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Charge Transfer Dynamics at Dye-Sensitized ZnO and TiO2 Interfaces Studied by Ultrafast XUV Photoelectron Spectroscopy

机译:超快XUV光电子能谱研究染料敏化ZnO和TiO2界面上的电荷转移动力学

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摘要

Interfacial charge transfer from photoexcited ruthenium-based N3 dye molecules into ZnO thin films received controversial interpretations. To identify the physical origin for the delayed electron transfer in ZnO compared to TiO2, we probe directly the electronic structure at both dye-semiconductor interfaces by applying ultrafast XUV photoemission spectroscopy. In the range of pump-probe time delays between 0.5 to 1.0 ps, the transient signal of the intermediate states was compared, revealing a distinct difference in their electron binding energies of 0.4 eV. This finding strongly indicates the nature of the charge injection at the ZnO interface associated with the formation of an interfacial electron-cation complex. It further highlights that the energetic alignment between the dye donor and semiconductor acceptor states appears to be of minor importance for the injection kinetics and that the injection efficiency is dominated by the electronic coupling.
机译:从光激发的钌基N3染料分子到ZnO薄膜的界面电荷转移受到了有争议的解释。为了确定与TiO2相比ZnO中延迟电子转移的物理起源,我们通过应用超快XUV光发射光谱法直接探测了两个染料-半导体界面的电子结构。在泵浦探针时间延迟范围为0.5至1.0µps之间,对中间态的瞬态信号进行了比较,发现它们的电子结合能明显不同,为0.4µeV。这一发现有力地表明了在ZnO界面上电荷注入的性质,与界面电子阳离子络合物的形成有关。它进一步突出显示,染料供体和半导体受体状态之间的能量对准对于注入动力学似乎不太重要,并且注入效率由电子耦合决定。

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