El Moutaoukal Yassir, Riso Rosario R, Castagnola Matteo, Koch Henrik
Department of Chemistry, Norwegian University of Science and Technology, 7491 Trondheim, Norway.
J Chem Theory Comput. 2024 Oct 22;20(20):8911-8920. doi: 10.1021/acs.jctc.4c00808. Epub 2024 Sep 30.
A comprehensive understanding of electron-photon correlation is essential for describing the reshaping of molecular orbitals in quantum electrodynamics (QED) environments. The strong coupling QED Hartree-Fock (SC-QED-HF) theory tackles these aspects by providing consistent molecular orbitals in the strong coupling regime. The previous implementation, however, has significant convergence issues that limit the applicability. In this work, we introduce two second-order algorithms that significantly reduce the computational requirements, thereby enhancing the modeling of large molecular systems in QED environments. Furthermore, the implementation will enable the development of correlated methods based on a reliable molecular orbital framework as well as multi-level methodologies able to model the inclusion of solvent effects in this kind of complex systems.
全面理解电子 - 光子相关性对于描述量子电动力学（QED）环境中分子轨道的重塑至关重要。强耦合QED哈特里 - 福克（SC-QED-HF）理论通过在强耦合 regime 中提供一致的分子轨道来处理这些方面。然而，先前的实现存在严重的收敛问题，限制了其适用性。在这项工作中，我们引入了两种二阶算法，显著降低了计算需求，从而增强了在QED环境中对大分子系统的建模。此外，该实现将能够基于可靠的分子轨道框架开发相关方法，以及能够对这类复杂系统中溶剂效应的纳入进行建模的多级方法。
