First-principles study of the crystal and magnetic structures of multiferroic Cu2OCl2

Peter Tsung-Wen Yen; Hung-Cheng Wu; Shin-Ming Huang

doi:10.1088/1361-648X/ac75a2

First-principles study of the crystal and magnetic structures of multiferroic Cu₂OCl₂

J Phys Condens Matter. 2022 Jun 17;34(33). doi: 10.1088/1361-648X/ac75a2.

Authors

Peter Tsung-Wen Yen^{1

2

3}, Hung-Cheng Wu¹, Shin-Ming Huang^{1

2

3}

Affiliations

¹ Physics Department, National Sun Yat-sen University, Kaohsiung 80424, Taiwan.
² Center for Crystal Researches, National Sun Yat-sen University, Kaohsiung 80424, Taiwan.
³ Center for Theoretical and Computational Physics, National Sun Yat-sen University, Kaohsiung 80424, Taiwan.

PMID: 35654030
DOI: 10.1088/1361-648X/ac75a2

Abstract

Recently, the discovery of multiferroicity in pyrochlore-like compound Cu₂OCl₂has generated significant interest, and several studies have been performed in this area. This transition metal oxychloride is unique because the divalent copper atoms create anS=1/2correlated insulator and the pyrochlore lattice tends to frustrate spins. From neutron powder diffraction measurements, an incommensurate magnetic order of the ordering vectorq=(0.827,0,0)emerges below the Néel temperature of 70 K. At this temperature or slightly above, ferroelectricity (FE) or antiferroelectricity, accompanying a lattice distortion, has been observed. Experimentally, some discrepancies remain. In this paper, we report our first-principles simulation results by evaluating the possible lattice and spin spiral states. We found that theFdddstructure is not more stable thanFdd2(a), which is supported by our reexamination of the x-ray diffraction data. In addition, we find that after we include magnetism in the calculation, it predicts that theFdd2(a)lattice with a helical (proper screw) spin structure is energetically more stable than other spin configurations. Our results indicate charge-order-driven FE that subsequently induces magnetism.

Keywords: ab initio methods; density-functional theory; frustrated spin systems; incommensurate spin spirals; multiferroics; pyrochlore lattice; spin configurations.