基于Ru (II) 和Os (II) 聚烯基复合物的高效光采集天线聚合物中的超快兴奋状态能量迁移动态
C N Fleming1, K A Maxwell, J M DeSimone
1Department of Chemistry, Venable and Kenan Laboratories, The University of North Carolina at Chapel Hill, 27599-3290, USA.
Journal of the American Chemical Society
|October 18, 2001
概括
研究了聚合物骨干上和聚烯基复合物的能量迁移. 该过程由光刺激启动,将能量转移到奥斯陷,其动力学揭示了复杂的动力学和高效的远程传输.
科学领域:
- 协调化学 协调化学
- 聚合物科学 聚合物科学
- 光物理学的光学物理学
背景情况:
- (II) 和 (II) 聚烯基复合物是光物理研究中的关键组成部分.
- 聚合物支系统为能量转移研究提供受控架构.
- 了解激发状态动态对于开发光采集材料至关重要.
研究的目的:
- 在聚合物骨干上研究Ru (II) 和Os (II) 聚烯基复合物的兴奋状态能量迁移动态.
- 阐明能量转移的机制,包括直接转移和跳跃.
- 为了将聚合物结构与能量迁移效率相关联.
主要方法:
- 时间分辨率发光光谱学监测Os (II) 发射在780nm.
- 的光激发 (II) 金属到合金电荷转移 (MLCT) 过渡.
- 蒙特卡洛模拟用于模拟聚合物结构和能量转移动态.
主要成果:
- 能量迁移通过直接转移到Os (II) 陷或通过在Ru (II) 站点之间跳跃而发生.
- 复杂的动力学,通过两个指数的和,表示距离和时间尺度的分布.
- 蒙特卡洛模拟表明,Ru>Os的能量传输时间为~400 ps,Ru>Ru的跳跃时间为1-4 ns.
结论:
- 聚合物系统从Ru (II) 到Os (II) 陷中表现出高效的能量迁移.
- 观察到的动态受到捐赠者-接受者距离和传输时间尺度的影响.
- 该系统的效率表明有可能扩展到更长的聚合物尺寸.
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