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混合量子-经典方法在复杂分子体系动力学过程的模拟方面有重要应用.我们采用Ehrenfest方法、surfacehopping方法和混合量子经典Liouville方程计算了在非绝热极限下的电荷转移速率.然后将这三种方法应用于有机半导体材料电荷转移速率的计算.研究结果发现,Ehrenfest方法和surface hopping方法可能严重偏离正确的结果.偏离的原因是这两种方法没有正确处理相干项的运动,而且这种偏离在涉及到高频模式时显得更加严重.
The mixed quantum-classical method has important applications in the simulation of kinetic processes of complex molecular systems.We calculated the charge transfer rate at the non-adiabatic limit using the Ehrenfest method, the surfacehopping method and the mixed quantum classical Liouville equation.Then we compare these three methods Is used to calculate the charge transfer rate of organic semiconductor materials. The results show that the Ehrenfest method and the surface hopping method may deviate seriously from the correct results. The reason for the deviation is that the two methods do not properly handle the motion of the coherent item, To high-frequency mode is even more serious.