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Validation of Ab‐Initio‐Predicted Magnetic Anisotropies and Magneto‐structural Correlations in Linear Hetero‐trinuclear Dy III ‐Ni II 2 Compounds
Author(s) -
Comba Peter,
Enders Markus,
Großhauser Michael,
Hiller Markus,
Klingeler Rüdiger,
Koo Changhyun,
Müller Dennis,
Rajaraman Gopalan,
Swain Abinash,
Tavhelidse Msia,
Wadepohl Hubert
Publication year - 2021
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202100626
Subject(s) - ab initio , ab initio quantum chemistry methods , electron paramagnetic resonance , chemistry , ground state , wave function , anisotropy , paramagnetism , single crystal , molecular physics , atomic physics , crystallography , molecule , condensed matter physics , nuclear magnetic resonance , physics , quantum mechanics , organic chemistry
Reported are single crystal SQUID and single crystal high‐frequency/high‐field EPR data of a trinuclear complex with a rare six‐coordinate coordination sphere of a Dy III center coupled to two terminal six‐coordinate Ni II ions. The analysis of the single crystal spectroscopic parameters allows for an accurate description of the ground state wavefunction. The experimental analysis is supplemented by the analysis of the paramagnetic NMR spectra, allowing for a thorough description of the Dy III center. The experimental data are interpreted on the basis of an ab initio ligand field analysis, and the computed parameters are in good agreement with the experimental observations. This supports the quality of the theoretical approach based on a pseudo‐spin Hamiltonian for the electronic ground state. Further support emerges from the ab initio ligand field theory based analysis of a structurally very similar system that, in contrast to the complex reported here, shows single molecule magnetic properties, and this is in agreement with the quantum‐chemical prediction and analysis.