Correlated Light-Matter Interactions in Picocavities and Cavity QED

In recent years, research at the interface of chemistry, material science, and quantum optics has surged and opened new possibilities to study ultra-strong light-matter interactions. Besides collective strong coupling of many molecules for cavity-QED systems, recent experiments have demonstrated strong light-matter coupling in the single molecule regime for plasmonic picocavities [1]. In this talk, we show how such cavity optomechanical systems can alter chemical reactions such as photochemistry [2] using the methods of cavity Born-Oppenheimer approximation (CBOA) [3] and quantum-electrodynamical density functional theory (QEDFT) [4]. We will also discuss how phonons are formally included in QEDFT to predict new single molecule - cavity optomechanical effects.

[1] F. Benz et al., Science, 354 6313, 726-729 (2016).
[2] J. Flick, P. Narang, work in progress.
[3] J. Flick, et al. J. Chem. Theory Comput., 13 4, 1616-1625 (2017).
[4] M. Ruggenthaler et al., Phys. Rev. A 90, 012508 (2014).