Issue 36, 2022

Electronic structure and magnetic properties of transition metal kagome metal–organic frameworks

Abstract

Kagome metal–organic frameworks (MOFs) are considered a new class of materials that can host two-dimensional (2D) magnetism and correlated electron phenomena such as superconductivity and quantum anomalous Hall effect. Despite its potential for spintronics applications and others, the systematic understanding between the electronic structure and magnetic properties of kagome MOFs is still missing. This work determines the crystal structure, magnetic ground states, and anisotropy of a series of transition metal atoms and ligands from first-principles calculations. We reveal that the coexistence of covalent and ionic bonding characters of 3d orbitals is a distinctive feature of the 2D kagome MOFs. Furthermore, we demonstrate that the occupancies of active Image ID:d2cp02612k-t1.gif bands near the Fermi level are responsible for different superexchange mechanisms: the partially filled Image ID:d2cp02612k-t2.gif bands with empty Image ID:d2cp02612k-t3.gif for V and Co MOFs lead to antiferromagnetic ordering, and the partially filled Image ID:d2cp02612k-t4.gif bands with full Image ID:d2cp02612k-t5.gif for Mn, Fe, and Co MOFs lead to ferromagnetic ordering between transition metal ions. It is pointed out that the Image ID:d2cp02612k-t6.gif bands are formed through dpπ-hybridization between the transition metal dyz, dzx and ligand pz orbitals in the square planar coordination of metal atoms. This mechanism provides valuable insights into understanding magnetism in 2D kagome MOFs.

Graphical abstract: Electronic structure and magnetic properties of transition metal kagome metal–organic frameworks

Article information

Article type
Paper
Submitted
09 Jun 2022
Accepted
12 Aug 2022
First published
19 Aug 2022

Phys. Chem. Chem. Phys., 2022,24, 22168-22180

Electronic structure and magnetic properties of transition metal kagome metal–organic frameworks

S. Kang and J. Yu, Phys. Chem. Chem. Phys., 2022, 24, 22168 DOI: 10.1039/D2CP02612K

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