论文标题

非线性光谱镜的自动Feynman图生成

Automatic Feynman diagram generation for nonlinear optical spectroscopies

论文作者

Rose, Peter A., Krich, Jacob J.

论文摘要

扰动非线性光谱镜是了解激子和其他冷凝相系统动力学的强大方法。长期以来,Feynman图提供了理解和解释实验光谱并组织模型系统光谱的计算的必要工具。当严格按时排序光学脉冲时,只有少量图会造成任何贡献,但是在许多实验中,脉冲叠加效应对于解释结果很重要。当脉冲重叠时,贡献图的数量可能会迅速增加,尤其是在高阶光谱中,并且在尝试写下所有图表时,人为错误尤其可能。我们提出了一个自动图生成器(DG),该发生器生成了计算任何$ n^{\ text {th}} $ - 订购光谱信号所需的所有Feynman图。我们通过相关的相位歧视条件以及脉冲幅度非零的时间间隔来表征所有扰动非线性光谱。尽管DG可用于自动化冲动计算,但其最大的强度在于自动化脉冲重叠很重要的有限脉冲计算。我们考虑三阶瞬态吸收光谱和五阶激子相互作用2D(EEI2D)光谱法,当脉冲重叠时,在冲动性极限的6或7个图中分别由6或7个图表描述。 DG允许用户以相对较低的计算成本自动包含所有相关图,因为额外的图仅是针对相关的脉冲延迟生成的。对于EEI2D光谱,我们显示了包括重叠图的重要效果。

Perturbative nonlinear optical spectroscopies are powerful methods to understand the dynamics of excitonic and other condensed phase systems. Feynman diagrams have long provided the essential tool to understand and interpret experimental spectra and to organize the calculation of spectra for model systems. When optical pulses are strictly time ordered, only a small number of diagrams contribute, but in many experiments pulse-overlap effects are important for interpreting results. When pulses overlap, the number of contributing diagrams can increase rapidly, especially with higher order spectroscopies, and human error is especially likely when attempting to write down all of the diagrams. We present an automated Diagram Generator (DG) that generates all of the Feynman diagrams needed to calculate any $n^{\text{th}}$-order spectroscopic signal. We characterize all perturbative nonlinear spectroscopies by their associated phase-discrimination condition as well as the time intervals where pulse amplitudes are nonzero. Although the DG can be used to automate impulsive calculations, its greatest strength lies in automating finite pulse calculations where pulse overlaps are important. We consider third-order transient absorption spectroscopy and fifth-order exciton-exciton interaction 2D (EEI2D) spectroscopy, which are respectively described by 6 or 7 diagrams in the impulsive limit but 16 or 240 diagrams, respectively, when pulses overlap. The DG allows users to automatically include all relevant diagrams at relatively low computational cost, since the extra diagrams are only generated for the inter-pulse delays where they are relevant. For EEI2D spectroscopy, we show the important effects of including the overlap diagrams.

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