固体吸收光谱的周期性运动方程耦合团簇理论
Absorption Spectra of Solids from Periodic Equation-of-Motion Coupled-Cluster Theory
摘要：
本文采用基于高斯的周期性运动方程耦合团簇单激发和双激发理论（EOM-CCSD）计算了六种三维半导体和绝缘体的吸收光谱。通过求解每个频率下的线性方程组，可以有效地计算光谱，从而在没有明确列举激发态的情况下获得数十eV的能量范围。我们评估了布里渊区采样的影响，由于EOM-CCSD的成本，很难实现收敛。虽然我们最收敛的光谱表现出的线形与实验吻合得很好，它们均匀地移动到更高的能量约1 eV。我们暂时将这种差异归因于振动效应和剩余电子相关性的结合，即，三重激励及以上。
英文摘要：
We present ab initio absorption spectra of six three-dimensional semiconductors and insulators calculated using Gaussian-based periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). The spectra are calculated efficiently by solving a system of linear equations at each frequency, giving access to an energy range of tens of eV without explicit enumeration of excited states. We assess the impact of Brillouin zone sampling, for which it is hard to achieve convergence due to the cost of EOM-CCSD. Although our most converged spectra exhibit lineshapes that are in good agreement with experiment, they are uniformly shifted to higher energies by about 1 eV. We tentatively attribute this discrepancy to a combination of vibrational effects and the remaining electron correlation, i.e., triple excitations and above.
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