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arXiv · 1909.02401

Polaritonic Coupled-Cluster Theory

Uliana Mordovina·Callum Bungey·Heiko Appel·Peter J. Knowles·Angel Rubio·Frederick R. Manby
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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.

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Uliana Mordovina, Callum Bungey, Heiko Appel, Peter J. Knowles, Angel Rubio, Frederick R. Manby. 2019-09-05. Polaritonic Coupled-Cluster Theory. https://doi.org/10.1103/physrevresearch.2.023262

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