Simple Exchange-Correlation Energy Functionals for Strongly Coupled Light-Matter Systems based on the Fluctuation-Dissipation Theorem (2104.06980v1)

Abstract: Recent experimental advances in strongly coupled light-matter systems has sparked the development of general ab-initio methods capable of describing interacting light-matter systems from first principles. One of these methods, quantum-electrodynamical density-functional theory (QEDFT), promises computationally efficient calculations for large correlated light-matter systems with the quality of the calculation depending on the underlying approximation for the exchange-correlation functional. So far no true density-functional approximation has been introduced limiting the efficient application of the theory. In this paper, we introduce the first gradient-based density functional for the QEDFT exchange-correlation energy derived from the adiabatic-connection fluctuation-dissipation theorem. We benchmark this simple-to-implement approximation on small systems in optical cavities and demonstrate its relatively low computational costs for fullerene molecules up to C$_{180}$ coupled to 400,000 photon modes in a dissipative optical cavity. This work now makes first principle calculations of much larger systems possible within the QEDFT framework effectively combining quantum optics with large-scale electronic structure theory.