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超快速的电荷转移动力学在一个滑叠的捐助者-接受者-接受者系统

Chenjian Lin¹, James P O'Connor¹, Brian T Phelan¹

¹Department of Chemistry and Paula M. Trienens Institute for Sustainability and Energy, Northwestern University, Evanston, Illinois 60208-3113, United States.

The journal of physical chemistry. A

|December 28, 2023

概括

分子系统中的激发性合会影响电荷转移动态. 在烯-捐赠-二胺-接受器 (Per-PDI) 系统中,合减缓了电子传输,并防止了破坏对称性的电荷分离 (SB-CS).

科学领域:

摄影化学的使用.
分子光物理学的分子光物理.
电荷转移动力学电荷转移动力学

背景情况:

由于刺激性合,分子聚合物表现出改变的电荷转移动态.
刺激性合可以启用新的光物理路径,如对称性破坏电荷分离 (SB-CS).

研究的目的:

调查激发性合对电荷转移动态在共价的捐赠者-受体-受体系统 (Per-PDI) 的影响.
将Per-PDI的 femtosecond短暂吸收数据与相关系统 (Per-PDI和PDI二极管) 进行比较,以了解刺激效应.

主要方法:

选择性光激发皮利伦胺胺 (PDI) 染色体.
五秒秒短暂吸收光谱学.
对具有不同供体-接受体配置的分子系统进行比较分析.

主要成果:

电子从乙烯供体 (Per) 转移到PDI二元体的低激电位比单个PDI受体系统更慢.
PDI之间的激发性合电子稳定了系统,减少了电荷分离的驱动力.
在Per-PDI中,Per和PDI之间强大的π-π相互作用打破了PDI二元体的电子对称性,导致Per氧化而不是SB-CS.

结论:

分子系统中的电子合必须仔细平衡,以促进所需的光物理路径,如SB-CS.
设计SB-CS系统需要优化捐赠者,接受者及其激发性相互作用之间的相互作用.

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