Unparalleled selectivity and electronic structure of heterometallic [LnLn'Ln] molecules as 3-qubit quantum gates

Maniaki, D. ; Garay-Ruiz, D. ; Barrios, L. A. ; Martins, D. O. T. A. ; Aguilà, D. ; Tuna, F. ; Reta, D. ; Roubeau, O. ; Bo, C. ; Aromí, G.

Resumen: Heterometallic lanthanide LnLn'] coordination complexes that are accessible thermodynamically are very scarce because the metals of this series have very similar chemical behaviour. Trinuclear systems of this category have not been reported. A coordination chemistry scaffold has been shown to produce molecules of type LnLn'Ln] of high purity, i.e. exhibiting high metal distribution ability, based on their differences in ionic radius. Through a detailed analysis of density functional theory (DFT) based calculations, we discern the energy contributions that lead to the unparalleled chemical selectivity of this molecular system. Some of the previously reported examples are compared here with the newly prepared member of this exotic list, Er2Pr(LA)2(LB)2(py)(H2O)2](NO3) (1) (H2LA and H2LB are two ß-diketone ligands). A magnetic analysis extracted from magnetization and calorimetry determinations identifies the necessary attributes for it to act as an addressable, conditional multiqubit spin-based quantum gate. Complementary ab initio calculations confirm the feasibility of these complexes as composite quantum gates, since they present well-isolated ground states with highly anisotropic and distinct g-tensors. The electronic structure of 1 has also been analyzed by EPR. Pulsed experiments have allowed the establishment of the quantum coherence of the transitions within the relevant spin states, as well as the feasibility of a coherent control of these states via nutation experiments. © 2022 The Royal Society of Chemistry

Idioma: Inglés

DOI: 10.1039/d2sc00436d

Año: 2022

Publicado en: CHEMICAL SCIENCE 13 (2022), 5574 - 5581
ISSN: 2041-6520

Factor impacto JCR: 8.4 (2022)

Categ. JCR: CHEMISTRY, MULTIDISCIPLINARY rank: 32 / 178 = 0.18 (2022) - Q1 - T1

Factor impacto CITESCORE: 15.2 - Chemistry (Q1)

Factor impacto SCIMAGO: 2.762 - Chemistry (miscellaneous) (Q1)

Financiación: info:eu-repo/grantAgreement/ES/AEI/PID2020-118329RB-I00
Financiación: info:eu-repo/grantAgreement/EC/H2020/862893/EU/Molecular spin qudits offering new hope for quantum computing/FATMOLS
Financiación: info:eu-repo/grantAgreement/EUR/QUANTERA/SUMO

Tipo y forma: Artículo (Versión definitiva)