Chemical tuning of spin clock transitions in molecular monomers based on nuclear spin-free Ni(ii)

Rubín-Osanz M. ; Lambert F. ; Shao F. ; Rivière E. ; Guillot R. ; Suaud N. ; Guihéry N. ; Zueco D. ; Barra A.-L. ; Mallah T. ; Luis F.

Resumen: We report the existence of a sizeable quantum tunnelling splitting between the two lowest electronic spin levels of mononuclear Ni complexes. The level anti-crossing, or magnetic “clock transition”, associated with this gap has been directly monitored by heat capacity experiments. The comparison of these results with those obtained for a Co derivative, for which tunnelling is forbidden by symmetry, shows that the clock transition leads to an effective suppression of intermolecular spin-spin interactions. In addition, we show that the quantum tunnelling splitting admits a chemical tuningviathe modification of the ligand shell that determines the crystal field and the magnetic anisotropy. These properties are crucial to realize model spin qubits that combine the necessary resilience against decoherence, a proper interfacing with other qubits and with the control circuitry and the ability to initialize them by cooling.

Idioma: Inglés

DOI: 10.1039/d0sc05856d

Año: 2021

Publicado en: CHEMICAL SCIENCE 12, 14 (2021), 5123-5133
ISSN: 2041-6520

Factor impacto JCR: 9.969 (2021)

Categ. JCR: CHEMISTRY, MULTIDISCIPLINARY rank: 25 / 179 = 0.14 (2021) - Q1 - T1

Factor impacto SCIMAGO: 2.878 - Chemistry (miscellaneous) (Q1)

Financiación: info:eu-repo/grantAgreement/ES/DGA/E09-17R-Q-MAD
Financiación: info:eu-repo/grantAgreement/EC/H2020/862893/EU/Molecular spin qudits offering new hope for quantum computing/FATMOLS
Financiación: info:eu-repo/grantAgreement/ES/MCINN/PCI2018-093116
Financiación: info:eu-repo/grantAgreement/ES/MICINN/RTI2018-096075-B-C21
Financiación: info:eu-repo/grantAgreement/EUR/MOLSPIN-COST/CA15128

Tipo y forma: Artículo (Versión definitiva)