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

Author

Listed:
  • Andrea Mattioni

    (The University of Manchester)

  • Jakob K. Staab

    (The University of Manchester)

  • William J. A. Blackmore

    (The University of Manchester)

  • Daniel Reta

    (The University of Manchester
    The University of the Basque Country UPV/EHU
    Donostia International Physics Center (DIPC)
    IKERBASQUE, Basque Foundation for Science)

  • Jake Iles-Smith

    (The University of Manchester)

  • Ahsan Nazir

    (The University of Manchester)

  • Nicholas F. Chilton

    (The University of Manchester)

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 of magnetic polarons lowers the tunnelling probability in both amorphous and crystalline systems by stabilising the low-lying spin states. This work, thus, shows that spin-phonon coupling subtly influences magnetic relaxation in single-molecule magnets even at extremely low temperatures where no vibrational excitations are present.

Suggested Citation

  • Andrea Mattioni & Jakob K. Staab & William J. A. Blackmore & Daniel Reta & Jake Iles-Smith & Ahsan Nazir & Nicholas F. Chilton, 2024. "Vibronic effects on the quantum tunnelling of magnetisation in Kramers single-molecule magnets," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-023-44486-3
    DOI: 10.1038/s41467-023-44486-3
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    References listed on IDEAS

    as
    1. Michael N. Leuenberger & Daniel Loss, 2001. "Quantum computing in molecular magnets," Nature, Nature, vol. 410(6830), pages 789-793, April.
    2. Roberta Sessoli, 2017. "Magnetic molecules back in the race," Nature, Nature, vol. 548(7668), pages 400-401, August.
    3. Kilian Irländer & Heinz-Jürgen Schmidt & Jürgen Schnack, 2021. "Supersymmetric spin–phonon coupling prevents odd integer spins from quantum tunneling," The European Physical Journal B: Condensed Matter and Complex Systems, Springer;EDP Sciences, vol. 94(3), pages 1-10, March.
    4. Conrad A. P. Goodwin & Fabrizio Ortu & Daniel Reta & Nicholas F. Chilton & David P. Mills, 2017. "Molecular magnetic hysteresis at 60 kelvin in dysprosocenium," Nature, Nature, vol. 548(7668), pages 439-442, August.
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