Impact of Finite Phonon Lifetimes on the Spin Dynamics of Single-Molecule Magnets

24 February 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


The development of single-molecule magnets (SMMs) for information storage and processing relies on compounds with long spin lifetimes, and thus requires an understanding of the spin-phonon coupling. The phonon bath itself has a central role in these interactions, and hence knowledge of the impact of the intrinsic phonon lifetimes is crucial. Here we address this challenge by performing fully ab initio calculations of the phonon linewidths for a molecular crystal of a high-performance SMM. We find that the commonly assumed Born-Markov approximation is justified as phonon dynamics are orders of magnitude faster than the spin dynamics, and that employing ab initio-calculated linewidths in spin-dynamics simulations are secondary to employing a dense numerical sampling of the phonon modes in reciprocal space.


Single-molecule magnet
magnetic relaxation

Supplementary materials

Contains supplementary data.


Comments are not moderated before they are posted, but they can be removed by the site moderators if they are found to be in contravention of our Commenting Policy [opens in a new tab] - please read this policy before you post. Comments should be used for scholarly discussion of the content in question. You can find more information about how to use the commenting feature here [opens in a new tab] .
This site is protected by reCAPTCHA and the Google Privacy Policy [opens in a new tab] and Terms of Service [opens in a new tab] apply.