Vibrational coherence in ultrafast electron transfer reaction observed by broadband transient absorption spectroscopy
Vibrational coherence in ultrafast electron transfer reaction observed by broadband transient absorption spectroscopy
复制标题
宽带瞬态吸收光谱观察超快电子转移反应中的振动相干性
DOI：
10.1051/epjconf/201920509028
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发表时间：
2019
影响因子：
--
通讯作者：
Miyasaka Hiroshi
中科院分区：
文献类型：
--
作者：
Yoneda Yusuke;Kudisch Bryan;Rafiq Shahnawaz;Maiuri Margherita;Scholes Gregory;Miyasaka Hiroshi
光诱导电子转移（ET）是光能转换系统中最重要的过程之一。马库斯理论是凝聚相 ET 反应最著名的框架之一。在这一理论中，周围媒体的重组被视为主要的反应坐标。然而，超出 Marcus 框架的超快 ET 已在各种系统中被报道。为了阐明分子振动在超快 ET 中的作用，我们通过宽带瞬态吸收光谱研究了并四苯染料和苯胺衍生物之间的 ET 动力学。在时域中观察到频率为300-1600 cm-1的并四苯染料的相干波包运动。 310 cm-1 模式的振动相干性随着电子转移速率的增加而降低，表明这种振动与电子转移反应耦合。
Photoinduced electron transfer (ET) is one of the most important processes in light energy conversion systems. Marcus theory is one of the most famous frameworks on ET reaction in condensed phase. In this theory, reorganization of surrounding media is regarded as a main reaction coordinate. However, ultrafast ET beyond Marcus’ framework has been reported in various systems. To elucidate the role of molecular vibration in ultrafast ET, we have investigated the ET dynamics between a naphthacene dye and aniline derivatives by means of broadband transient absorption spectroscopy. Coherent wavepacket motions of naphthacene dye with frequencies of 300-1600 cm-1were observed in time domain. The vibrational coherence of 310 cm-1mode was reduced with increasing electron transfer rate, suggesting this vibration is coupled to electron transfer reaction.