Atoms and Molecules in Cavities: From Weak to Strong Coupling in QED Chemistry

Proceedings Of The National Academy Of Sciences Of The United States Of America 114, 3026 - 3034 (2017)

Atoms and Molecules in Cavities: From Weak to Strong Coupling in QED Chemistry

Johannes Flick,Michael Ruggenthaler,Heiko Appel, Angel Rubio

In this work, we provide an overview of how well-established concepts in the fields of quantum chemistry and material sciences have to be adapted when the quantum nature of light becomes important in correlated matter-photon problems. Therefore, we analyze model systems in optical cavities, where the matter-photon interaction is considered from the weak- to the strong coupling limit and for individual photon modes as well as for the multi-mode case. We identify fundamental changes in Born-Oppenheimer surfaces, spectroscopic quantities, conical intersections and efficiency for quantum control. We conclude by applying our novel recently developed quantum-electrodynamical density-functional theory [1, 2] to single-photon emission and show how a straightforward approximation accurately describes the correlated electron-photon dynamics. This paves the road to describe matter-photon interactions from first-principles and addresses the emergence of new states of matter in chemistry and material science.

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Preprint - 1.87 MB
We acknowledges financial support from the European Research Council(ERC-2015-AdG-694097), Spanish grant (FIS2013-46159-C3-1-P), Grupos Consolidados (IT578-13), and AFOSR Grant No. FA2386- 15-1-0006 AOARD 144088, H2020-NMP-2014 project MOSTOPHOS (GA no. 646259) and COST Action MP1306 (EUSpec) and the Austrian Science Foundation (FWF P25739-N27).

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