Pan Duohai, Hu Dehong, Lu H Peter
Pacific Northwest National Laboratory, Fundamental Science Division, Richland, Washington 99352, USA.
J Phys Chem B. 2005 Sep 1;109(34):16390-5. doi: 10.1021/jp058043v.
An atomic force microscopy (AFM) and confocal Raman microscopy study of the interfacial electron transfer of a dye-sensitization system, i.e., alizarin adsorbed upon TiO(2) nanoparticles, has revealed the distribution of the mode-specific vibrational reorganization energies encompassing different local sites ( approximately 250-nm spatial resolution). Our experimental results suggest inhomogeneous vibrational reorganization energy barriers and different Franck-Condon coupling factors of the interfacial electron transfer. The total vibrational reorganization energy was inhomogeneous from site to site; specifically, mode-specific analyses indicated that energy distributions were inhomogeneous for bridging normal modes and less inhomogeneous or homogeneous for nonbridging normal modes, especially for modes far away from the alizarin-TiO(2) coupling hydroxyl modes. The results demonstrate a significant step forward in characterizing site-specific inhomogeneous interfacial charge-transfer dynamics.
一项关于染料敏化体系（即茜素吸附在二氧化钛纳米颗粒上）界面电子转移的原子力显微镜（AFM）和共聚焦拉曼显微镜研究，揭示了包含不同局部位点的模式特异性振动重组能的分布（空间分辨率约为250纳米）。我们的实验结果表明，界面电子转移存在不均匀的振动重组能垒和不同的弗兰克 - 康登耦合因子。总的振动重组能在不同位点之间是不均匀的；具体而言，模式特异性分析表明，桥连正常模式的能量分布不均匀，而非桥连正常模式的能量分布不均匀性较小或呈均匀分布，特别是对于远离茜素 - 二氧化钛耦合羟基模式的模式。这些结果表明在表征位点特异性非均匀界面电荷转移动力学方面向前迈出了重要一步。
