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Issue 40, 2019
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How to link theory and experiment for single-chain magnets beyond the Ising model: magnetic properties modeled from ab initio calculations of molecular fragments

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Abstract

Magnetic properties of coordination polymers like single-chain magnets (SCMs) are based on magnetic domains, which are formed due to magnetic exchange between neighboring anisotropic spin centers. However, the computational restrictions imposed by the high level of theory needed for an adequate ab initio quantum mechanical treatment on the basis of multi-reference methods for these systems limit the feasibility of such calculations to mononuclear fragments as appropriate structural cutouts for the metal centers along the chains. Hence, results from such calculations describe single-ion properties and cannot be directly correlated with experimental data representing magnetic domains. We present a theoretical approach based on n-membered Ising-spin rings with n = 3–12, which allows us to simulate magnetic domains and to derive important magnetic properties for SCM compounds. Magnetic exchange, which is not provided by calculations of mononuclear fragments, is obtained by fitting the theoretical magnetic susceptibility against experimental data. The presented approach is tested for cobalt(II)-based SCMs with three types of repeating sequences, which differ in nuclearity and symmetry. The magnetic parameters derived using the presented approach were found to be in good agreement with the experimental data. Moreover, the energy spectra obtained for the three test cases using the presented approach are characteristic of a deviation of the individual systems from the ideal Ising behavior. An extrapolation technique towards larger systems (n > 12) is presented which can provide information on the statistical mean length of the magnetic domains in the three investigated SCM compounds.

Graphical abstract: How to link theory and experiment for single-chain magnets beyond the Ising model: magnetic properties modeled from ab initio calculations of molecular fragments

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Publication details

The article was received on 04 Jun 2019, accepted on 15 Aug 2019 and first published on 19 Aug 2019


Article type: Edge Article
DOI: 10.1039/C9SC02735A
Chem. Sci., 2019,10, 9189-9202
  • Open access: Creative Commons BY license
    All publication charges for this article have been paid for by the Royal Society of Chemistry

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    How to link theory and experiment for single-chain magnets beyond the Ising model: magnetic properties modeled from ab initio calculations of molecular fragments

    M. Böhme and W. Plass, Chem. Sci., 2019, 10, 9189
    DOI: 10.1039/C9SC02735A

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