Ab Initio Approaches to Simulate Molecular Polaritons and Quantum Dynamics

Molecular polaritons are hybrid states formed by the quantum mechanical interaction between light and matter. Recent experiments have shown the ability to drastically modify chemical reactions in both the ground and excited states through the hybridization of the electronic and photonic degrees of freedom. Ab initio simulations of molecular polaritons have demonstrated similar effects for simple ground and excited state reactions. However, the theoretical community has been limited in its ability to describe the complicated dynamical processes of many-molecule collective effects with a high-level treatment of all degrees of freedom within a rigorous Hamiltonian. In this review, we provide a general description and overall procedure for exploring molecular polaritons, leveraging standard many-body electronic structure calculations combined with the exact, non-relativistic quantum electrodynamics light-matter Hamiltonian.

This article is categorized under:

• Electronic Structure Theory > Ab Initio Electronic Structure Methods
• Software > Quantum Chemistry
• Structure and Mechanism > Reaction Mechanisms and Catalysis