Applied Magnetic Resonance ( IF 1.1 ) Pub Date : 2021-08-17 , DOI: 10.1007/s00723-021-01402-6 Yuheng Huang 1 , Matthew D. Krzyaniak 1 , Ryan M. Young 1 , Michael R. Wasielewski 1
The mechanism of spin polarization transfer from a photogenerated spin-correlated radical pair to a stable radical was studied in a covalent donor-chromophore-acceptor-stable radical (D-C-A-R•) system, where the donor (D) is 4-methoxyaniline (MeOAn), the chromophore (C) is 4-(N-piperidinyl)-naphthalene-1,8-dicarboximide (ANI), the acceptor (A) is naphthalene-1,8:4,5-bis(dicarboximide) (NDI) and the stable radical (R•) is (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO). Experiments probed the effect of the spin–spin exchange interaction between D•+ and A•− as well as the charge recombination dynamics of D•+-C-A•− on spin polarization transfer from the D•+-C-A•− SCRP to R• as a function of the dielectric environment in glassy media at cryogenic temperatures. The results show that spin polarization on R• is generated by asymmetry in the charge recombination pathways rather than variations in the spin–spin exchange interaction between D•+ and A•−. These results inform design criteria for using an SCRP to spin polarize a third spin for potential applications in quantum information science.
中文翻译:
共价供体-受体-自由基体系中电子自旋极化转移的机理研究
在共价供体-发色团-受体-稳定自由基(DCAR •)系统中研究了从光生自旋相关自由基对到稳定自由基的自旋极化转移机制,其中供体(D)是4-甲氧基苯胺(MeOAn) ,发色团 (C) 是 4-( N-哌啶基)-萘-1,8-二甲酰亚胺 (ANI),受体 (A) 是萘-1,8:4,5-双 (二甲酰亚胺) (NDI) 和稳定的基团 (R • ) 是 (2,2,6,6-四甲基哌啶-1-基)氧基 (TEMPO)。实验探讨了 D •+和 A •-之间的自旋-自旋交换相互作用以及 D •+ -CA •-的电荷复合动力学对 D • 的自旋极化转移的影响•+ -CA • - SCRP至R •如在低温下在玻璃媒体的介电环境的函数。结果表明,R •上的自旋极化是由电荷复合途径的不对称性产生的,而不是由 D •+和 A •-之间的自旋-自旋交换相互作用的变化产生的。这些结果为使用 SCRP 自旋极化第三自旋的设计标准提供了信息,以用于量子信息科学的潜在应用。