Abstract
We synthesized the dinuclear and mononuclear dysprosium(III) complexes [{Dy(Tp)2}2(Cl2An)]·2CH2Cl2 (1) and [Co(Cp)2][Dy(Tp)2(Cl2An)] (3), where Cl2An2− and Tp− are the chloranilate and hydrotris(pyrazolyl)borate ligand, respectively. In addition, the magnitude of the magnetic coupling between the lanthanide centers through the Cl2An2− bridge has been probed through the synthesis of [{Gd(Tp)2}2(Cl2An)]·2CH2Cl2 (2), which is a gadolinium(III) analogue of 1. Complexes 1–3 were characterized by infrared (IR) spectroscopy, elemental analysis, single-crystal X-ray diffraction, and SQUID measurements. IR and single-crystal X-ray structural analyses confirm that the coordination environments of the lanthanide(III) centers in 1 and 3 are similar to each other; i.e., eight-coordinated metal centers, each occupied by an N6O2 donor set from two Tp− ligands and one Cl2An2− ligand. The coordination geometries of the lanthanide(III) centers in 1 and 2 are distorted triangular dodecahedral, while that in the mononuclear complex 3 is square antiprismatic, where the Cl2An2− ligand takes the bi-separated delocalized form in 1 and 2, and the o-quinone form in 3. Alternating-current (AC) magnetic studies clearly reveal that both 1 and 3 exhibit field-induced slow relaxations of magnetization that occur via Raman and direct processes. Complexes 1 and 3 exhibit different spin relaxation behavior, which reflects the coordination geometry around each DyIII center and its nuclearity, as well as the molecular packing in the crystal lattice. Although the magnetic analysis of 2 revealed negligible magnetic coupling, Cl2An2− bridges with small biases may form in the dinuclear complexes, which play roles in the spin relaxation dynamics through dipolar interactions.
Highlights
Molecule-based nanomagnets, such as single-molecule magnets (SMMs) [1,2,3,4,5,6,7] and single-ion magnets (SIMs) [8,9,10,11,12], are strictly low-dimensional magnetic systems that exhibit magnetization blocking at low temperatures, quantum tunneling of magnetization (QTM) [13], and quantum coherence [14,15]
Bright yellow microcrystalline solid appeared immediately, which was collected by filtration, washed with a small amount of Et2 O (5 mL), and allowed to dry on the filter for 15 min
Magnetic data were collected on a Quantum Design MPMS3 or MPMS-5S superconducting quantum interference device (SQUID)
Summary
Molecule-based nanomagnets, such as single-molecule magnets (SMMs) [1,2,3,4,5,6,7] and single-ion magnets (SIMs) [8,9,10,11,12], are strictly low-dimensional magnetic systems that exhibit magnetization blocking at low temperatures, quantum tunneling of magnetization (QTM) [13], and quantum coherence [14,15]. Surveys of SMMs[16], were focused on polynuclear cluster complexes high nuclearities for quantum computing high-density information storage [17], and more with recently, molecular due to the realization large ground spin states [2]. More recent frontline SMMs studies have tended to focus on enhancing method for increasing the blocking temperature and the activation energy barrier From these magnetic anisotropy, rather than augmenting ground spin states, which is a much more informative. SMMs, and more recently, SIMs, based on trivalent lanthanide (LnIII ),from bothions spin-orbit coupling crystal-field splitting, where crystal-field splitting is normally much have proceeded at and a rapid pace because of their significant magnetic anisotropies that arise from.
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