Disordered ensembles of strongly coupled single-molecule plasmonic picocavities as nonlinear optical metamaterials
arXiv:2104.00852 · doi:10.1063/5.0080063
Abstract
We propose to use molecular picocavity ensembles as macroscopic coherent nonlinear optical devices enabled by nanoscale strong coupling. For a generic picocavity model that includes molecular and photonic disorder, we derive theoretical performance bounds for coherent cross-phase modulation signals using weak classical fields of different frequencies. We show that strong coupling of the picocavity {\it vacua} with a specific vibronic sideband in the molecular emission spectrum results in a significant variation of the effective refractive index of the metamaterial relative to a molecule-free scenario, due to a vacuum-induced Autler-Townes effect. For a realistic molecular disorder model, we demonstrate that cross-phase modulation of optical fields as weak as 10 kW/cm is feasible using dilute ensembles of molecular picocavities at room temperature, provided that the confined vacuum is not resonantly driven by the external probe field}. Our work paves the way for the development of plasmonic metamaterials that exploit strong coupling for optical state preparation and quantum control.
arXiv comment13 pages, 7 figs, 3 appendices
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- Exact Results for the Tavis-Cummings and Hckel Hamiltonians with Diagonal Disorder