title: Black-box determination of temperature-dependent susceptibilities for crystalline organic radicals with complex magnetic topologies.
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.
authors.affiliation: Organisch-Chemisches Institut, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, 48149 Münster, Germany. j.neugebauer@uni-muenster.de and Center for Multiscale Theory and Computation, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, 48149 Münster, Germany.
authors.forename: Thomas
authors.initials: T
authors.lastname: Dresselhaus
authors.affiliation: Organisch-Chemisches Institut, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, 48149 Münster, Germany. j.neugebauer@uni-muenster.de.
authors.forename: Steffen
authors.initials: S
authors.lastname: Eusterwiemann
authors.affiliation: Organisch-Chemisches Institut, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, 48149 Münster, Germany. j.neugebauer@uni-muenster.de.
authors.forename: David R
authors.initials: DR
authors.lastname: Matuschek
authors.affiliation: Organisch-Chemisches Institut, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, 48149 Münster, Germany. j.neugebauer@uni-muenster.de.
authors.forename: Constantin G
authors.initials: CG
authors.lastname: Daniliuc
authors.affiliation: Institut für Anorganische und Analytische Chemie, Westfälische Wilhelms-Universität Münster, Corrensstraße 28/30, 48149 Münster, Germany.
authors.forename: Oliver
authors.initials: O
authors.lastname: Janka
authors.affiliation: Institut für Anorganische und Analytische Chemie, Westfälische Wilhelms-Universität Münster, Corrensstraße 28/30, 48149 Münster, Germany.
authors.forename: Rainer
authors.initials: R
authors.lastname: Pöttgen
authors.affiliation: Organisch-Chemisches Institut, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, 48149 Münster, Germany. j.neugebauer@uni-muenster.de.
authors.forename: Armido
authors.initials: A
authors.lastname: Studer
authors.affiliation: Organisch-Chemisches Institut, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, 48149 Münster, Germany. j.neugebauer@uni-muenster.de and Center for Multiscale Theory and Computation, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, 48149 Münster, Germany.
authors.forename: Johannes
authors.initials: J
authors.lastname: Neugebauer