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 multiphoton processes. Furthermore, a path on how to incorporate our bosonic extension of coupled-cluster theory into existing quantum chemistry programs is given.
- Publication:
-
Physical Review Research
- Pub Date:
- June 2020
- DOI:
- 10.1103/PhysRevResearch.2.023262
- arXiv:
- arXiv:1909.02401
- Bibcode:
- 2020PhRvR...2b3262M
- Keywords:
-
- Physics - Chemical Physics;
- Quantum Physics
- E-Print:
- 9 pages, 6 figures