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The critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits

Author

Listed:
  • E. Garlatti

    (Università di Parma and UdR Parma, INSTM
    INFN, Sezione di Milano-Bicocca, gruppo collegato di Parma)

  • A. Albino

    (Università Degli Studi di Firenze and UdR Firenze, INSTM)

  • S. Chicco

    (Università di Parma and UdR Parma, INSTM)

  • V. H. A. Nguyen

    (Trinity College)

  • F. Santanni

    (Università Degli Studi di Firenze and UdR Firenze, INSTM)

  • L. Paolasini

    (ESRF - The European Synchrotron Radiation Facility)

  • C. Mazzoli

    (Brookhaven National Laboratory)

  • R. Caciuffo

    (INFN, Sezione di Genova)

  • F. Totti

    (Università Degli Studi di Firenze and UdR Firenze, INSTM)

  • P. Santini

    (Università di Parma and UdR Parma, INSTM
    INFN, Sezione di Milano-Bicocca, gruppo collegato di Parma)

  • R. Sessoli

    (Università Degli Studi di Firenze and UdR Firenze, INSTM)

  • A. Lunghi

    (Trinity College)

  • S. Carretta

    (Università di Parma and UdR Parma, INSTM
    INFN, Sezione di Milano-Bicocca, gruppo collegato di Parma)

Abstract

Improving the performance of molecular qubits is a fundamental milestone towards unleashing the power of molecular magnetism in the second quantum revolution. Taming spin relaxation and decoherence due to vibrations is crucial to reach this milestone, but this is hindered by our lack of understanding on the nature of vibrations and their coupling to spins. Here we propose a synergistic approach to study a prototypical molecular qubit. It combines inelastic X-ray scattering to measure phonon dispersions along the main symmetry directions of the crystal and spin dynamics simulations based on DFT. We show that the canonical Debye picture of lattice dynamics breaks down and that intra-molecular vibrations with very-low energies of 1-2 meV are largely responsible for spin relaxation up to ambient temperature. We identify the origin of these modes, thus providing a rationale for improving spin coherence. The power and flexibility of our approach open new avenues for the investigation of magnetic molecules with the potential of removing roadblocks toward their use in quantum devices.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36852-y
    DOI: 10.1038/s41467-023-36852-y
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    References listed on IDEAS

    as
    1. N. Bar-Gill & L.M. Pham & A. Jarmola & D. Budker & R.L. Walsworth, 2013. "Solid-state electronic spin coherence time approaching one second," Nature Communications, Nature, vol. 4(1), pages 1-6, June.
    2. E. Garlatti & L. Tesi & A. Lunghi & M. Atzori & D. J. Voneshen & P. Santini & S. Sanvito & T. Guidi & R. Sessoli & S. Carretta, 2020. "Unveiling phonons in a molecular qubit with four-dimensional inelastic neutron scattering and density functional theory," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    3. Jesús Ferrando-Soria & Eufemio Moreno Pineda & Alessandro Chiesa & Antonio Fernandez & Samantha A. Magee & Stefano Carretta & Paolo Santini & Iñigo J. Vitorica-Yrezabal & Floriana Tuna & Grigore A. Ti, 2016. "A modular design of molecular qubits to implement universal quantum gates," Nature Communications, Nature, vol. 7(1), pages 1-10, September.
    4. E. Garlatti & T. Guidi & S. Ansbro & P. Santini & G. Amoretti & J. Ollivier & H. Mutka & G. Timco & I. J. Vitorica-Yrezabal & G. F. S. Whitehead & R. E. P. Winpenny & S. Carretta, 2017. "Portraying entanglement between molecular qubits with four-dimensional inelastic neutron scattering," Nature Communications, Nature, vol. 8(1), pages 1-7, April.
    5. 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.
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