Journal
ACS PHOTONICS
Volume 7, Issue 4, Pages 975-990Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsphotonics.9b01649
Keywords
ab initio quantum electrodynamics; strong light-matter coupling; electronic structure; polaritonic chemistry; quantum optics
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Funding
- European Research Council [ERC-2015-AdG694097]
- Cluster of Excellence Advanced Imaging of Matter (AIM), Grupos Consolidados [IT1249-19]
- Federal Ministry of Education and Research [RouTe-13N14839]
- Light Induced Dynamics and Control of Correlated Quantum Systems [SFB925]
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Experiments at the interface of quantum optics and chemistry have revealed that strong coupling between light and matter can substantially modify the chemical and physical properties of molecules and solids. While the theoretical description of such situations is usually based on nonrelativistic quantum electrodynamics, which contains quadratic light-matter coupling terms, it is commonplace to disregard these terms and restrict the treatment to purely bilinear couplings. In this work, we clarify the physical origin and the substantial impact of the most common quadratic terms, the diamagnetic and self-polarization terms, and highlight why neglecting them can lead to rather unphysical results. Specifically, we demonstrate their relevance by showing that neglecting these terms leads to the loss of gauge invariance, basis set dependence, disintegration (loss of bound states) of any system in the basis set limit, unphysical radiation of the ground state, and an artificial dependence on the static dipole. Besides providing important guidance for modeling of strongly coupled light-matter systems, the presented results also indicate conditions under which those effects might become accessible.
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