内分子单片裂变中的刺激相关性
Samuel N Sanders1, Elango Kumarasamy1, Andrew B Pun1
1Department of Chemistry, Columbia University , New York, New York 10027, United States.
Journal of the American Chemical Society
|May 17, 2016
概括
我们合成了不对称的五四二聚体, 桥梁长度会影响激子局部化和iSF速率,从而提供三重组对动态的洞察力.
科学领域:
- 有机光化学
- 材料科学
- 激发动力学
背景情况:
- 内分子单片裂变 (iSF) 是提高太阳能电池效率的关键过程.
- 了解激子动态和相关性是优化iSF的关键.
研究的目的:
- 合成和表征具有可变联接桥长度的不对称五烯-四烯异构体.
- 在iSF过程中调查激子和三重组对的空间动态.
- 阐明激子相关性和桥梁长度在iSF效率和三重组合中的作用.
主要方法:
- 不对称的五烯-四烯异构体的合成,具有不同的结合桥梁长度.
- 用光谱分析来确定单元和三元的能量.
- 时间解析的光物理测量以研究激子动力学和重组动力学.
- 支持实验观察的理论计算.
主要成果:
- 在合成的异构体中观察到快速有效的iSF.
- 与对称二次体相比,增加的桥梁长度导致单点局部化和较慢的iSF速率.
- 不等价的三重重组合动力学得到解决,主要是通过协同过程衰减.
- 鉴定和分离了包括相关和非相关的三胞胎在内的过渡物种.
- 尽管有局部的三胞胎,但三胞胎对的重组速度很快.
结论:
- 不对称的异构体提供了一个可调的平台来研究iSF机制.
- 桥梁的长度极大地影响了激素的移位,iSF的效率和三重体的形成.
- 这些系统可以隔离和研究对iSF至关重要的过渡物种,有助于设计先进的光物理材料.
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