Cr3+ spin dynamics under the octahedral crystal field in van der Waals antiferromagnets
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| Main Authors: | , , , , , |
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| Format: | Preprint |
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2026
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| _version_ | 1866914344289173504 |
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| author | Basnet, Rabindra Chatterjee, Subhashree Kigaya, Paul Negusse, Ezana van Tol, J. Budhani, Ramesh C. |
| author_facet | Basnet, Rabindra Chatterjee, Subhashree Kigaya, Paul Negusse, Ezana van Tol, J. Budhani, Ramesh C. |
| contents | The magnetic moment in van der Waals (vdW) materials containing 3d transition metals originates from unpaired d-electron spins and their interaction with surrounding ligands. The interplay between exchange interactions and magnetic anisotropy stabilizes long-range ordering of such moments. The compound CuCrP2S6 (CCPS) presents an interesting class of vdW solids where the coupling of Cr3+ moments and ordering of Cu1+ ions give rise to a multiferroic ground state. Here we investigate the spin dynamics of Cr3+ ions in CCPS through magnetization and broadband as well as single sub-THz magnetic resonance measurements. The orbital moment of Cr3+ is quenched under the octahedral crystal field of surrounding chalcogen ions, resulting in negligible magnetic anisotropy-a feature common to Cr-based vdW antiferromagnets (AFM). Resonance spectra over a wide frequency-field-temperature range reveal quasi-2D AFM dynamics governed mainly by isotropic Cr-Cr exchange interactions, which determine the magnetic order, spin reorientation, and damping. Sub-THz resonance spectra also uncover a field-induced ferromagnetic polarization, highlighting the universal role of Cr-Cr exchange in layered Cr compounds. Moreover, persistent magnetic correlations far above the Néel temperature (TN ~ 32 K) points to short-range magnetic order in CCPS and motivates future studies of a possible interplay between AFM and antiferroelectric orders. These results establish CCPS as an exemplary system for exploring 2D magnetism and electric-field-tunable spintronic functionalities in layered multiferroics. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2602_20033 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Cr3+ spin dynamics under the octahedral crystal field in van der Waals antiferromagnets Basnet, Rabindra Chatterjee, Subhashree Kigaya, Paul Negusse, Ezana van Tol, J. Budhani, Ramesh C. Materials Science The magnetic moment in van der Waals (vdW) materials containing 3d transition metals originates from unpaired d-electron spins and their interaction with surrounding ligands. The interplay between exchange interactions and magnetic anisotropy stabilizes long-range ordering of such moments. The compound CuCrP2S6 (CCPS) presents an interesting class of vdW solids where the coupling of Cr3+ moments and ordering of Cu1+ ions give rise to a multiferroic ground state. Here we investigate the spin dynamics of Cr3+ ions in CCPS through magnetization and broadband as well as single sub-THz magnetic resonance measurements. The orbital moment of Cr3+ is quenched under the octahedral crystal field of surrounding chalcogen ions, resulting in negligible magnetic anisotropy-a feature common to Cr-based vdW antiferromagnets (AFM). Resonance spectra over a wide frequency-field-temperature range reveal quasi-2D AFM dynamics governed mainly by isotropic Cr-Cr exchange interactions, which determine the magnetic order, spin reorientation, and damping. Sub-THz resonance spectra also uncover a field-induced ferromagnetic polarization, highlighting the universal role of Cr-Cr exchange in layered Cr compounds. Moreover, persistent magnetic correlations far above the Néel temperature (TN ~ 32 K) points to short-range magnetic order in CCPS and motivates future studies of a possible interplay between AFM and antiferroelectric orders. These results establish CCPS as an exemplary system for exploring 2D magnetism and electric-field-tunable spintronic functionalities in layered multiferroics. |
| title | Cr3+ spin dynamics under the octahedral crystal field in van der Waals antiferromagnets |
| topic | Materials Science |
| url | https://arxiv.org/abs/2602.20033 |