Ranieri Davide, Santanni Fabio, Privitera Alberto, Albino Andrea, Salvadori Enrico, Chiesa Mario, Totti Federico, Sorace Lorenzo, Sessoli Roberta
Department of Chemistry "Ugo Schiff" & INSTM RU, University of Florence Via della Lastruccia 3 50019 Sesto Fiorentino Italy
Department of Chemistry, NIS, University of Turin Via P. Giuria 7 I10125 Torino Italy.
Chem Sci. 2022 Nov 14;14(1):61-69. doi: 10.1039/d2sc04969d. eCollection 2022 Dec 21.
We report here the synthesis of a new - (-) singly linked vanadyl-porphyrin dimer that crystallizes in two different pseudo-polymorphs. The single crystal continuous-wave electron paramagnetic resonance investigation evidences a small but crucial isotropic exchange interaction, , between the two tilted, and thus distinguishable, spin centers of the order of 10 cm. The experimental and DFT studies evidence a correlation between values and porphyrin plane tilting angle and distortion. Pulsed EPR analysis shows that the two vanadyl dimers maintain the coherence time of the monomer. With the obtained spin Hamiltonian parameters, we identify suitable transitions that could be used as computational basis states. Our results, coupled with the evaporability of porphyrin systems, establish this class of dimers as extremely promising for quantum information processing applications.
我们在此报告一种新型的 - (-) 单链钒氧基 - 卟啉二聚体的合成,该二聚体以两种不同的假多晶型形式结晶。单晶连续波电子顺磁共振研究表明,在两个倾斜且因此可区分的自旋中心之间存在一个小但关键的各向同性交换相互作用,其大小约为10 cm。实验和密度泛函理论研究表明 值与卟啉平面倾斜角和畸变之间存在相关性。脉冲电子顺磁共振分析表明,两个钒氧基二聚体保持了单体的相干时间。利用获得的自旋哈密顿参数,我们确定了可作为计算基态的合适跃迁。我们的结果,再加上卟啉系统的可蒸发性,使得这类二聚体在量子信息处理应用方面极具前景。