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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.citation	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.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.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	journal article	es_ES
dc.date.updated	2021-10-25T13:12:20Z
dc.identifier.doi	10.1021/acs.inorgchem.1c01474
dc.identifier.idgrec	148418
dc.rights.accessRights	open access	es_ES