Vibronic effects on the quantum tunnelling of magnetisation in Kramers single-molecule magnets.

ABSTRACT: Single-molecule magnets are among the most promising platforms for achieving molecular-scale data storage and processing. Their magnetisation dynamics are determined by the interplay between electronic and vibrational degrees of freedom, which can couple coherently, leading to complex vibronic dynamics. Building on an ab initio description of the electronic and vibrational Hamiltonians, we formulate a non-perturbative vibronic model of the low-energy magnetic degrees of freedom in monometallic single-molecule magnets. Describing their low-temperature magnetism in terms of magnetic polarons, we are able to quantify the vibronic contribution to the quantum tunnelling of the magnetisation, a process that is commonly assumed to be independent of spin-phonon coupling. We find that the formation

SUBMITTER: Mattioni A 

PROVIDER: S-EPMC10784566 | biostudies-literature | 2024 Jan

REPOSITORIES: biostudies-literature