Autor segons l'article: Qiu, Jiawei; Abella, Laura; Du, Xiya; Cao, Zhengkai; He, Zhiwen; Meng, Qingyu; Yan, Yingjing; Poblet, Josep M; Sun, Lei; Rodriguez-Fortea, Antonio; Chen, Ning
Departament: Química Física i Inorgànica
Autor/s de la URV: Abella Guzman, Laura / Poblet Rius, Josep Maria / Rodríguez Fortea, Antonio
Paraules clau: Approximation Cluste Complexes Crystallographic evidence Electronic-structure Metallofullerene Mg-mg Pulsed esr Relaxation Stable compound
Resum: Metal-metal bonding is crucial in chemistry for advancing our understanding of the fundamental aspects of chemical bonds. Metal-metal bonds based on alkaline-earth (Ae) elements, especially the heavier Ae elements (Ca, Sr, and Ba), are rarely reported due to their high electropositivity. Herein, we report two heteronuclear di-EMFs CaY@C-s(6)-C-82 and CaY@C-2v(5)-C-80, which contain unprecedented single-electron Ca-Y metal-metal bonds. These compounds were characterized by single-crystal X-ray crystallography, electron paramagnetic resonance (EPR) spectroscopy, and DFT calculations. The crystallographic study of CaY@C-s(6)-C-82 shows that Ca and Y are successfully encapsulated into the carbon cage with a Ca-Y distance of 3.691 & Aring;. The CW-EPR study of both CaY@C-s(6)-C-82 and CaY@C-2v(5)-C-80 exhibits a doublet, suggesting the presence of an unpaired electron located between Ca and Y. The combined experimental and theoretical results confirm the presence of a Ca-Y single-electron metal-metal bond with substantial covalent interaction, attributed to significant overlap between the 4s4p orbitals of Ca and the 5s5p4d orbitals of Y. Furthermore, pulse EPR spectroscopy was used to investigate the quantum coherence of the electron spin within this bond. The unpaired electron, characterized by its s orbital nature, is effectively protected by the carbon cage, resulting in efficient suppression of both spin-lattice relaxation and decoherence. CaY@C-s(6)-C-82 behaves as an electron spin qubit, displaying a maximum decoherence time of 7.74 mu s at 40 K. This study reveals an unprecedented Ae-rare-earth metal-metal bond stabilized by the fullerene cages and elucidates the molecular qubit properties stemming from their unique bonding character, highlighting their potential in quantum information processing applications.
Àrees temàtiques: Astronomia / física Biochemistry Catalysis Chemistry Chemistry (all) Chemistry (miscellaneous) Chemistry, multidisciplinary Ciência de alimentos Ciências agrárias i Ciências biológicas i Ciências biológicas ii Colloid and surface chemistry Engenharias ii Engenharias iii Engenharias iv Farmacia General chemistry Interdisciplinar Materiais Química
Accès a la llicència d'ús: https://creativecommons.org/licenses/by/3.0/es/
Adreça de correu electrònic de l'autor: antonio.rodriguezf@urv.cat josepmaria.poblet@urv.cat
Identificador de l'autor: 0000-0001-5884-5629 0000-0002-4533-0623
Data d'alta del registre: 2024-10-12
Versió de l'article dipositat: info:eu-repo/semantics/publishedVersion
Referència a l'article segons font original: Journal Of The American Chemical Society. 146 (35): 24310-24319
Referència de l'ítem segons les normes APA: Qiu, Jiawei; Abella, Laura; Du, Xiya; Cao, Zhengkai; He, Zhiwen; Meng, Qingyu; Yan, Yingjing; Poblet, Josep M; Sun, Lei; Rodriguez-Fortea, Antonio; Ch (2024). CaY@C2n : Exploring Molecular Qubits with Ca-Y Metal-Metal Bonds. Journal Of The American Chemical Society, 146(35), 24310-24319. DOI: 10.1021/jacs.4c04720
URL Document de llicència: https://repositori.urv.cat/ca/proteccio-de-dades/
Entitat: Universitat Rovira i Virgili
Any de publicació de la revista: 2024
Tipus de publicació: Journal Publications
Repositori URV