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Theoretical Studies on Polynuclear {CuII5GdIIIn} Clusters (n = 4, 2): Towards Understanding Their Large Magnetocaloric Effect

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    Theoretical Studies on Polynuclear {CuII5GdIIIn} Clusters (n = 4, 2): Towards Understanding Their Large Magnetocaloric Effect
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    † Department of Chemistry, Indian Institute of Technology Bombay, Powai, Mumabi 400076, India
    § Instituto de Ciencia de Materiales de Aragón and Departamento de Física de la Materia Condensada, CSIC-Universidad de Zaragoza, 50009 Zaragoza, Spain
    ‡ School of Chemistry, Monash University, Clayton, Victoria 3800, Australia
    ⊥ School of Chemistry, The University of Manchester, Manchester M13 9PL, United Kingdom
    *Fax: (+91)-22-2576-7152. Tel: (+91)-22-2576-7183. E-mail: [email protected]
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2015, 54, 4, 1661–1670
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    https://doi.org/10.1021/ic502651w
    Published January 23, 2015
    Copyright © 2015 American Chemical Society
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    Abstract

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    Density functional theory (DFT) studies on two polynuclear clusters, [CuII5GdIII4O2(OMe)4(teaH)4(O2CC(CH3)3)2(NO3)4] (1) and [Cu5Gd2(OH)4(Br)2-(H2L)2(H3L)2(NO3)2(OH2)4] (2), have been carried out to probe the origin of the large magnetocaloric effect (MCE). The magnetic exchange interactions for 1 and 2 via multiple pathways are estimated using DFT calculations. While the calculated exchange parameters deviate from previous experimental estimates obtained by fitting the magnetic data, the DFT parameter set is found to offer a striking match to the magnetic data for both complexes, highlighting the problem of overparameterization. Magnetostructural correlations for {Cu–Gd} pairs have been developed where both the Cu–O–Gd angles and Cu–O–Gd–O dihedral angles are found to significantly influence the magnitude and sign of the exchange constants. The magnitude of the MCE has been examined as a function of the exchange interactions, and clues on how the effect can be enhanced are discussed.

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    Information such as spin density plots, overlap integral values, selected structural parameters corresponding to each J values, dinuclear models for each J values, simulated magnetic susceptibility vs temperature data of 2 etc. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cite this: Inorg. Chem. 2015, 54, 4, 1661–1670
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    https://doi.org/10.1021/ic502651w
    Published January 23, 2015
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