Electric-Field-Switchable Altermagnetism via Ligand Rotation in a d0 Metal-Organic Framework
Abstract
Altermagnetism combines vanishing net magnetization with momentum-dependent spin splitting. While altermagnetic signatures have been identified in metal-organic frameworks (MOFs), non-invasive reversible control remains challenging. Here we report a route to electric-field-switchable altermagnetism in a flexible d0-MOF, in which polar substituents couple the external field to ligand rotation. In the planar ground state, pz orbitals mediate 180-degree ligand-metal-ligand superexchange (J2), stabilizing antiferromagnetic order. Rotating ligands out of plane activates px/py orbitals, enhances 90-degree pathways (J1), and reverses J1/J2 competition. The antiferromagnetic-to-altermagnetic crossover occurs at approx. 34 degrees, with spin splitting of 84 meV at 90 degrees. The 90-degree altermagnetic state is switched on by the electric field and switched off upon field removal, as the constrained-rotation landscape decreases monotonically back toward 0 degrees, enabling barrierless relaxation to the antiferromagnetic state and reversible on/off operation. Ab initio molecular dynamics at 300 K shows thermal fluctuations alone cannot synchronize ligand rotation. Polar substituents provide the required coupling for electric-field control; for fluorinated substituents, the critical field is approx. 0.22 V/Angstrom, comparable to field-effect devices. This work establishes ligand p orbitals, rather than transition-metal d orbitals, as the origin of altermagnetic order and shows that polar substituents enable electric-field control for organic spintronics.
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BibTeX
@misc{wang2026electricfieldswitchable,
title = {{Electric-Field-Switchable Altermagnetism via Ligand Rotation in a d0 Metal-Organic Framework}},
author = {Hongjing Wang and Xiuling Li and Xiaojun Wu},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2609.16749},
eprint = {2609.16749},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.16749},
}
RIS
TY - UNPB
TI - Electric-Field-Switchable Altermagnetism via Ligand Rotation in a d0 Metal-Organic Framework
AU - Hongjing Wang
AU - Xiuling Li
AU - Xiaojun Wu
PY - 2026
DA - 2026/10/12
PB - arXiv
DO - 10.48550/arxiv.2609.16749
UR - https://arxiv.org/abs/2609.16749
AB - Altermagnetism combines vanishing net magnetization with momentum-dependent spin splitting. While altermagnetic signatures have been identified in metal-organic frameworks (MOFs), non-invasive reversible control remains challenging. Here we report a route to electric-field-switchable altermagnetism in a flexible d0-MOF, in which polar substituents couple the external field to ligand rotation. In the planar ground state, pz orbitals mediate 180-degree ligand-metal-ligand superexchange (J2), stabilizing antiferromagnetic order. Rotating ligands out of plane activates px/py orbitals, enhances 90-degree pathways (J1), and reverses J1/J2 competition. The antiferromagnetic-to-altermagnetic crossover occurs at approx. 34 degrees, with spin splitting of 84 meV at 90 degrees. The 90-degree altermagnetic state is switched on by the electric field and switched off upon field removal, as the constrained-rotation landscape decreases monotonically back toward 0 degrees, enabling barrierless relaxation to the antiferromagnetic state and reversible on/off operation. Ab initio molecular dynamics at 300 K shows thermal fluctuations alone cannot synchronize ligand rotation. Polar substituents provide the required coupling for electric-field control; for fluorinated substituents, the critical field is approx. 0.22 V/Angstrom, comparable to field-effect devices. This work establishes ligand p orbitals, rather than transition-metal d orbitals, as the origin of altermagnetic order and shows that polar substituents enable electric-field control for organic spintronics.
ER -