Kubota Yoji, Nobusada Katsuyuki
Department of Theoretical and Computational Molecular Science, Institute for Molecular Science, Myodaiji, Okazaki 444-8585, Japan.
J Chem Phys. 2008 Sep 7;129(9):094704. doi: 10.1063/1.2975328.
We discuss differences between eigenbasis and site basis representations for models of exciton transfers in an array of quantum dots. The exciton relaxation processes are well described by the master equation in the eigenbasis representation. The site basis evolution equation up to the second order of the interdot interaction is straightforwardly derived from the eigenbasis equation by using perturbation theory when the interaction is sufficiently small compared to the energy difference between the exciton states in each quantum dot. Although the higher order site basis equations can be derived similarly, the resultant equations are too complicated to use in the actual calculations. The master equation in the eigenbasis representation has several advantages over the site basis one: (i) the system described in terms of the eigenbasis representation can evolve into thermal equilibrium because the equation satisfies the detailed balance, (ii) the site basis equation does not reasonably describe the exciton state trapped in a local energy minimum at very low temperature, and (iii) it is computationally less demanding to carry out the eigenbasis evolution equation.
我们讨论了量子点阵列中激子转移模型在本征基和位点基表示之间的差异。在本征基表示中,激子弛豫过程可以通过主方程很好地描述。当点间相互作用与每个量子点中激子态之间的能量差相比足够小时,利用微扰理论可以直接从本征基方程推导出位点基演化方程到点间相互作用的二阶项。虽然可以类似地推导出高阶位点基方程,但所得方程过于复杂,无法用于实际计算。本征基表示中的主方程比位点基表示具有几个优点:(i)用本征基表示描述的系统可以演化到热平衡,因为该方程满足细致平衡;(ii)位点基方程不能合理地描述在非常低的温度下被困在局部能量最小值处的激子态;(iii)进行本征基演化方程的计算要求较低。