用前向和后向随机波函数计算相干二维电子谱
Calculations of coherent two-dimensional electronic spectra using forward and backward stochastic wavefunctions
摘要：
本文在已有的光学响应函数理论基础上，提出了一种新的方法，其核心思想是分段求解前后向随机薛定谔方程，从而精确地获得二维电子光谱。基于简单的激子耦合二聚体模型系统，详细论证了所提出方案的有效性和效率，并与确定性的运动方程和微扰的二阶无时间卷积量子主方程进行了比较.此外，本文还指出，过阻尼环境的特征频率是影响二维电子光谱中振荡信号寿命和系统动力学量子相干性特征的一个极其重要的因素。值得注意的是，所提出的方案受益于其随机性和波函数框架和许多其他优点，大大减少了数值成本，有很大的潜力，系统地研究各种量子效应在现实的大规模自然和人工光合系统中观察到的。
英文摘要：
Within the well-established optical response function formalism, a new strategy with the central idea of employing the forward-backward stochastic Schrödinger equations in a segmented way to accurately obtain the two-dimensional (2D) electronic spectrum is presented in this paper. Based on the simple excitonically coupled dimer model system, the validity and efficiency of the proposed schemes are demonstrated in detail, along with the comparison against the deterministic hierarchy equations of motion and perturbative second order time-convolutionless quantum master equations. In addition, an important insight is provided in this paper that the characteristic frequency of the overdamped environment is an extremely crucial factor to regulate the lifetimes of the oscillating signals in 2D electronic spectra and of quantum coherence features of system dynamics. It is worth noting that the proposed scheme benefiting from its stochastic nature and wavefunction framework and many other advantages of substantially reducing the numerical cost, has a great potential to systematically investigate various quantum effects observed in realistic large-scale natural and artificial photosynthetic systems.
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