Polaritonic Coupled-Cluster Theory

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.

9 pages, 6 figures

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Cited by in corpus (33)

• Coupled Cluster Theory for Molecular Polaritons: Changing Ground and Excited States
• A perspective on ab initio modeling of polaritonic chemistry: The role of non-equilibrium effects and quantum collectivity
• Cavity-modulated ionization potentials and electron affinities from quantum electrodynamics coupled-cluster theory
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• Enhanced diastereocontrol via strong light-matter interactions in an optical cavity
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