A Cost-Effective Semi-Ab Initio Approach to Model Relaxation in Rare-Earth Single-Molecule Magnets
Elena Garlatti, Alessandro Chiesa, Pietro Bonfà, Emilio Macaluso, Ifeanyi John Onuorah, Vijay S. Parmar, You‐Song Ding, Yan‐Zhen Zheng, Marcus J. Giansiracusa, Daniel Reta, Eva Pavarini, T. Guidi, David P. Mills, Nicholas F. Chilton, Richard E. P. Winpenny, P. Santini, Stefano Carretta
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.