论文标题
超出等离子底近似值的伯特 - 盐蛋白方程的动力校正
Dynamical Correction to the Bethe-Salpeter Equation Beyond the Plasmon-Pole Approximation
论文作者
论文摘要
伯特盐盐方程（BSE）形式主义是一种计算负担得起的方法，用于计算分子系统中准确的光激发能。与时间相关密度功能功能理论的无处不在的绝热近似相似，静态近似在BSE形式主义的大多数实现中通常会实现动态（即频率依赖性）内核的静态近似。在这里，除了静态近似之外，我们通过对静态BSE激发能进行了重新归一化的一阶扰动校正，计算了分子激发能的电子孔筛选的动力校正。由于库仑相互作用的动态筛选精确地计算在随机相近似中，因此目前的动态校正超出了等离子极近似值。我们的计算是针对高级（耦合群集）计算的基准测试的，从而可以评估SINGLET和TRIPLET光学转变的动态校正带来的明显改进。
The Bethe-Salpeter equation (BSE) formalism is a computationally affordable method for the calculation of accurate optical excitation energies in molecular systems. Similar to the ubiquitous adiabatic approximation of time-dependent density-functional theory, the static approximation, which substitutes a dynamical (i.e., frequency-dependent) kernel by its static limit, is usually enforced in most implementations of the BSE formalism. Here, going beyond the static approximation, we compute the dynamical correction of the electron-hole screening for molecular excitation energies thanks to a renormalized first-order perturbative correction to the static BSE excitation energies. The present dynamical correction goes beyond the plasmon-pole approximation as the dynamical screening of the Coulomb interaction is computed exactly within the random-phase approximation. Our calculations are benchmarked against high-level (coupled-cluster) calculations, allowing to assess the clear improvement brought by the dynamical correction for both singlet and triplet optical transitions.
