Quantum Nonlinear Optics with Polar J-Aggregates in Microcavities.
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.
†Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States.
Felipe
F
Herrera
†Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States.
Borja
B
Peropadre
†Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States.|‡Grupo de Fı́sica Atómica y Molecular, Instituto de Fı́sica, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellı́n, Colombia.
Leonardo A
LA
Pachon
†Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States.|¶Institute of Physics, Kazan Federal University, 18 Kremlevskaya Street, Kazan 420008, Russian Federation.
Semion K
SK
Saikin
†Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States.
Alán
A
Aspuru-Guzik
J-aggregates; cavity-QED; electromagnetically induced transparency; optical microcavity; quantum nonlinear optics