Hu Ziyang, Xu Ziyao, Chen GuanHua
Department of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong, China.
J Chem Phys. 2021 Apr 21;154(15):154703. doi: 10.1063/5.0049176.
Examination of a recent open-system Ehrenfest dynamics simulation suggests that a vibration-mediate resonance may play a pivotal role in the charge transfer across a donor-acceptor interface in an organic solar cell. Based on this, a concise dissipative two-level electronic system coupled to a molecular vibrational mode is proposed and solved quantum mechanically. It is found that the charge transfer is enhanced substantially when the vibrational energy quanta is equal to the electronic energy loss across the interface. This vibration-mediate resonant charge transfer process is ultrafast, occurring within 100 fs, comparable to experimental findings. The open-system Ehrenfest dynamics simulation of the two-level model is carried out, and similar results are obtained, which confirms further that the earlier open-system Ehrenfest dynamics simulation indeed correctly predicted the occurrence of the resonant charge transfer across the donor-acceptor interface.
对最近的一个开放系统埃伦费斯特动力学模拟的研究表明，振动介导的共振可能在有机太阳能电池中供体-受体界面的电荷转移中起关键作用。基于此，提出了一个与分子振动模式耦合的简洁耗散双能级电子系统，并用量子力学方法求解。研究发现，当振动能量量子等于界面上的电子能量损失时，电荷转移会显著增强。这种振动介导的共振电荷转移过程非常快，发生在100飞秒内，与实验结果相当。对双能级模型进行了开放系统埃伦费斯特动力学模拟，得到了类似的结果，这进一步证实了早期的开放系统埃伦费斯特动力学模拟确实正确地预测了供体-受体界面上共振电荷转移的发生。
