Relationship between the Coordination Geometry and Spin Dynamics of Dysprosium(III) Heteroleptic Triple-Decker Complexes

Tetsu Sato,Brian K Breedlove,Satoshi Matsuzawa,Masahiro Yamashita,Keiichi Katoh

doi:10.3390/magnetochemistry5040065

Tetsu Sato, Brian K Breedlove + Show 3 more

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https://doi.org/10.3390/magnetochemistry5040065

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Journal: Magnetochemistry	Publication Date: Nov 26, 2019
Citations: 7	License type: CC BY 4.0

Affiliation: Tohoku University, Nankai University

Abstract

When using single molecule magnets (SMMs) in spintronics devices, controlling the quantum tunneling of the magnetization (QTM) and spin-lattice interactions is important. To improve the functionality of SMMs, researchers have explored the effects of changing the coordination geometry of SMMs and the magnetic interactions between them. Here, we report on the effects of the octa-coordination geometry on the magnetic relaxation processes of dinuclear dysprosium(III) complexes in the low-temperature region. Mixed ligand dinuclear Dy3+ triple-decker complexes [(TPP)Dy(Pc)Dy(TPP)] (1), which have crystallographically equivalent Dy3+ ions, and [(Pc)Dy(Pc)Dy(TPP)] (2), which have non-equivalent Dy3+ ions, (Pc2− = phthalocyaninato; TPP2− = tetraphenylporphyrinato), undergo dual magnetic relaxation processes. This is due to the differences in the ground states due to the twist angle (φ) between the ligands. The relationship between the off-diagonal terms and the dual magnetic relaxation processes that appears due to a deviation from D4h symmetry is discussed.

Highlights

Rational design and synthesis of single molecular magnets (SMMs) and molecular nanomagnets (MNMs) suitable for quantum information processing (QIP) in quantum computers (QCs) remains difficult [1,2,3,4,5,6,7]
In addition to the dinuclear Dy3+ triple-decker complexes we have reported so far, we discuss the relationship between coordination environment and magnetic properties for (TPP)Dy(Pc)Dy(TPP)] (1) and [(Pc)Dy(Pc)Dy(TPP)] (2) (Pc2− = phthalocyaninato and TPP2− = tetraphenylporphyrinato) with C4 symmetry
For 1, which crystallized in the tetragonal space group I4/m, the twist angle (φ) between the outer TPP2− ligand and the inner Pc ligand was determined to be 4◦

Summary

Introduction

Rational design and synthesis of single molecular magnets (SMMs) and molecular nanomagnets (MNMs) suitable for quantum information processing (QIP) in quantum computers (QCs) remains difficult [1,2,3,4,5,6,7]. In the D4d ligand field system, the SMM characteristics can be controlled by manipulating the ground state via rotation of the ligands by protonation/deprotonation [11,12], coupling of Tb3+-bisphthalocyaninato (Pc2−) complex with cadmium ions, etc. Several groups have shown the relationship between octa-coordination environments and the magnetic relaxation processes of Tb3+-Pc2− multiple-decker SMMs along the C4 rotation axis. From these reports, correlations between the twist angle (φ), ligand field (LF) parameters, and the lowest ground state of Pc2− have been clarified [14].

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