Suppressing Spin–Phonon Relaxation and Enhancing Stability of Dysprosocenium Single-Ion Magnets via Metal-Organic Framework Confinement: A Theoretical Perspective

Abstract

Detailed ab initio CASSCF calculations coupled with periodic density functional theory studies on [(Cp*)Dy(Cp^iPr5)]⁺ molecule encapsulated in a metal-organic framework (MOF) revealed that MOF encapsulation offers stability to these fragile molecules, keeping intact the U_eff (barrier height for magnetization reversal) values. Most importantly, this encapsulation suppresses the key vibrations responsible for reducing the blocking temperature, offering a hitherto unknown strategy for a new generation of SIM-based devices.