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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Interligand Electron Transfer Dynamics in [Os(bpy)_3]~(2+): Exploring the Excited State Potential Surfaces with Femtosecond Spectroscopy
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Interligand Electron Transfer Dynamics in [Os(bpy)_3]~(2+): Exploring the Excited State Potential Surfaces with Femtosecond Spectroscopy

机译：[Os（bpy）_3]〜（2+）中的配体电子转移动力学：用飞秒光谱探索激发态势面

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摘要

Femtosecond transient absorption studies of [Os(bpy)_3]~(2+) have been performed to gain new insights into the excited-state dynamics. Experiments were performed for a series of excitation wavelengths throughout both the singlet and triplet metal-to-ligand charge transfer (MLCT) bands. The dynamics are probed via the π-π~* transition on the bpy~- anion at 370 nm. Time scales for interligand electron transfer (ILET) and vibrational cooling are extracted from the amplitude and anisotropy of the excited state absorptions. The ILET rate has been measured as a function of temperature and, from these data, estimates for the electron transfer activation energy and ligand-ligand coupling are made. Our data also provide insight into the vibrational cooling dynamics within these large complexes, suggesting that vibrational cooling occurs only when exciting into the singlet MLCT state, after intersystem crossing. It appears that photoexcitation within the triplet MLCT absorption produces molecules that are vibrationally cold, even for excitation at the blue edge of the absorption band.
机译：飞秒[Os（bpy）_3]〜（2+）的瞬态吸收研究已经获得，从而对激发态动力学有了新的认识。对整个单重态和三重态金属到配体电荷转移（MLCT）波段的一系列激发波长进行了实验。通过在370 nm处bpy〜-阴离子上的π-π〜*跃迁探测动力学。从激发态吸收的幅度和各向异性中提取了配体电子转移（ILET）和振动冷却的时间标度。根据温度测量了ILET速率，并根据这些数据估算了电子转移活化能和配体-配体偶联。我们的数据还提供了对这些大型复合体内的振动冷却动力学的洞察力，表明振动冷却仅在系统间交叉之后仅当激发到单重MLCT状态时才会发生。似乎三重态MLCT吸收内的光激发产生的分子即使在吸收带的蓝色边缘被激发，也会产生振动冷态。

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