Temperature Dependence of Spin-Phonon Coupling in [VO(acac)2]: A Computational and Spectroscopic Study
Year: 2021
Authors: Albino A., Benci S., Atzori M., Chelazzi L., Ciattini S., Taschin A., Bartolini P., Lunghi A., Righini R., Torre R., Totti F., Sessoli R.
Autors Affiliation: Univ Firenze, Dipartimento Chim Ugo Schiff, I-50019 Florence, Italy; Univ Firenze, INSTM RU, I-50019 Florence, Italy; Univ Firenze, European Lab Nonlinear Spect LENS, I-50019 Florence, Italy; Univ Toulouse Paul Sabatier, Univ Grenoble Alpes, INSA Toulouse, Lab Natl Champs Magnet Intenses LNCMI,EMFL,CNRS, F-38043 Grenoble, France; Univ Firenze, Ctr Crystallog, I-50019 Florence, Italy; Agenzia Nazl Nuove Tecnol Energia & Sviluppo Econ, Ctr Ric Frascati, ENEA, I-00044 Rome, Italy; Trinity Coll Dublin, Sch Phys, AMBER, Dublin 2, Ireland; Trinity Coll Dublin, Sch Phys, CRANN Inst, Dublin 2, Ireland; Univ Firenze, Dipartimento Fis Astron, I-50019 Florence, Italy.
Abstract: Molecular electronic spins are good candidates as qubits since they are characterized by a large tunability of their electronic and magnetic properties through a rational chemical design. Coordination compounds of light transition metals are promising systems for spin-based quantum information technologies, thanks to their long spin coherence times up to room temperature. Our work aims at presenting an in-depth study on how the spin-phonon coupling in vanadyl-acetylacetonate, [VO(acac)(2)], can change as a function of temperature using terahertz time-domain spectroscopy and density functional theory (DFT) calculations. Powder THz spectra were recorded between 10 and 300 K. The temperature dependence of vibrational frequencies was then accounted for in the periodic DFT calculations using unit-cell parameters measured at two different temperatures and the optimized ones, as usually reported in the literature. In this way, it was possible to calculate the observed THz anharmonic frequency shift with high accuracy. The overall differences in the spin-phonon coupling magnitudes as a function of temperature were also highlighted showing that the computed trends have to be ascribed to the anisotropic variation of cell parameters.
Journal/Review: JOURNAL OF PHYSICAL CHEMISTRY C
Volume: 125 (40) Pages from: 22100 to: 22110
More Information: Financial support by the EU Commission through the QuantERA Project SUMO by the FETOPEN project FATMOLS (GA 862893), by Ente Cassa di Risparmio firenze (prog. 2018.1042), Ministero dell’Istruzione dell’Universita e della Ricerca Italiano (PRIN2017-2017Z55KCW), and by European Union’s Horizon 2020 research and innovation program under grant agreement no. 871124 Laserlab-Europe are acknowledged. The computing resources and the related technical support used for this work have been provided by CRESCO/ENEAGRID High Performance Computing infrastructure and its staff.61 CRESCO/ENEAGRID High Performance Computing infrastructure is funded by ENEA, the Italian National Agency for New Technologies, Energy and Sustainable Economic Development and by the Italian and European research programs, see http://www.cresco.enea.it/english for information.KeyWords: Density-functional Theory; Vibrational-relaxation; Pseudopotentials; Dynamics; Qubits; TimeDOI: 10.1021/acs.jpcc.1c06916ImpactFactor: 4.177Citations: 18data from “WEB OF SCIENCE” (of Thomson Reuters) are update at: 2024-11-10References taken from IsiWeb of Knowledge: (subscribers only)
