Identification of Favorable Silica Surface Sites for Single‐Molecule Magnets

Industrial data storage application based on single‐molecule magnets (SMMs) necessitates not only strong magnetic remanence at high temperatures but also requires the implementation of SMMs into a solid material to increase their durability and addressability. While the understanding of the relation...

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Bibliographic Details
Published in:Helvetica chimica acta 2023-11, Vol.106 (11), p.n/a
Main Authors: Bernhardt, Moritz, Lätsch, Lukas, Le Guennic, Boris, Copéret, Christophe
Format: Article
Language:English
Subjects:
Chemical Sciences
computational chemistry
Coordination numbers
Data storage
Dispersion
Durability
High temperature
Ions
lanthanide
Ligands
Low temperature
Magnetic induction
Magnetic materials
Magnetic properties
Magnetic relaxation
Magnets
Organometallic compounds
Remanence
Silica
Silicon dioxide
single-molecule magnetism
single-molecule studies
surface chemistry
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Summary:Industrial data storage application based on single‐molecule magnets (SMMs) necessitates not only strong magnetic remanence at high temperatures but also requires the implementation of SMMs into a solid material to increase their durability and addressability. While the understanding of the relationship between the local structure of the metal and the resulting magnetic behavior is well understood in molecular systems, it remains challenging to establish a similar understanding for magnetic materials, especially for isolated lanthanide sites on surfaces. For instance, dispersed Dy(III) ions on silica prepared via surface organometallic chemistry exhibit slow magnetic relaxation at low temperatures, but the origin of these properties remains unclear. In this work, we modelled ten neutral complexes with coordination numbers (CN) between three and six ([Dy(OSiF3)3(O(SiF3)2)CN‐3]) representing possible surface sites for dispersed Dy(III) ions and investigated their SMM potential via ab initio CASSCF/RASSI‐SO calculations. Detailed analysis of the data shows the strong influence of the spatial position of the anionic ligands while the neutral ligands only play a minor role for the magnetic properties. In particular, a T‐shape like orientation of the anionic ligands is predicted to exhibit good SMM properties making it a promising targeted coordination environment for molecular and surface‐based SMMs.
ISSN:0018-019X
1522-2675
DOI:10.1002/hlca.202300130