Luca Binci^1*, Michele Kotiuga^1*, Iurii Timrov^1*, Nicola Marzari^1,2*

1 Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland

2 Laboratory for Materials Simulations, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland

* Corresponding authors emails: luca.binci@epfl.ch, michele.kotiuga@epfl.ch, iurii.timrov@epfl.ch, nicola.marzari@epfl.ch

DOI10.24435/materialscloud:2h-gq [version v1]

Publication date: Mar 02, 2023

How to cite this record

Luca Binci, Michele Kotiuga, Iurii Timrov, Nicola Marzari, Hybridization driving distortions and multiferroicity in rare-earth nickelates, Materials Cloud Archive 2023.34 (2023), doi: 10.24435/materialscloud:2h-gq.

Description

For decades transition-metal oxides have generated a huge interest due to the multitude of physical phenomena they exhibit. In this class of materials, the rare-earth nickelates, RNiO₃, stand out for their rich phase diagram stemming from complex couplings between the lattice, electronic and magnetic degrees of freedom. Here, we present a first-principles study of the low-temperature phase for two members of the RNiO₃ series, with R = Pr, Y. We employ density-functional theory with Hubbard corrections accounting not only for the on-site localizing interactions among the Ni-3d electrons (U), but also the inter-site hybridization effects between the transition-metals and the ligands (V). All the U and V parameters are calculated from first-principles using density-functional perturbation theory, resulting in a fully ab initio methodology. Our simulations show that the inclusion of the inter-site interaction parameters V is necessary to simultaneously capture the features well-established by experimental characterizations of the low-temperature state: insulating character, antiferromagnetism and bond disproportionation. On the contrary, for some magnetic orderings the inclusion of on-site interaction parameters U alone completely suppresses the breathing distortion occurring in the low-temperature phase and produces an erroneous electronic state with a vanishing band gap. In addition - only when both the U and V are considered - we predict a polar phase with a magnetization-dependent electric polarization, supporting very recent experimental observations that suggest a possible occurrence of type-II multiferroicity for these materials.

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Keywords

electronic structure magnetism rare-earth nickelates MARVEL