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Analysis of vibronic coupling in a 4f molecular magnet with FIRMS

Author

Listed:
  • Jon G. C. Kragskow

    (University of Manchester)

  • Jonathan Marbey

    (National High Magnetic Field Laboratory
    Florida State University)

  • Christian D. Buch

    (University of Copenhagen)

  • Joscha Nehrkorn

    (National High Magnetic Field Laboratory)

  • Mykhaylo Ozerov

    (National High Magnetic Field Laboratory)

  • Stergios Piligkos

    (University of Copenhagen)

  • Stephen Hill

    (National High Magnetic Field Laboratory
    Florida State University)

  • Nicholas F. Chilton

    (University of Manchester)

Abstract

Vibronic coupling, the interaction between molecular vibrations and electronic states, is a fundamental effect that profoundly affects chemical processes. In the case of molecular magnetic materials, vibronic, or spin-phonon, coupling leads to magnetic relaxation, which equates to loss of magnetic memory and loss of phase coherence in molecular magnets and qubits, respectively. The study of vibronic coupling is challenging, and most experimental evidence is indirect. Here we employ far-infrared magnetospectroscopy to directly probe vibronic transitions in [Yb(trensal)] (where H3trensal = 2,2,2-tris(salicylideneimino)trimethylamine). We find intense signals near electronic states, which we show arise due to an “envelope effect” in the vibronic coupling Hamiltonian, which we calculate fully ab initio to simulate the spectra. We subsequently show that vibronic coupling is strongest for vibrational modes that simultaneously distort the first coordination sphere and break the C3 symmetry of the molecule. With this knowledge, vibrational modes could be identified and engineered to shift their energy towards or away from particular electronic states to alter their impact. Hence, these findings provide new insights towards developing general guidelines for the control of vibronic coupling in molecules.

Suggested Citation

  • Jon G. C. Kragskow & Jonathan Marbey & Christian D. Buch & Joscha Nehrkorn & Mykhaylo Ozerov & Stergios Piligkos & Stephen Hill & Nicholas F. Chilton, 2022. "Analysis of vibronic coupling in a 4f molecular magnet with FIRMS," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28352-2
    DOI: 10.1038/s41467-022-28352-2
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    References listed on IDEAS

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