Issue 28, 2025

The mechanism of spin-phonon relaxation in endohedral metallofullerene single molecule magnets

Abstract

This study presents the investigation of spin-phonon coupling mechanisms in fullerene-based single-molecule magnets (SMMs) using ab initio CASSCF combined with DFT calculations. While lanthanide-based SMMs, particularly those with DyIII ions, are known for their impressive blocking temperatures and relaxation barriers, endohedral metallofullerene (EMFs) offer a unique platform for housing low-coordinated lanthanides within rigid carbon cages. We have explored the spin dynamics in DyScS@C82 exhibiting among the highest blocking temperature (TB) reported. Through our computational analysis, we reveal that while the fullerene cage enhances crystal field splitting and provides structural stability without significantly contributing to spin-relaxation driving low-energy phonons, the internal ionic motion emerges as the primary factor controlling spin relaxation and limiting blocking temperature. This computational investigation into the spin dynamics of EMF-based SMMs provides key insights into their magnetic behaviour and suggests potential strategies for improving their performance towards futuristic SMMs.

Graphical abstract: The mechanism of spin-phonon relaxation in endohedral metallofullerene single molecule magnets

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Article information

Article type
Edge Article
Submitted
16 Pun 2024
Accepted
07 Jan 2025
First published
09 Jan 2025
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2025,16, 13012-13021

The mechanism of spin-phonon relaxation in endohedral metallofullerene single molecule magnets

T. Sharma, R. K. Tiwari, S. Dey, L. A. Mariano, A. Lunghi and G. Rajaraman, Chem. Sci., 2025, 16, 13012 DOI: 10.1039/D4SC07786E

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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