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首页> 外文期刊>Chemistry: A European journal >The Multichromophore Approach:Prolonged Room-Temperature Luminescence Lifetimes in Ru~(II) Complexes Based on Tridentate Polypyridine Ligands
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The Multichromophore Approach:Prolonged Room-Temperature Luminescence Lifetimes in Ru~(II) Complexes Based on Tridentate Polypyridine Ligands

机译：多发色团方法：基于三齿多吡啶配体的Ru〜（II）配合物延长了室温发光寿命

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A new family of rutheni-um(II) complexes with multichromo-phoric properties was prepared based on a "chemistry-on-the-complex" synthetic approach.The new compounds are based on tridentate chelating sites (tpy-type ligands,tpy=2,2':6',2"-terpyr-idine) and most of them carry appended anthryl chromophores.Complexes 2 a and 2 b were synthesized through the Pd-catalyzed Suzuki coupling reaction between 9-anthrylboronic acid and the chloro ligands on the presursor species 1a and 1b,respectively.The mono-coupling product 2 c was also synthesized as the starting complex for a di-metallic complex under optimized Suzuki coupling conditions.The palla-dium(0)-catalyzed homocoupling reaction on complexes 1a and 2c led to di-metallic Ru~(II) species 2d and 2e,respectively.The solid structures of complexes 2 a and 2 b were characterized by X-ray diffraction.The absorption spectra,redox behavior,luminescence properties (both at room temperature and at 77 K),and transient absorption spectra and decays of 2a-e were investigated.The absorption spectra of all new species are dominated by ligand-centered (LC) bands in the UV region and metal-to-ligand charge-transfer (MLCT) bands in the visible region.The new compounds undergo reversible metal-centered oxidation processes and several ligand-centered reduction processes,which have been assigned to specific sites.The complexes exhibit luminescence both at room temperature in fluid solution and at 77 K in rigid matrices;the emission was attributed to ~3MLCT states at room temperature and to the lowest-lying anthracene triplet (~3An) at low temperature,except for 2 c,which does not contain any anthryl chromophore and whose low temperature emission is also of MLCT origin.The luminescence lifetimes of complexes 2a-d showed that multi-chromophoric behavior occurs in these species,allowing the luminescence lifetime of the Ru~(II)-based chromophores to be prolonged to the microsecond timescale,with the anthryl groups behaving as energy-storage elements for the repopulation of the ~3MLCT state.Nanosecond transient-absorption spec-troscopy confirmed the equilibration process between the triplet MLCT and An levels at room temperature.Ther-modynamic and kinetic factors governing the equilibration time and the lifetime of the equilibrated excited state are discussed.
机译：基于“复杂化学”合成方法，制备了具有多色性的钌-钌（II）配合物新家族。新化合物基于三齿螯合位点（tpy型配体，tpy = 2,2'：6'，2“-叔吡啶），大部分带有附加的蒽发色团。络合物2a和2b是通过Pd催化9-蒽硼酸与氯代配体上的Suzuki偶联反应合成的。在优化的Suzuki偶联条件下，还合成了单偶联产物2c作为双金属络合物的起始络合物。钯（0）催化了络合物1a和1b上的均偶联反应。 2c分别导致了双金属Ru〜（II）物种2d和2e。配合物2a和2b的固体结构通过X射线衍射表征。吸收光谱，氧化还原行为，发光性质（均在室温下）并且在77 K时），以及瞬态吸收光谱和衰减研究了2a-e中所有化合物的吸收光谱，其中紫外区的配体中心（LC）带和可见区的金属-配体电荷转移（MLCT）带占主导地位。可逆金属中心的氧化过程和几个配体中心的还原过程已被分配到特定的位置。配合物在室温下在流体溶液中和在77 K在刚性基质中均表现出发光;该发光归因于〜3MLCT状态室温和最低温度下的蒽三联体（〜3An）处于低温状态（2 c除外），其中不包含任何蒽基发色团并且其低温发射也是MLCT起源的。复合物2a-d的发光寿命这些物种中发生多发色行为，从而使基于Ru〜（II）的发色团的发光寿命延长至微秒级，并且蒽基表现为能量存储纳秒瞬态吸收光谱法证实了三重态MLCT和An水平在室温下的平衡过程。控制平衡时间和平衡激发态寿命的热力学和动力学因素讨论。

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