Polyimido Sulfur Compounds as Promising Ligands in Molecular Magnets

by Jochen Jung
Doctoral thesis
Date of Examination:2021-11-09
Date of issue:2022-04-08
Advisor:Prof. Dr. Dietmar Stalke
Referee:Prof. Dr. Dietmar Stalke
Referee:Prof. Dr. Franc Meyer
Persistent Address: http://dx.doi.org/10.53846/goediss-9175

 

 

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Abstract

English

Single-molecule magnets (SMMs) are molecules that exhibit slow relaxation of the magnetization after the removal of an applied external field. Therefore, they may find potential application in high density information storage or in the field of quantum computing. The sulfur imido (SN) ligand platform seems to be a promising alternative to the intensively studied ligand systems commonly used for the design of single-molecule magnets. The polar S–N bonds can easily adapt to the electronic and geometric requirements of various metals, offering a wide range of possible coordination complexes and due to their cap-shaped character, they provide a similar steric demand as the cyclopentadienyl ligands. This work aims to investigate the suitability of polyimido sulfur compounds as ligands for the synthesis of molecular magnets. The focus was based on the tetraimido sulfate [S(NtBu)4]2–, to study exchange coupled systems and the triimido sulfonate [Ph2PCH2S(NtBu)3]–, to investigate the influence of soft donor atoms on the magnetic properties. The influence of such ligand designs on the magnetic properties were thoroughly studied for highly anisotropic 3d transition metals like Fe(II) and Co(II) and for 4f elements like Tb(III) and Dy(III). Furthermore, the valence isoelectronic imido analogue H2S(NtBu)4 to sulfuric acid was synthesized, isolated and characterized by NMR spectroscopy and single crystal X-ray diffraction analysis.
Keywords: sulfur nitrogen ligands, single-molecule magnet, slow magnetic relaxation, lanthanide SMMs, 3d transition metal SMMs, tetraimido sulfate, triimido sulfonate
 
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