Magnetic and Thermodynamic Computations for Supramolecular Assemblies between a Cr(III) and Fe(III) Single-Ion Magnet and an Fe(II) Spin-Crossover Complex

Angel Albavera-Mata; Shuanglong Liu; Hai-Ping Cheng; Richard G Hennig; S B Trickey

doi:10.1021/acs.jpca.4c06723

Magnetic and Thermodynamic Computations for Supramolecular Assemblies between a Cr(III) and Fe(III) Single-Ion Magnet and an Fe(II) Spin-Crossover Complex

J Phys Chem A. 2024 Dec 19;128(50):10929-10935. doi: 10.1021/acs.jpca.4c06723. Epub 2024 Dec 6.

Authors

Angel Albavera-Mata^{1

2}, Shuanglong Liu^{1

3}, Hai-Ping Cheng^{1

3}, Richard G Hennig^{1

2}, S B Trickey^{1

4}

Affiliations

¹ Center for Molecular Magnetic Quantum Materials, University of Florida, Gainesville, Florida 32611, United States.
² Department of Materials Science and Engineering, University of Florida, Gainesville, Florida 32611, United States.
³ Department of Physics, Northeastern University, Boston, Massachusetts 02115, United States.
⁴ Department of Physics and Department of Chemistry, University of Florida, Gainesville, Florida 32611, United States.

PMID: 39642178
DOI: 10.1021/acs.jpca.4c06723

Abstract

Experimental results on two supramolecular complexes in which a Cr^III or Fe^III d-orbital single-ion magnet center is embedded between a pair of Fe^II spin-crossover moieties make those two complexes interesting as possible candidates for use in quantum information technologies. We report detailed computational results for their structure and electronic properties and use the resulting data to parametrize a spin Hamiltonian that facilitates comparison with experimental results and their interpretation. Consistent with experimental results on decoherence in [Fe(ox)₃]@[Fe₂L₃]⁺, we find it to be easy-plane type while the [Cr(ox)₃]@[Fe₂L₃]⁺ system is easy-axis type.