Univ. Grenoble Alpes, CNRS, Inst NEEL, F-38042 Grenoble, France.
Chem Soc Rev. 2018 Feb 5;47(3):1022-1043. doi: 10.1039/c7cs00049a.
We review the many-body Green's function Bethe-Salpeter equation (BSE) formalism that is rapidly gaining importance for the study of the optical properties of molecular organic systems. We emphasize in particular its similarities and differences with time-dependent density functional theory (TD-DFT), both methods sharing the same formal O(N) computing time scaling with system size. By comparison with higher level wavefunction based methods and experimental results, the advantages of BSE over TD-DFT are presented, including an accurate description of charge-transfer states and an improved accuracy for the challenging cyanine dyes. We further discuss the models that have been developed for including environmental effects. Finally, we summarize the challenges to be faced so that BSE reaches the same popularity as TD-DFT.
我们回顾了多体格林函数贝塞尔-萨尔皮特方程（BSE）形式，该形式对于研究分子有机体系的光学性质正变得越来越重要。我们特别强调了它与含时密度泛函理论（TD-DFT）的相似性和不同之处，这两种方法都具有相同的与系统大小成比例的 O(N)计算时间复杂度。通过与更高阶的基于波函数的方法和实验结果进行比较，展示了 BSE 相对于 TD-DFT 的优势，包括对电荷转移态的准确描述以及对挑战性的花菁染料的准确性提高。我们进一步讨论了为包括环境效应而开发的模型。最后，我们总结了 BSE 需要面对的挑战，以便它能像 TD-DFT 一样普及。
