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arXiv 2106.09587cond-mat.mtrl-sci
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激子效应对固体三阶非线性光学性质的影响:理论与应用

Excitonic effects on the third-order nonlinear optical properties of solids: Theory and application

You-Zhao Lan

摘要:

本文提出了一种基于多体Bethe-Salpeter方程本征态的态求和方法来计算固体的线性和非线性光学性质。计算中包括激子和局部场效应。作为应用,我们计算了固体C_(60)富勒烯的单光子吸收、三次谐波产生和简并四波混频光谱。理论和实验结果之间的总体协议是非常好的所有三个计算的光谱。通过与基于独立粒子近似的态求和方法的比较,我们发现激子效应将独立粒子跃迁峰混合成新的激子跃迁峰。光谱峰的位置和强度被显著改变。通过跟踪态求和过程,确定了三次谐波特征峰的非线性极化共振类型,从而消除了两个实验结果的差异。

英文摘要:

We present a many-body Bethe-Salpeter equation eigenstates based sum-over-states method to calculate the linear and nonlinear optical properties of solids. Excitonic and local field effects are included in the calculations. As applications, we calculate the one-photon absorption, third harmonic generation, degenerate four-wave mixing spectra of solid C60 fullerene. The overall agreement between the theoretical and experimental results is very good for all three calculated spectra. By comparisons with the independent particle approximation based sum-over-states method, we show that excitonic effects mix the independent particle transition peaks to new excitonic ones. The position and intensity of spectral peaks are modified significantly. By tracing the sum-over-states progress, we determine the type of nonlinear polarization resonances for the characteristic peaks of third harmonic generation process, which may clear up a discrepancy in two experimental results.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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