Polaritonic Coupled-Cluster Theory

Physical Review Research 2, 2, 023262 (2020)

Polaritonic Coupled-Cluster Theory

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

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 groundstate 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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Preprint - 1.49 MB
The authors thank M. Ruggenthaler and C. Schäfer for helpful discussions. The authors are grateful to EPSRC (EP/R014493/1 and EP/R014183/1)and to the European Research Council (ERC-2015-AdG-694097) for funding. UM is supported through IMPRS-UFAST. CB is supported through the EPSRC TMCS Centre for Doctoral Training (EP/L015722/1). The Flatiron Institute is a division of the Simons Foundation.

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