Beyond Bleaney’s Theory: Experimental and Theoretical Analysis of Periodic Trends in Lanthanide Induced Chemical Shift
A detailed analysis of paramagnetic NMR shifts in a series of isostructural lanthanide complexes relavant to PARASHIFT con- trast agents reveals unexpected trends in the magnetic susceptibility anisotropy that cannot be explained by the commonly used Bleaney’s theory. Ab initio calculations reveal that the primary as- sumption of Bleaney’s theory – that thermal energy is larger than the ligand field splitting – does not hold for the lanthanide complexes in question, and likely for a large fraction of lanthanide complexes in general. This makes the orientation of the magnetic susceptibility tensor differ significantly between complexes of different lanthanides with the same ligand: one of the most popular assumptions about isostructural lanthanide series is wrong.
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