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Dynamical correction to the Bethe-Salpeter equation beyond the plasmon-pole approximation.
The Journal of Chemical Physics ( IF 4.4 ) Pub Date : 2020-09-21 , DOI: 10.1063/5.0023168
Pierre-François Loos 1 , Xavier Blase 2
Affiliation  

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 one to assess the clear improvement brought by the dynamical correction for both singlet and triplet optical transitions.

中文翻译:

对Bethe-Salpeter方程的动态校正超出了等离激元极点近似。

Bethe–Salpeter方程(BSE)形式主义是计算分子系统中精确的光激发能的一种计算上可承受的方法。类似于随时间变化的密度泛函理论的绝热逼近,静态逼近通常由BSE形式主义的大多数实现方式强制执行,该静态逼近以其静态极限替代了动态(即与频率相关)的内核。在这里,除了静态逼近以外,我们还对分子激发能的电子-空穴筛选进行了动态校正,这要归功于对静态BSE激发能的重新规范化的一阶扰动校正。由于精确地在随机相位近似内计算了库仑相互作用的动态筛选,因此当前的动力学校正超出了等离子极近似。我们的计算以高水平(耦合集群)计算为基准,从而使我们能够评估由单态和三态光学跃迁的动态校正带来的明显改善。
更新日期:2020-09-21
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