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arXiv:1409.1930 · The Journal of Physical Chemistry Letters

Quantum Nonlinear Optics with Polar J-Aggregates in Microcavities

Felipe Herrera, Borja Peropadre, Leonardo A. Pachón, Semion K. Saikin, Alán Aspuru‐Guzik

Published Oct 7, 2014• 44 citations
arXivHTMLPDF

Abstract

We predict 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 develop a semiclassical model to 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 cavity field with an average photon number near unity can significantly modify the absorptive and dispersive response of the medium to a weak probe field 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.

DOI
10.1021/jz501905h

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Results of coherent transients of pseudoisocyanine J aggregates in distributed feedback microcavities are reported. Under resonant excitation of the cavity-mode observed at the low energy side of the excitonic resonance, the response time is less than 1 ps, approximately equal to the pump pulse duration. We find an enhancement of the optical nonlinearity by one-order of magnitude in the microcavity. The excitation of the cavity-mode is effective in enhancing the nonlinearity with ultrafast response.
Summary form only given. The interaction between light and matter can be significantly altered by placing the material in an optical microcavity. Under appropriate conditions strong coupling may occur, a process in which the confined electromagnetic field of the microcavity dramatically modifies the optical transitions of the material, resulting in an anti-crossing (Rabi splitting) of the coupled modes of the microcavity. Recently strong coupling has been observed in organic materials including J-aggregates of cyanine dyes. They have the desired properties of large oscillator strength and narrow linewidth, and have shown large Rabi splitting at room temperature. We report here significant strong coupling in a new structure, a metal clad organic microcavity.
Abstract Control of light–matter coupling at the quantum level is an enabling technique for many emerging quantum technologies. This tutorial describes recent advances in achieving efficient coupling of light with a single molecule using an optical Fabry–Perot microcavity. We demonstrate that the efficient cavity-molecule coupling converts the molecule to an effective two-level system. In this regime, a single molecule can act as a nearly perfect reflecting mirror and exhibits optical nonlinearity at the ultimate level of single photons.