Pushing the frontiers of paramagnetic NMR spectroscopy for f-element compounds

The calculation and interpretation of magnetic-resonance parameters for open-shell f-element compounds remain challenging because of the large influence of spin-orbit coupling and thermally accessible excited states. The use of state-of-the-art approaches is hampered by the presence of large zero-field splitting and the multi-reference electronic character of these systems. In this project we will develop new computational protocols for the calculation, analysis, and interpretation of paramagnetic NMR shifts for lanthanide compounds. The developed methods will be calibrated to experimental EPR/NMR measurements and used to elucidate the structure and analyze the magnetic properties of contrast agents for imaging and molecular magnets. The results of the project will push the current frontiers of paramagnetic NMR spectroscopy.