2022/02/09 by D. Szaller, L. Prodan, Szaller, D. +27 · 2 citations
Materials Science · Physics and Astronomy · #Advanced Condensed Matter Physics #FOS: Physical sciences #Multiferroics and related materials #Physics of Superconductivity and Magnetism #Strongly Correlated Electrons (cond-mat.str-el)
paper · pdf · doi:10.48550/arxiv.2202.04700
openalex publication_date 2022/02/09 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
Antiferromagnetic and ferro/ferrimagnetic orders are typically exclusive in nature, thus, their co-existence in atomic-scale proximity is expected only in heterostructures. Breaking this paradigm and broadening the range of unconventional magnetic states, we report here on an atomic-scale hybrid spin state, which is stabilized in three-dimensional crystals of the polar antiferromagnet Co2Mo3O8 by magnetic fields applied perpendicular to the Co honeycomb layers and possesses a spontaneous in-plane ferromagnetic moment. Our microscopic spin model, capturing the observed field dependence of the longitudinal and transverse magnetization as well as the magnetoelectric/elastic properties, reveals that this novel spin state is composed of an alternating stacking of antiferromagnetic and ferrimagnetic honeycomb layers. The strong intra-layer and the weak inter-layer exchange couplings together with competing anisotropies at octahedral and tetrahedral Co sites are identified as the key ingredients to stabilize antiferromagnetic and ferrimagnetic layers in such a close proximity. We show that the proper balance of magnetic interactions can extend the stability range of this hybrid phase down to zero magnetic field. The possibility to realize a layer-by-layer stacking of such distinct spin orders via suitable combinations of microscopic interactions opens a new dimension towards the nanoscale engineering of magnetic states.