Calculating nonlinear response functions for multidimensional electronic spectroscopy using dyadic non-Markovian quantum state diffusion
Calculating nonlinear response functions for multidimensional electronic spectroscopy using dyadic non-Markovian quantum state diffusion
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DOI：
10.1063/5.0107925
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发表时间：
2022-09-21
影响因子：
4.4
通讯作者：
Eisfeld, Alexander
中科院分区：
文献类型：
--
作者：
Chen, Lipeng;Bennett, Doran I. G.;Eisfeld, Alexander
我们提出了一种方法来模拟多维电子光谱的分子聚集体的电子激发耦合到一个结构化的环境，使用随机非马尔可夫量子态扩散（NMQSD）方法结合微扰理论的响应函数。我们的方法的一个重要方面是，我们传播的NMQSD方程在一个双重系统的希尔伯特空间，但具有相同的噪声。我们证明，我们的方法显示出快速收敛的随机轨迹的数量，提供了一个很有前途的技术数值计算的大分子聚集体的二维电子光谱。
We present a methodology for simulating multidimensional electronic spectra of molecular aggregates with coupling of electronic excitation to a structured environment using the stochastic non-Markovian quantum state diffusion (NMQSD) method in combination with perturbation theory for the response functions. A crucial aspect of our approach is that we propagate the NMQSD equation in a doubled system Hilbert space but with the same noise. We demonstrate that our approach shows fast convergence with respect to the number of stochastic trajectories, providing a promising technique for numerical calculation of two-dimensional electronic spectra of large molecular aggregates.