Issue 9, 2017

Intra-molecular origin of the spin-phonon coupling in slow-relaxing molecular magnets

Abstract

We perform a systematic investigation of the spin-phonon coupling leading to spin relaxation in the prototypical mononuclear single molecule magnet [(tpaPh)Fe]. In particular we analyze in detail the nature of the most relevant vibrational modes giving rise to the relaxation. Our fully ab initio calculations, where the phonon modes are evaluated at the level of density functional theory and the spin-phonon coupling by mapping post-Hartree–Fock electronic structures onto an effective spin Hamiltonian, reveal that acoustic phonons are not active in the spin-phonon relaxation process of dilute SMMs crystals. Furthermore, we find that intra-molecular vibrational modes produce anisotropy tensor modulations orders of magnitude higher than those associated to rotations. In light of these results we are able to suggest new designing rules for spin-long-living SMMs which go beyond the tailoring of static molecular features but fully take into account dynamical features of the vibrational thermal bath evidencing those internal molecular distortions more relevant to the spin dynamics.

Graphical abstract: Intra-molecular origin of the spin-phonon coupling in slow-relaxing molecular magnets

Supplementary files

Article information

Article type
Edge Article
Submitted
26 Jun 2017
Accepted
27 Jul 2017
First published
31 Jul 2017
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., 2017,8, 6051-6059

Intra-molecular origin of the spin-phonon coupling in slow-relaxing molecular magnets

A. Lunghi, F. Totti, S. Sanvito and R. Sessoli, Chem. Sci., 2017, 8, 6051 DOI: 10.1039/C7SC02832F

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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