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Analysis of the Magnetic Exchange Interactions in Yttrium(III) Complexes Containing Nitronyl Nitroxide Radicals. | LitMetric

Analysis of the Magnetic Exchange Interactions in Yttrium(III) Complexes Containing Nitronyl Nitroxide Radicals.

Inorg Chem

Institut des Sciences Chimiques de Rennes, UMR 6226 CNRS, Université de Rennes 1, 263 Avenue du Général Leclerc, 35042 Cedex Rennes, France.

Published: June 2017

AI Article Synopsis

Article Abstract

We report a combined theoretical and experimental investigation of the exchange interactions governing the magnetic behavior of a series of nitronyl nitroxide (NIT)-based Y(III) complexes, i.e., Y(hfac)(NIT-R) with R = PhOPh (1), PhOEt (2), and PhOMe (3a, 3b). Even though some of these complexes or their Dy(III) parents were previously described in the literature [ Zhao et al. Transition Met. Chem. 2006 , 31 , 593 ; Bernot et al. J. Am. Chem. Soc. 2009 , 131 , 5573 ], their synthesis procedure as well as their structural and magnetic properties were completely reconsidered. Depending on the nature of R and the crystallization conditions, Y(hfac)(NIT-R) units can be organized as supramolecular dimers or linear or orthogonal chains. Such structural diversity within the series induces extremely different magnetic behaviors. The observed behaviors are rationalized by state-of-the-art wave function-based quantum-chemical approaches (CASSCF/DDCI) that demonstrate the existence of not only effective intramolecular interactions between the NIT-R radical ligands of an isolated Y(hfac)(NIT-R) molecule but also intermolecular interactions between NIT-R moieties belonging to different Y(hfac)(NIT-R) units. These results are supported by the use of spin Hamiltonian models going beyond the basic Bleaney-Bowers formalism to properly fit the experimental magnetic data. Finally, the microscopic mechanisms behind the evidenced intramolecular exchange interactions are elucidated through the inspection of the calculated wave functions. In particular, whereas the role of Y orbitals was already proposed, we herein demonstrate the contribution of the hfac ancillary ligands in mediating the magnetic interactions between the NIT radicals.

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Source
http://dx.doi.org/10.1021/acs.inorgchem.6b02952DOI Listing

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