio Bernardini, Quintin N. Meier, J. B. de Vaulx et al.
Physical Review Materials
Magnetic and transport properties of perovskites and related materials
article

Pressure and doping effects on the electronic structure and magnetism of the single-layer nickelate <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:msub> <mml:mi>La</mml:mi> <mml:mn>2</mml:mn> </mml:msub> <mml:msub> <mml:mi>

A. Cano, Fabio Bernardini, Quintin N. Meier, J. B. de Vaulx, Valério Olevano
article en

Abstract

${\mathrm{La}}_{2}{\mathrm{NiO}}_{4}$ is a prototypical member of the Ruddlesden-Popper nickelate series that offers a valuable reference point for elucidating the key ingredients behind the intriguing properties of these systems. However, the structural and electronic properties of ${\mathrm{La}}_{2}{\mathrm{NiO}}_{4}$ under pressure and doping remain surprisingly underexplored. Here, we investigate these properties using density-functional-theory calculations. We find that its tetragonal $I4/mmm$ structure can be stabilized, not only under pressure, but also at ambient pressure via the partial substitution of La with Ba. In both cases, we find a pronounced magnetostructural interplay that manifests, in particular, as anomalies in the lattice-parameter evolution with composition, deviating from Vegard's law. Moreover, we show that the combined effects of Ba substitution and pressure leads to qualitative changes in the electronic structure toward the formal ${d}^{7.5}$ configuration of the superconducting bilayer nickelates. Further, while ${\mathrm{La}}_{2}{\mathrm{NiO}}_{4}$ can undergo an insulator-metal transition with pressure retaining G-type antiferromagnetic order, ${\mathrm{La}}_{1.5}{\mathrm{Ba}}_{0.5}{\mathrm{NiO}}_{4}$ exhibits metallic behavior with an enhanced competition between different magnetic states. Our results thus offer additional insights into the interplay of structure, doping, and magnetism across the Ruddlesden-Popper nickelate series.

Physical Review MaterialsVol. 9(11)
University of Cagliari (IT), Institut Néel (FR)
Openalex Percentile: Top 74%
Magnetic and transport properties of perovskites and related materials
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