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Element specific determination of the magnetic properties of two macrocyclic tetranuclear 3d–4f complexes with a Cu3Tb core by means of X-ray magnetic circular dichroism (XMCD)

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Abstract

We apply X-ray magnetic circular dichroism to study the internal magnetic structure of two very promising star shaped macrocyclic complexes with a CuII3TbIII core. These complexes are rare examples prepared with a macrocyclic ligand that show indications of SMM (Single Molecule Magnet) behavior, and they differ only in ring size: one has a propylene linked macrocycle, [CuII3TbIII(LPr)(NO3)2(MeOH)(H2O)2](NO3)·3H2O (nickname: Cu3Tb(LPr)), and the other has the butylene linked analogue, [CuII3TbIII(LBu)(NO3)2(MeOH)(H2O)](NO3)·3H2O (nickname: Cu3Tb(LBu)). We analyze the orbital and spin contributions to the Cu and Tb ions quantitatively by applying the spin and orbital sum rules concerning the L2 (M4)/L3 (M5) edges. In combination with appropriate ligand field simulations, we demonstrate that the Tb(III) ions contribute with high orbital magnetic moments to the magnetic anisotropy, whereas the ligand field determines the easy axis of magnetization. Furthermore, we confirm that the Cu(II) ions in both molecules are in a divalent valence state, the magnetic moments of the three Cu ions appear to be canted due to 3d–3d intramolecular magnetic interactions. For Cu3Tb(LPr), the corresponding element specific magnetization loops reflect that the Cu(II) contribution to the overall magnetic picture becomes more important as the temperature is lowered. This implies a low value for the 3d–4f coupling.

Graphical abstract: Element specific determination of the magnetic properties of two macrocyclic tetranuclear 3d–4f complexes with a Cu3Tb core by means of X-ray magnetic circular dichroism (XMCD)

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Publication details

The article was received on 29 Dec 2017, accepted on 29 May 2018 and first published on 08 Jun 2018


Article type: Paper
DOI: 10.1039/C7CP08689J
Citation: Phys. Chem. Chem. Phys., 2018, Advance Article
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    Element specific determination of the magnetic properties of two macrocyclic tetranuclear 3d–4f complexes with a Cu3Tb core by means of X-ray magnetic circular dichroism (XMCD)

    K. Balinski, L. Schneider, J. Wöllermann, A. Buling, L. Joly, C. Piamonteze, H. L. C. Feltham, S. Brooker, A. K. Powell, B. Delley and K. Kuepper, Phys. Chem. Chem. Phys., 2018, Advance Article , DOI: 10.1039/C7CP08689J

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