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Octanuclear heterobimetallic {Ni4Ln4} assemblies possessing Ln4 square grid [2×2] motifs : synthesis, structure and magnetism
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Biswas, Sourav , Goura, Joydeb , Das, Sourav , Topping, Craig V., Brambleby, Jamie, Goddard, Paul and Chandrasekhar, Vadapalli (2016) Octanuclear heterobimetallic {Ni4Ln4} assemblies possessing Ln4 square grid [2×2] motifs : synthesis, structure and magnetism. Inorganic Chemistry, 55 (17). pp. 8422-8436. doi:10.1021/acs.inorgchem.6b01019
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Official URL: http://doi.org/10.1021/acs.inorgchem.6b01019
Abstract
Octanuclear heterobimetallic complexes, [Ln4Ni4(H3L)4(µ3-OH)4(µ2-OH)4]4Cl·xH2O·yCHCl3 (Dy3+ , x = 30.6, y = 2 (1); Tb3+ , x = 28, y = 0 (2) ; Gd3+ , x = 25.3, y = 0 (3); Ho3+ , x = 30.6, y = 3 (4)) (H5L = N1, N3-bis(6-formyl-2-(hydroxymethyl)
-4-methylphenol) diethylenetriamine) are reported. These are assembled by the cumulative coordination action of four doubly deprotonated compartmental ligands, [H3L] 2- , along with eight exogenous –OH ligands. Within the core of these complexes, four Ln3+ are distributed to the four corners of a perfect square grid while four Ni2+ are projected away from the plane of the Ln4 unit. Each of the four Ni2+ possesses distorted octahedral geometry while all the Ln3+ are crystallographically equivalent and are present in an elongated square antiprism geometry. The magnetic properties of compound 3 are dominated by an easy-plane single-ion anisotropy of the Ni2+ ions [DNi = 6.7(7) K] and dipolar interactions between Gd3+ centers. Detailed ac magnetometry reveals the presence of distinct temperature-dependent out-of-phase signals for compounds 1 and 2, indicative of slow magnetic relaxation. Magnetochemical analysis of complex 1 implies the 3d and the 4f metal ions are engaged in ferromagnetic interactions with SMM behavior, while dc magnetometry of compound 2 is suggestive of an antiferromagnetic Ni-Tb spin-exchange with slow magnetic relaxation due to a field-induced level crossing. Compound 4 exhibits an easy-plane single-ion anisotropy for the Ho3+ ions and weak interactions between spin centers.
| Item Type: | Journal Article | ||||||
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| Alternative Title: | |||||||
| Subjects: | Q Science > QD Chemistry | ||||||
| Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||
| Library of Congress Subject Headings (LCSH): | Inorganic compounds -- Synthesis, Inorganic compounds -- Magnetic properties | ||||||
| Journal or Publication Title: | Inorganic Chemistry | ||||||
| Publisher: | American Chemical Society | ||||||
| ISSN: | 0020-1669 | ||||||
| Official Date: | 8 August 2016 | ||||||
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| Volume: | 55 | ||||||
| Number: | 17 | ||||||
| Page Range: | pp. 8422-8436 | ||||||
| DOI: | 10.1021/acs.inorgchem.6b01019 | ||||||
| Status: | Peer Reviewed | ||||||
| Publication Status: | Published | ||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||
| RIOXX Funder/Project Grant: |
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