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Noninnocent Ligands as a Design Strategy for Fully Compensated Ferrimagnetism in Two-Dimensional Metal-Organic
Yuxuan Li1, Yixuan Che1, Haifeng Lv2
1Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui230026, China.
Journal of the American Chemical Society
|July 27, 2026
Summary
We introduce a new strategy for designing two-dimensional fully compensated ferrimagnets (fFiMs) using metal-organic frameworks with noninnocent ligands. This approach enables precise control over magnetic properties for advanced spintronic applications.
Area of Science:
- Materials Science
- Condensed Matter Physics
- Chemistry
Background:
- Fully compensated ferrimagnets (fFiMs) offer stray-field-free spintronics due to vanishing macroscopic magnetization.
- Designing fFiMs is challenging due to the need for precise control over magnetic sublattices.
Purpose of the Study:
- To develop a general design strategy for two-dimensional (2D) fFiMs.
- To enable stoichiometric moment compensation in 2D magnets through controlled charge transfer.
Main Methods:
- First-principles calculations were employed to investigate electronic and magnetic properties.
- A novel approach integrating redox-active noninnocent ligands (NILs) into metal-organic frameworks (MOFs) was proposed.
- Chemical modifications, including ligand fluorination and heavy-chalcogen substitution, were explored to enhance material stability.
Main Results:
- Fractional metal-to-ligand charge transfer was shown to create a spin-bearing ligand sublattice antiparallel to metal centers, achieving moment compensation.
- The prototype Cr(BTT)2 demonstrated fFiM properties but lacked thermal stability.
- Chemically optimized Cr(F-BTT)2 exhibited stable fFiM behavior with a magnetic transition temperature of 132 K and a quasi-Dirac band feature.
Conclusions:
- NIL-directed charge transfer provides a chemically programmable method for engineering 2D compensated magnets.
- The developed strategy offers a pathway for designing stable, high-performance fFiMs for spintronic devices.
- The study validates the use of MOFs and NILs for creating novel magnetic materials.
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