Black-box determination of temperature-dependent susceptibilities for crystalline organic radicals with complex magnetic topologies

Literature Information

Publication Date 2016-10-03
DOI 10.1039/C6CP05875B
Impact Factor 3.676
Authors

Steffen Eusterwiemann, David R. Matuschek, Constantin G. Daniliuc, Oliver Janka, Rainer Pöttgen, Armido Studer


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Abstract

In all but the simplest crystal structures, the identification of all relevant interactions between magnetic sites as well as the setup of magnetic model spaces, which are necessary for modeling macroscopic magnetism, are tedious and error-prone tasks. Here, we present a procedure to generate magnetic susceptibility versus temperature curves using only a crystal structure as input. The procedure, which is based on the first-principles bottom-up approach [Deumal et al., J. Phys. Chem. A, 2002, 106, 1299], is designed in a way to require as little user interference as possible. We employ quantum chemical calculations to parametrize a Heisenberg Hamiltonian, which is set up and diagonalized for different magnetic model spaces to ensure convergence of the model. We apply the procedure to several 6-oxo-verdazyl radical structures, including newly synthesized compounds, and compare the results to data we obtained from magnetic susceptibility measurements as well as published data to further benchmark our procedure. Furthermore, the different impact of certain dominating coupling constants is systematically analyzed.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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