Electronic structure, spin state, and magnetism of the square-lattice Mott insulator La2Co2Se2O3 from first principles

TL;DR

This study uses first-principles calculations to reveal that La2Co2Se2O3 is a Mott insulator with a stable high-spin Co2+ state, complex magnetic interactions, and potential for a frustrated antiferromagnetic structure.

Contribution

It provides the first detailed electronic and magnetic structure analysis of La2Co2Se2O3, predicting a frustrated antiferromagnetic order not yet experimentally confirmed.

Findings

La2Co2Se2O3 is a Mott insulator.

Co2+ ions are in a high-spin state with orbital ordering.

Complex magnetic couplings suggest a frustrated antiferromagnetic structure.

Abstract

Electronic and magnetic structures of the newly synthesized cobalt oxyselenide La2Co2Se2O3 (structurally similar to the superconducting iron pnictides) are studied through density functional calculations. The obtained results show that this material is a Mott insulator, and that it has a very stable Co2+ high-spin ground state with a t2g-like orbital ordering, which is substantiated by the calculated crystal-field excitation energies. The square lattice of the Co2+ spins is found to have a strong antiferro (a weak ferro) magnetic coupling for the second nearest neighbors (2nn) via O (Se2) and an intermediate antiferro one for the 1nn, with the strength ratio about 10:1:3. The present results account for the available experimental data of magnetism, and the prediction of a planar frustrated (2x2) antiferromagnetic structure would motivate a new experiment.