The role of anharmonic phonons in under-barrier spin relaxation of single molecule magnets

Alessandro Lunghi, Federico Totti, Roberta Sessoli and Stefano Sanvito ()
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Alessandro Lunghi: Università degli Studi di Firenze
Federico Totti: Università degli Studi di Firenze
Roberta Sessoli: Università degli Studi di Firenze
Stefano Sanvito: School of Physics, AMBER and CRANN, Trinity College

Nature Communications, 2017, vol. 8, issue 1, 1-7

Abstract: Abstract The use of single molecule magnets in mainstream electronics requires their magnetic moment to be stable over long times. One can achieve such a goal by designing compounds with spin-reversal barriers exceeding room temperature, namely with large uniaxial anisotropies. Such strategy, however, has been defeated by several recent experiments demonstrating under-barrier relaxation at high temperature, a behaviour today unexplained. Here we propose spin–phonon coupling to be responsible for such anomaly. With a combination of electronic structure theory and master equations we show that, in the presence of phonon dissipation, the relevant energy scale for the spin relaxation is given by the lower-lying phonon modes interacting with the local spins. These open a channel for spin reversal at energies lower than that set by the magnetic anisotropy, producing fast under-barrier spin relaxation. Our findings rationalize a significant body of experimental work and suggest a possible strategy for engineering room temperature single molecule magnets.

Date: 2017
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DOI: 10.1038/ncomms14620

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