论文标题
光异构化耦合电子传输
Photoisomerization-coupled electron transfer
论文作者
论文摘要
光致变色分子结构构成了一个独特的平台，用于构建分子开关，传感器和内存设备。他们最有前途的应用之一是可轻开关电子受体或供体单位。在这里，我们研究了我们假设在这样的系统中可能发生的先前未开发的过程：由捐赠者或受体部分的同时光异构化触发的超快电子转移。我们为这种现象提出了一个理论模型，并借助DFT计算，将其应用于二氢吡喃型光致变色分子供体的情况。通过考虑波袋动力学和光异构化产量，我们表明涉及的两个过程，电子传递和光异构化是不可分割的，需要以统一的方式进行处理。我们通过讨论如何通过实验控制光异构化耦合电子传输的效率。
Photochromic molecular structures constitute a unique platform for constructing molecular switches, sensors and memory devices. One of their most promising applications is as light-switchable electron acceptor or donor units. Here, we investigate a previously unexplored process that we postulate may occur in such systems: an ultrafast electron transfer triggered by a simultaneous photoisomerization of the donor or the acceptor moiety. We propose a theoretical model for this phenomenon and, with the aid of DFT calculations, apply it to the case of a dihydropyrene-type photochromic molecular donor. By considering the wavepacket dynamics and the photoisomerization yield, we show that the two processes involved, electron transfer and photoisomerization, are in general inseparable and need to be treated in a unified manner. We finish by discussing how the efficiency of photoisomerization-coupled electron transfer can be controlled experimentally.
