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Title: Influence of lanthanides on spin-relaxation and spin-structure in a family of Fe 7Ln 4 single molecule magnets

A family of isostructural undecanuclear 3d–4f coordination clusters of formula [Fe III 7Ln III 4O 4(OH) 3(tea) 2(Htea) 3(Piv) 7(H 2O) 2(NO 3) 3], where Ln = Y (1), Gd (2), Tb (3), Dy (4); PivH ≡ pivalic acid and H 3tea ≡ triethanolamine, was synthesised in this paper. The central Fe7 core of the coordination cluster can be described in terms of two {Fe 4O 2} butterfly motifs sharing a common body Fe atom. The two Fe 4 mean-planes subtend a dihedral angle of ca. 72°. The Tb (3) and Dy (4) compounds show Single Molecule Magnet (SMM) behaviour as confirmed by ac-susceptibility and μ-SQUID measurements. Furthermore, 57Fe Mössbauer spectra of 1–4 confirm the presence of high-spin Fe III sites. The spectra of all complexes in the high temperature range (30–300 K) show broad overlapping doublets which were assigned to the body and wing-tip pairs of metal ions within the Fe 7 core. The low temperature Mössbauer spectra show dependence on the nature of the rare-earth metal as a result of its interaction with the iron sites. Finally, we observed a transition from fast (2), to intermediate (1) and very slow (frozen) (3, 4) spin fluctuation phenomena in thesemore » compounds.« less
Authors:
ORCiD logo [1] ; ORCiD logo [2] ;  [3] ;  [4] ; ORCiD logo [5] ; ORCiD logo [3] ; ORCiD logo [6] ; ORCiD logo [7] ; ORCiD logo [8]
  1. Karlsruhe Inst. of Technology (KIT) (Germany). Inst. of Inorganic Chemistry; Ames Lab., Ames, IA (United States). Critical Materials Inst.
  2. Karlsruhe Inst. of Technology (KIT) (Germany). KIT Steel and Lightweight Structures. Research Center for Steel, Timber and Masonry
  3. Ames Lab. and Iowa State Univ., Ames, IA (United States). Material Science & Engineering
  4. Karlsruhe Inst. of Technology (KIT) (Germany). Inst. of Inorganic Chemistry. Inst. of Nanotechnology; Inst. Neel, Grenoble (France)
  5. Univ. of Strasbourg (France). Dept. of Chemistry
  6. Karlsruhe Inst. of Technology (KIT) (Germany). Inst. of Nanotechnology; Inst. Neel, Grenoble (France)
  7. Karlsruhe Inst. of Technology (KIT) (Germany). Inst. of Inorganic Chemistry
  8. Karlsruhe Inst. of Technology (KIT) (Germany). Inst. of Inorganic Chemistry. Inst. of Nanotechnology
Publication Date:
Report Number(s):
IS-J-9582
Journal ID: ISSN 2050-7526
Grant/Contract Number:
AC02-07CH11358
Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry C
Additional Journal Information:
Journal Volume: 6; Journal Issue: 11; Journal ID: ISSN 2050-7526
Publisher:
Royal Society of Chemistry
Research Org:
Ames Lab. and Iowa State Univ., Ames, IA (United States); Karlsruhe Inst. of Technology (KIT) (Germany)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Advanced Manufacturing Office (EE-5A); Alexander von Humboldt Foundation (Germany); German Research Foundation (DFG)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1425470
Alternate Identifier(s):
OSTI ID: 1434127