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Spin–phonon couplings in transition metal complexes with slow magnetic relaxation

Author

Listed:
  • Duncan H. Moseley

    (University of Tennessee)

  • Shelby E. Stavretis

    (University of Tennessee)

  • Komalavalli Thirunavukkuarasu

    (Florida A&M University)

  • Mykhaylo Ozerov

    (National High Magnetic Field Laboratory)

  • Yongqiang Cheng

    (Oak Ridge National Laboratory)

  • Luke L. Daemen

    (Oak Ridge National Laboratory)

  • Jonathan Ludwig

    (National High Magnetic Field Laboratory)

  • Zhengguang Lu

    (National High Magnetic Field Laboratory)

  • Dmitry Smirnov

    (National High Magnetic Field Laboratory)

  • Craig M. Brown

    (National Institute of Standards and Technology)

  • Anup Pandey

    (Oak Ridge National Laboratory)

  • A. J. Ramirez-Cuesta

    (Oak Ridge National Laboratory)

  • Adam C. Lamb

    (University of Tennessee)

  • Mihail Atanasov

    (Max Planck Institute for Coal Research
    Bulgarian Academy of Sciences)

  • Eckhard Bill

    (Max Planck Institute for Chemical Energy Conversion)

  • Frank Neese

    (Max Planck Institute for Coal Research)

  • Zi-Ling Xue

    (University of Tennessee)

Abstract

Spin–phonon coupling plays an important role in single-molecule magnets and molecular qubits. However, there have been few detailed studies of its nature. Here, we show for the first time distinct couplings of g phonons of CoII(acac)2(H2O)2 (acac = acetylacetonate) and its deuterated analogs with zero-field-split, excited magnetic/spin levels (Kramers doublet (KD)) of the S = 3/2 electronic ground state. The couplings are observed as avoided crossings in magnetic-field-dependent Raman spectra with coupling constants of 1–2 cm−1. Far-IR spectra reveal the magnetic-dipole-allowed, inter-KD transition, shifting to higher energy with increasing field. Density functional theory calculations are used to rationalize energies and symmetries of the phonons. A vibronic coupling model, supported by electronic structure calculations, is proposed to rationalize the behavior of the coupled Raman peaks. This work spectroscopically reveals and quantitates the spin–phonon couplings in typical transition metal complexes and sheds light on the origin of the spin–phonon entanglement.

Suggested Citation

  • Duncan H. Moseley & Shelby E. Stavretis & Komalavalli Thirunavukkuarasu & Mykhaylo Ozerov & Yongqiang Cheng & Luke L. Daemen & Jonathan Ludwig & Zhengguang Lu & Dmitry Smirnov & Craig M. Brown & Anup , 2018. "Spin–phonon couplings in transition metal complexes with slow magnetic relaxation," Nature Communications, Nature, vol. 9(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-04896-0
    DOI: 10.1038/s41467-018-04896-0
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    Cited by:

    1. E. Garlatti & A. Albino & S. Chicco & V. H. A. Nguyen & F. Santanni & L. Paolasini & C. Mazzoli & R. Caciuffo & F. Totti & P. Santini & R. Sessoli & A. Lunghi & S. Carretta, 2023. "The critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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