在同位素N-无效二胺二元体中的桥式电荷分离
Yuanyuan Guo1, Zetong Ma1, Xinmiao Niu1
1University of Chinese Academy of Sciences , Beijing 100049 , China.
Journal of the American Chemical Society
|July 24, 2019
概括
分子系统中的电荷分离受电子合和溶剂极性影响. 在元替代桥梁中的破坏性干扰显著减缓了电荷分离,影响了分子电子和光合作用研究.
科学领域:
- 摄影化学
- 分子电子
- 超分子化学
背景情况:
- 电荷分离对于分子电子和光合作用等自然过程至关重要.
- 捐赠者-桥梁-接受者分子促进CS,电子合和溶剂效应是关键决定因素.
- 了解具有相同染色体的系统中的CS动态是基本的.
研究的目的:
- 研究结合桥结构对电荷分离动态的影响.
- 在不同溶剂中比较同位素N-取消的二烯二胺 (BDNP) 的电荷分离率.
- 阐明溶剂效应和电子合在电荷分离中的作用.
主要方法:
- 使用femtosecond暂时吸收光谱 (fs-TA) 来研究电荷分离动态.
- 对具有不同桥梁结构的异构BDNP二元体进行比较研究.
- 使用量子化学计算分析溶剂效应和电子合.
主要成果:
- 在弱极性溶剂中,电荷分离是不利的,但在极性溶剂中观察到,电荷分离率随着极性的增加而增加.
- 甲基替代BDNP的电荷分离速率比其同位素缓慢一个数量级.
- 转基因替代BDNP中较慢的CS归因于通过桥梁的破坏性波函数干扰.
结论:
- 结合式桥梁结构决定了电荷分离的效率.
- 溶剂极性显著调节电荷分离速度和可行性.
- 在元替代桥梁中的破坏性干扰对有效的电荷分离构成重大障碍.
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