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Structural factors controlling the spin-spin exchange coupling: EPR spectroscopic studies of highly asymmetric trityl-nitroxide biradicals

机译:控制自旋-自旋交换耦合的结构因素:高不对称三苯甲基-硝基氧双自由基的EPR光谱研究

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摘要

Highly asymmetric exchange-coupled biradicals, like the trityl-nitroxides (TN), possess particular magnetic properties opening new possibilities for their application in biophysical, physicochemical and biological studies. In the present work, we investigated the effect of the linker length on the spin-spin coupling interaction in TN biradicals using the newly synthesized biradicals CT02-GT, CT02-AT, CT02-VT and CT02-PPT as well as the previously reported biradicals TNN14 and TN1. Results show that the magnitude of the spin-spin interaction (J) can be easily tuned from ~ 4 G (conformer 1 in CT02-PPT) to over 1200 G (in TNN14) using various linkers separating the two radical moieties and with varying temperature. Computer simulation of EPR spectra was carried out to directly estimate J values of the TN biradicals. In addition to the spin-spin coupling interaction of TN biradicals, their g, hyperfine splitting and zero-field splitting interactions were explored at low temperature (220 K). Our present study clearly shows that the spin-spin interaction variation as a function of linker distance and temperature provides an effective strategy to develop new TN biradicals which can find wide applications in relevant fields.
机译:高度不对称的交换耦合双自由基,如三苯甲基-氮杂化物(TN),具有特殊的磁性,为它们在生物物理,物理化学和生物学研究中的应用开辟了新的可能性。在当前的工作中,我们使用新合成的双自由基CT02-GT,CT02-AT,CT02-VT和CT02-PPT以及先前报道的双自由基,研究了接头长度对TN双自由基中自旋-自旋偶联相互作用的影响TNN14和TN1。结果表明,使用分离两个自由基部分和不同温度的各种连接子,可以轻松地将自旋-自旋相互作用(J)的大小从〜4 G(CT02-PPT中的异构体1)调节至超过1200 G(TNN14中) 。进行EPR谱的计算机模拟以直接估计TN双基的J值。除了TN双自由基的自旋-自旋偶联相互作用外,还在低温(220 K)下研究了它们的g,超精细分裂和零场分裂相互作用。我们目前的研究清楚地表明,自旋-自旋相互作用的变化是连接子距离和温度的函数,为开发新的TN双自由基提供了有效的策略,该双自由基在相关领域具有广泛的应用。

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