Magnetic Anisotropy of Mononuclear Ni-II Complexes: On the Importance of Structural Diversity and the Structural Distortions
DSpace at IIT Bombay
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Title |
Magnetic Anisotropy of Mononuclear Ni-II Complexes: On the Importance of Structural Diversity and the Structural Distortions
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Creator |
SINGH, SK
GUPTA, T BADKUR, P RAJARAMAN, G |
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Subject |
CASSCF calculations
magnetic anisotropy nickel magneto-structural correlations zero-field splitting SINGLE-MOLECULE MAGNETS TRANSITION-METAL-COMPLEXES DENSITY-FUNCTIONAL THEORY ZERO-FIELD SPLITTINGS HETEROLEPTIC NICKEL(II) COMPLEXES SPIN-HAMILTONIAN PARAMETERS STATE PERTURBATION-THEORY NI(II) COMPLEXES COORDINATION-COMPLEXES LANTHANIDE COMPLEXES |
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Description |
Mononuclear Ni-II complexes are particularly attractive in the area of single-molecule magnets as the axial zero-field splitting (D) for the Ni-II complexes is in the range of -200 to +200cm(-1). Despite this advantage, very little is known on the origin of anisotropy across various coordination ligands, coordination numbers, and particularly what factors influence the D parameter in these complexes. To answer some of these questions, herein we have undertaken a detailed study of a series of mononuclear Ni-II complexes with ab initio calculations. Our results demonstrate that three prominent spin-conserved low-lying d-d transitions contribute significantly to the D value. Variation in the sign and the magnitude of D values are found to correlate to the specific structural distortions. Apart from the metal-ligand bond lengths, two different parameters, namely, and , which are correlated to the cis angles present in the coordination environment, are found to significantly influence the axial D values. Developed magneto-structural D correlations suggest that the D values can be enhanced significantly by fine tuning the structural distortion in the coordination environment. Calculations performed on a series of Ni-II models with coordination numbers two to six unfold an interesting observationthe D parameter increases significantly upon a reduction in coordination number compared with a reference octahedral coordination. Besides, if high symmetry is maintained, even larger coordination numbers yield large D values.
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Publisher |
WILEY-V C H VERLAG GMBH
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Date |
2014-12-28T12:46:13Z
2014-12-28T12:46:13Z 2014 |
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Type |
Article
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Identifier |
CHEMISTRY-A EUROPEAN JOURNAL, 20(33)10305-10313
0947-6539 1521-3765 http://dx.doi.org/10.1002/chem.201402694 http://dspace.library.iitb.ac.in/jspui/handle/100/16590 |
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Language |
English
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