A Cost-Effective Semi-Ab Initio Approach to Model Relaxation in Rare-Earth Single-Molecule Magnets

J Phys Chem Lett. 2021 Sep 16;12(36):8826-8832. doi: 10.1021/acs.jpclett.1c02367. Epub 2021 Sep 7.

Abstract

We discuss a cost-effective approach to understand magnetic relaxation in the new generation of rare-earth single-molecule magnets. It combines ab initio calculations of the crystal field parameters, of the magneto-elastic coupling with local modes, and of the phonon density of states with fitting of only three microscopic parameters. Although much less demanding than a fully ab initio approach, the method gives important physical insights into the origin of the observed relaxation. By applying it to high-anisotropy compounds with very different relaxation, we demonstrate the power of the approach and pinpoint ingredients for improving the performance of single-molecule magnets.