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

• Published in: Nature communications Vol. 14; no. 1; pp. 1653 - 11
• Main Authors: Garlatti, E., Albino, A., Chicco, S., Nguyen, V. H. A., Santanni, F., Paolasini, L., Mazzoli, C., Caciuffo, R., Totti, F., Santini, P., Sessoli, R., Lunghi, A., Carretta, S.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 24.03.2023; Nature Publishing Group; Nature Portfolio
• Subjects: 639/766/119/997; 639/766/483/2802; 639/766/94; Ambient temperature; Coupling (molecular); Density functional theory; Energy; Humanities and Social Sciences; Inelastic scattering; Investigations; Lattice vibration; Magnetism; multidisciplinary; Neutrons; Phonons; Qubits (quantum computing); Radiation; Science; Science (multidisciplinary); Simulation; Single crystals; Spectrum analysis; Spin dynamics; Vibrations; X-ray scattering; X-rays
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-36852-y

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. Understanding phonon-induced relaxation in molecular qubits is a crucial step in realizing their application potential. Garlatti at al. use a combination of inelastic X-ray scattering and density functional theory to investigate the role of low-energy phonons on spin relaxation of a prototypical molecular qubit.