The recent discovery of single-ion magnets with magnetic hysteresis above liquid-nitrogen temperatures placed these compounds among the best candidates to realize high-density storage devices. Starting from a prototypical dysprosocenium molecule, showing hysteresis up to 60 K, we derive here a general recipe to design high-blocking-temperature rare-earth single-ion magnets. The complex magnetic relaxation is unraveled by combining magnetization and nuclear magnetic resonance measurements with inelastic neutron scattering experiments and ab initio calculations, thus disentangling the different mechanisms and identifying the key ingredients behind slow relaxation.

• Received 28 November 2019
• Accepted 16 March 2020

DOI:https://doi.org/10.1103/PhysRevB.101.174402

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society