Absolute energy levels of liquid water from many-body perturbation theory with effective vertex corrections

• 成果类型: Article
• 署名作者: Tal, Alexey; Bischoff, Thomas; Pasquarello, Alfredo
• 署名单位: Swiss Federal Institutes of Technology Domain; Ecole Polytechnique Federale de Lausanne
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-10720
• DOI: 10.1073/pnas.2311472121
• 发表日期: 2024-03-05
• 关键词: magnetic-structure; spin polarization; analog

摘要

We demonstrate the importance of addressing the F vertex and thus going beyond the GW approximation for achieving the energy levels of liquid water in manybody perturbation theory. In particular, we consider an effective vertex function in both the polarizability and the self -energy, which does not produce any computational overhead compared with the GW approximation. We yield the band gap, the ionization potential, and the electron affinity in good agreement with experiment and with a hybrid functional description. The achieved electronic structure and dielectric screening further lead to a good description of the optical absorption spectrum, as obtained through the solution of the Bethe-Salpeter equation. In particular, the experimental peak position of the exciton is accurately reproduced.