Quantum nonlinear optics with polar J-aggregates in microcavities

Abstract: We show that an ensemble of organic dye molecules with permanent electric dipole moments embedded in a microcavity can lead to strong optical nonlinearities at the single photon level. The strong long-range electrostatic interaction between chromophores due to their permanent dipoles introduces the desired nonlinearity of the light-matter coupling in the microcavity. We obtain the absorption spectra of a weak probe field under the influence of strong exciton-photon coupling with the cavity field. Using realistic parameters, we demonstrate that a single cavity photon can significantly modify the absorptive and dispersive response of the medium to a probe photon at a different frequency. Finally, we show that the system is in the regime of cavity-induced transparency with a broad transparency window for dye dimers. We illustrate our findings using pseudoisocyanine chloride (PIC) J-aggregates in currently-available optical microcavities.