量子一致性提高了两个等价电子接收器的电子传输速率
Brian T Phelan1, Jinyuan Zhang1, Guan-Jhih Huang1
1Department of Chemistry and Institute for Sustainability and Energy at Northwestern , Northwestern University , Evanston , Illinois 60208-3113 , United States.
Journal of the American Chemical Society
|July 16, 2019
概括
当一个捐赠者与多个受体相互作用时,量子连贯性显著提高了电子转移 (ET) 速率. 这项研究表明,对两个基受体的ET比对一个更快,特别是在低温下.
科学领域:
- 摄影化学
- 量子动力学
- 分子相互作用
背景情况:
- 电子转移 (ET) 是化学和生物过程的基础.
- 量子连贯性可以影响ET速率,特别是在多个接受器的系统中.
- 捐赠者-接受者 (D-A) 化合物为研究这些现象提供了一个平台.
研究的目的:
- 研究量子连贯性对光驱电子转移速率的影响.
- 在捐赠者-接受者系统中比较一个与两个接受者的ET率.
- 阐明温度在这些系统中的ET动态上的作用.
主要方法:
- 提供者-接受者化合物的合成,将恩素 (An) 提供者与1,4-基 (BQ) 接受者连接起来.
- 超快速光谱技术用于测量亚皮秒电子传输速率.
- 可变温度研究 (室内和冷) 探测温度依赖的效应.
主要成果:
- 在室温下,从 antracen 转移到两种诺基的电子速度大约是诺基的2.4倍.
- 在冷温度下,两个基的ET速率大约是基的5倍.
- 在低温下观察到速度增强的2倍.
结论:
- 量子连贯性在增强多受体系统中的电子传输速率方面起着至关重要的作用.
- 观察到的速率提升归因于从单位ET过渡到涉及叠加状态的连贯ET.
- 在低温下相关的系统浴波动进一步提高了ET效率.
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