Cavity Born-Oppenheimer Approximation for Correlated Electron-Nuclear-Photon Systems

Journal Of Chemical Theory And Computation 13 (4), 1616 - 1625 (2017)

Cavity Born-Oppenheimer Approximation for Correlated Electron-Nuclear-Photon Systems

Johannes Flick,Heiko Appel,Michael Ruggenthaler,, Angel Rubio

In this work, we illustrate the recently introduced concept of the cavity Born- Oppenheimer approximation1 for correlated electron-nuclear-photon problems in detail. We demonstrate how an expansion in terms of conditional electronic and photon-nuclear wave functions accurately describes eigenstates of strongly correlated light-matter systems. For a GaAs quantum ring model in resonance with a photon mode we highlight how the ground-state electronic potential-energy surface changes the usual harmonic potential of the free photon mode to a dressed mode with a double-well structure. This change is accompanied by a splitting of the electronic ground-state density. For a model where the photon mode is in resonance with a vibrational transition, we observe in the excited-state electronic potential-energy surface a splitting from a single minimum to a double minimum. Furthermore, for a time-dependent setup, we show how the dynamics in correlated light-matter systems can be understood in terms of population transfer between potential energy surfaces. This work at the interface of quantum chemistry and quantum optics paves the way for the full ab-initio description of matter-photon systems.

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http://dx.doi.org/10.1021/acs.jctc.6b01126
Notes
We would like to thank C. Schafer for a careful reading of the manuscript, and MR acknowledges insightful discussions with F.G. Eich. In addition, we thank the referees for contributingto signi cant improvements in the manuscript. We acknowledge nancial support from the European Research Council (ERC-2015-AdG-694097), Grupos Consolidados (IT578-13), by the European Union's H2020 program under GA no.676580 (NOMAD), COST Action MP1306 (EUSpec) and the Austrian Science Fund (FWF P25739-N27).

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