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

Employing periodic density functional theory and ab initio CASSCF calculations, this study proposess a way forward to stabilize dysprosocenium SIMs by encapsulating them in a metal-organic framework, which not only offers stability but also is found to tune spin-vibrational coupling – a parameter hard to control at present.

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.

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