4.7 Article

Azide-Coordination in Homometallic Dinuclear Lanthanide(III) Complexes Containing Nonequivalent Lanthanide Metal Ions: Zero-Field SMM Behavior in the Dysprosium Analogue

期刊

INORGANIC CHEMISTRY
卷 60, 期 12, 页码 8530-8545

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.1c00249

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资金

  1. Department of Science and Technology (DST), India
  2. CNRS, Universite de Rennes 1
  3. European Commission [725184]
  4. Single Crystal CCD X-ray Diffractometer facility at IIT-Kanpur
  5. DST
  6. University Grants Commission (UGC), India
  7. DST/SERB [CRG/2018/000430, DST/SJF/CSA-03/2018-10, SB/SJF/2019-20/12]

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A series of homometallic dinuclear lanthanide complexes with nonequivalent lanthanide metal centers have been synthesized and characterized, with complex 1 showing zero-field single-molecule magnet behavior. Detailed magnetic studies revealed the influence of nonequivalent binding of the azide co-ligand and varying coordination of the deprotonated Schiff base ligand on the magnetic properties of the metal centers.
A series of homometallic dinuclear lanthanide complexes containing nonequivalent lanthanide metal centers [Ln(2)(LH2)(LH)(CH3OH)(N-3)]center dot xMeOH center dot yH(2)O [1, Ln = Dy-III, x = 0, y = 2; 2, Ln = Tb-III, x = 1, y = 1] have been synthesized [LH4 = 6-((bis(2-hydroxyethyl)amino)-N '-(2-hydroxybenzylidene)picolinohydrazide] and characterized. The dinuclear assembly contains two different types of nine-coordinated lanthanide centers, because the nonequivalent binding of the azide co-ligand as well as the varying coordination of the deprotonated Schiff base ligand. Detailed magnetic studies have been performed on the complexes 1 and 2. Complex 1 and its diluted analogue (1(5%)) are zero-field SMMs with effective energy barriers (U-eff) of magnetization reversal equal to 59(3) K and 66(3) K and relaxation times of tau(0) = 10(4) x 10(-6) s and 10(4) x 10(-8) s, respectively. On the other hand, complex 2 shows a field-induced SMM behavior. Combined ab initio and density functional theory calculations were performed to explain the experimental findings and to unravel the nature of the magnetic anisotropy, exchange-coupled spectra, and magnetic exchange interactions between the two lanthanide centers.

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