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首页> 外文期刊>Chemistry: A European journal >The Effect of Heavy Atoms on Photoinduced Electron Injection fromNonthermalized and Thermalized Donor States of MII–Polypyridyl ACHTUNGTRENUNG(M=Ru/Os) Complexes to Nanoparticulate TiO2 Surfaces: An Ultrafast Time-Resolved Absorption Study
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The Effect of Heavy Atoms on Photoinduced Electron Injection fromNonthermalized and Thermalized Donor States of MII–Polypyridyl ACHTUNGTRENUNG(M=Ru/Os) Complexes to Nanoparticulate TiO2 Surfaces: An Ultrafast Time-Resolved Absorption Study

机译：重原子对MII-聚吡啶基ACHTUNGTRENUNG（M = Ru / Os）配合物对纳米TiO2表面的非热供体态和热供体态光注入电子的影响：超快时间分辨吸收研究

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We have synthesized ruthenium(II)– and osmium(II)–polypyridylcomplexes ([MACHTUNGTRENUNG(bpy)2L]2+, in which M=OsII or RuII, bpy=2,2’-bipyridyl,and L=4-(2,2’-bipyridinyl-4-yl)benzene-1,2-diol) and studied the interfacialelectron-transfer process on a TiO2nanoparticle surface using femtosecond transient-absorption spectroscopy.Ruthenium(II)- and osmium(II)-based dyes have a similar molecular structure; nevertheless, we have observed quite different interfacial electrontransfer dynamics (both forward and backward). In the case of the RuII/TiO2 system, single-exponential electron injection takes place from photoexcited nonthermalized metal-to-ligand charge transfer (MLCT) states. However, in the case of the OsII/TiO2 system, electron injection takes place biexponentially from both nonthermalized and thermalized MLCT states (mainly 3MLCT states). Larger spin–orbit coupling for the heavier transition-metal osmium, relative to that of ruthenium, accounts for the more efficient population of the 3MLCT states in the OsIIbased dye during the electron-injection process that yields biexponential dynamics. Our results tend to suggest that appropriately designed OsII–polypyridyl dye can be a better sensitizer molecule relative to its RuII analogue not only due to much broader absorption in the visible region of the solaremission spectrum, but also on account of slower charge recombination.
机译：我们合成了钌（II）和–（II）聚吡啶基配合物（[MACHTUNGTRENUNG（bpy）2L] 2+，其中M = OsII或RuII，bpy = 2,2'-联吡啶，L = 4-（2 ，2'-联吡啶基-4-基）苯-1,2-二醇），并使用飞秒瞬态吸收光谱法研究了TiO2纳米颗粒表面的界面电子转移过程。钌（II）和（II）染料具有相似的分子结构;然而，我们已经观察到截然不同的界面电子转移动力学（向前和向后）。在RuII / TiO2系统的情况下，单指数电子注入是从光激发的非热金属到配体的电荷转移（MLCT）状态发生的。但是，在OsII / TiO2系统的情况下，电子注入是从非热化和热化MLCT状态（主要是3MLCT状态）双指数发生的。相对于钌而言，较大的过渡金属spin的自旋轨道耦合较大，这说明在电子注入过程中，OsII基染料中3MLCT状态的填充更为有效，从而产生了双指数动力学。我们的结果倾向于表明，相对于其RuII类似物，适当设计的OsII-聚吡啶基染料可能是更好的敏化剂分子，这不仅是由于在日光发射光谱的可见光区域吸收范围更广，而且还因为电荷重组较慢。

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