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首页> 外文期刊>Chemistry: A European journal >Redox-Responsive Molecular Switches Based on Azoterpyridine-Bridged Ru/Os Complexes
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Redox-Responsive Molecular Switches Based on Azoterpyridine-Bridged Ru/Os Complexes

机译：基于偶氮吡啶桥Ru / Os配合物的氧化还原响应分子开关。

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摘要

Three new terpyridine-based dinuclear complexes, [(tpy)Ru(azotpy)Ru(tpy)]~(4+) (tpy = 2,2':6',2''-terpyridine, azotpy = bix[2,6-bis(2-pyridyl)-4-pyridyl]diazene), [(tpy)Os(azotpy)Os(tpy)]]~(4+), and [(tpy)Ru(azotpy)Os(tpy)]~(4+) were prepared and their electrochemical and photophysical properties investigated. The bridging ligand, azotpy, in these complexes is reduced at less negative potentials than the unsubstituted tpy ligand. These complexes exhibit absorption bands due to the metal-to-ligand charge-transfer transitions both to the unsubstituted tpy ligand and the bridging azotpy ligand, the latter absorption being observed at the lower energy side of the former. These observations are consistent with the lower lying #pi# level of the azotpy ligand than that of the tpy ligand. These complexes are nonlumi-nescent, since the excited electron is trapped in this lower lying #pi# level of the azotpy ligand in the excited state. Reduction of this bridging ligand by constant potential electrolysis renders the shape of absorption spectra for these complexes nearly identical to those of the parent complexes, [M(tpy)_2]~(2+) (M = Ru, Os). In this reduced state, the homodinuclear Os complex becomes luminescent at room temperature, whereas the homodinuclear Ru complex becomes luminescent at 77 K, thus establishing their photoswitching behavior. The reduced heterodinuclear complex exhibits luminescence from the Os center, which is sensitized by the Ru center in the same molecule as evidenced by the excitations spectra. Thus, the intramolecular energy transfer can be switched on and off by the redox reaction of the bridging component.
机译：三种新的基于吡啶的双核配合物[[tpy）Ru（azotpy）Ru（tpy）]〜（4+）（tpy = 2,2'：6'，2''-叔吡啶，azotpy = bix [2,6 -双（2-吡啶基）-4-吡啶基]二氮烯），[（tpy）Os（偶氮）Os（tpy）]]〜（4+）和[（tpy）Ru（azotpy）Os（tpy）]〜制备了（4+），并研究了它们的电化学和光物理性质。与未取代的tpy配体相比，这些络合物中的桥联配体azotpy负电势降低。由于金属到配体的电荷转移跃迁到未取代的tpy配体和桥接偶氮配体上，这些配合物表现出吸收带，在前者的较低能量侧观察到后者的吸收。这些观察结果与偶氮配体比tpy配体的更低的＃pi＃水平相符。这些络合物是非发光的，因为被激发的电子在被激发态被俘获在偶氮配体的该较低的＃pi＃能级中。通过恒电位电解还原该桥联配体使得这些络合物的吸收光谱形状几乎与母体络合物[M（tpy）_2]〜（2+）（M = Ru，Os）相同。在这种还原状态下，同核Os络合物在室温下发光，而同核Ru络合物在77 K下发光，从而建立了它们的光开关行为。还原的异双核复合物表现出从Os中心发光，该发光由同一分子中的Ru中心敏化，如激发光谱所示。因此，分子内能量传递可以通过桥连组分的氧化还原反应来开启和关闭。

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