Towards polaritonic molecular orbitals for large molecular systems

TL;DR

This paper introduces two second-order algorithms that improve the computational efficiency of modeling large molecular systems in quantum electrodynamics environments, enabling better understanding of electron-photon interactions.

Contribution

The work presents novel second-order algorithms that reduce computational costs in QED Hartree-Fock theory, facilitating the study of larger molecules in strong coupling regimes.

Findings

Reduced computational requirements for large molecular systems

Enhanced convergence in QED Hartree-Fock calculations

Foundation for developing correlated methods in QED environments

Abstract

A comprehensive theoretical 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.