Spectroscopic analysis of vibronic relaxation pathways in molecular spin qubit [Ho(W5O18)2]9−: sparse spectra are key
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Spectroscopic analysis of vibronic relaxation pathways in molecular spin qubit [Ho(W5O18)2]9−: sparse spectra are key

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Spectroscopic analysis of vibronic relaxation pathways in molecular spin qubit [Ho(W5O18)2]9−: sparse spectra are key

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dc.contributor.author Blockmon, Avery L.
dc.contributor.author Ullah, Aman
dc.contributor.author Hughey, Kendall D.
dc.contributor.author Duan, Yan
dc.contributor.author O'Neal, Kenneth R.
dc.contributor.author Ozerov, Mykhaylo
dc.contributor.author Baldoví, José J.
dc.contributor.author Aragó, Juan
dc.contributor.author Gaita Ariño, Alejandro
dc.contributor.author Coronado Miralles, Eugenio
dc.contributor.author Musfeldt, Janice L.
dc.date.accessioned 2021-10-25T13:12:20Z
dc.date.available 2021-10-25T13:12:20Z
dc.date.issued 2021
dc.identifier.uri https://hdl.handle.net/10550/80578
dc.description.abstract Vibrations play a prominent role in magnetic relaxation processes of molecular spin qubits as they couple to spin states, leading to the loss of quantum information. Direct experimental determination of vibronic coupling is crucial to understand and control the spin dynamics of these nano-objects, which represent the limit of miniaturization for quantum devices. Herein, we measure the magneto-infrared properties of the molecular spin qubit system Na9[Ho(W5O18)2]·35H2O. Our results place significant constraints on the pattern of crystal field levels and the vibrational excitations allowing us to unravel vibronic decoherence pathways in this system. We observe field-induced spectral changes near 63 and 370 cm-1 that are modeled in terms of odd-symmetry vibrations mixed with f-manifold crystal field excitations. The overall extent of vibronic coupling in Na9[Ho(W5O18)2]·35H2O is limited by a modest coupling constant (on the order of 0.25) and a transparency window in the phonon density of states that acts to keep the intramolecular vibrations and MJ levels apart. These findings advance the understanding of vibronic coupling in a molecular magnet with atomic clock transitions and suggest strategies for designing molecular spin qubits with improved coherence lifetimes.
dc.language.iso eng
dc.relation.ispartof Inorganic Chemistry, 2021, vol. 60, num. 18, p. 14096-14104
dc.rights.uri info:eu-repo/semantics/openAccess
dc.source Blockmon, Avery L. Ullah, Aman Hughey, Kendall D. Duan, Yan O'Neal, Kenneth R. Ozerov, Mykhaylo Baldoví, José J. Aragó, Juan Gaita Ariño, Alejandro Coronado Miralles, Eugenio Musfeldt, Janice L. 2021 Spectroscopic analysis of vibronic relaxation pathways in molecular spin qubit [Ho(W5O18)2]9−: sparse spectra are key Inorganic Chemistry 60 18 14096 14104
dc.subject Cristalls
dc.subject Vibració
dc.title Spectroscopic analysis of vibronic relaxation pathways in molecular spin qubit [Ho(W5O18)2]9−: sparse spectra are key
dc.type info:eu-repo/semantics/article
dc.date.updated 2021-10-25T13:12:20Z
dc.identifier.doi https://doi.org/10.1021/acs.inorgchem.1c01474
dc.identifier.idgrec 148418

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