Switchable Altermagnetism in a Layered van der Waals Metal-Organic Framework Driven by Spin-Crossover
Abstract
Dynamical control of altermagnetism is a key requirement for translating its unique spin-dependent functionalities into practical spintronic devices, yet effective switching mechanisms remain largely unexplored. Here, we open an unprecedented, versatile and programmable route based on spin-crossover to switch altermagnetism on demand in molecular materials. Using density functional calculations, we demonstrate an altermagnetic ground state in the layered van der Waals MOFs MnX2(tdz)2 (X = Cl, Br; tdz = thiadiazole), stabilized by anisotropic interlayer exchange interactions, which gives rise to a characteristic d-wave momentum-space spin splitting and an associated spin-splitter transport response. Our findings reveal that under hydrostatic pressure, a high-spin to low-spin transition reconfigures the Mn d-orbital occupation, thus modifying the magnetic exchange network, and stabilizing a different antiferromagnetic ground state whose symmetry suppresses the nonrelativistic spin splitting. Crucially, spin-crossover switches altermagnetism not by directly altering the electronic structure, but by changing the symmetry of the magnetic ground state. These results establish molecular spin-crossover altermagnets as a platform for externally reconfigurable spintronic devices.
Related
- Electric-Field-Switchable Altermagnetism via Ligand Rotation in a d0 Metal-Organic Framework
- Layered spin-crossover metal-organic frameworks for light-induced control of two-dimensional quantum materials
- Altermagnetism across the BCS-BEC crossover
- Altermagnetism and generalised tensorial properties in the exchange multiplet framework
- NEMO: A Framework for Nematic and Morphological Analysis of Curved and Multi-layered Biological Surfaces
BibTeX
@misc{lopezalcala2026switchable,
title = {{Switchable Altermagnetism in a Layered van der Waals Metal-Organic Framework Driven by Spin-Crossover}},
author = {Diego López-Alcalá and Alberto M. Ruiz and Andrei Shumilin and José J. Baldoví},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.07548},
eprint = {2609.07548},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.07548},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Switchable Altermagnetism in a Layered van der Waals Metal-Organic Framework Driven by Spin-Crossover
AU - Diego López-Alcalá
AU - Alberto M. Ruiz
AU - Andrei Shumilin
AU - José J. Baldoví
PY - 2026
DA - 2026/09/07
PB - arXiv
DO - 10.48550/arxiv.2609.07548
UR - https://arxiv.org/abs/2609.07548
AB - Dynamical control of altermagnetism is a key requirement for translating its unique spin-dependent functionalities into practical spintronic devices, yet effective switching mechanisms remain largely unexplored. Here, we open an unprecedented, versatile and programmable route based on spin-crossover to switch altermagnetism on demand in molecular materials. Using density functional calculations, we demonstrate an altermagnetic ground state in the layered van der Waals MOFs MnX_2(tdz)_2 (X = Cl, Br; tdz = thiadiazole), stabilized by anisotropic interlayer exchange interactions, which gives rise to a characteristic d-wave momentum-space spin splitting and an associated spin-splitter transport response. Our findings reveal that under hydrostatic pressure, a high-spin to low-spin transition reconfigures the Mn d-orbital occupation, thus modifying the magnetic exchange network, and stabilizing a different antiferromagnetic ground state whose symmetry suppresses the nonrelativistic spin splitting. Crucially, spin-crossover switches altermagnetism not by directly altering the electronic structure, but by changing the symmetry of the magnetic ground state. These results establish molecular spin-crossover altermagnets as a platform for externally reconfigurable spintronic devices.
ER -