Abstract
We develop coupled-cluster theory for systems of electrons strongly coupled to photons, providing a promising theoretical tool in polaritonic chemistry with a perspective of application to all types of fermion-boson coupled systems. We show benchmark results for model molecular Hamiltonians coupled to cavity photons. By comparing to full configuration interaction results for various ground-state properties and optical spectra, we demonstrate that our method captures all key features present in the exact reference, including Rabi splittings and multi-photon processes. Further, a path on how to incorporate our bosonic extension of coupled-cluster theory into existing quantum chemistry programs is given.
Highlights
In recent years seminal experiments at the interface between quantum optics, quantum chemistry, and material sciences have shown that when photons and matter couple strongly the emergence of light-matter hybrid states, called polaritons, can substantially change chemical and physical properties of molecular systems [1,2,3,4,5,6,7,8,9]
We have shown that subtle light-matter correlations that appear in strong and ultrastrong cavity experiments can be captured in the framework of CC theory, paving the way for high-accuracy modeling and interpretation of experiments in these regimes
This work has focused on model systems, extension to real ab initio Hamiltonians is straightforward
Summary
In recent years seminal experiments at the interface between quantum optics, quantum chemistry, and material sciences have shown that when photons and matter couple strongly the emergence of light-matter hybrid states, called polaritons, can substantially change chemical and physical properties of molecular systems [1,2,3,4,5,6,7,8,9].
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