A variety of stimulated nonlinear optical processes are observed under relatively low intensity cw excitation in droplet spherical microcavities. These include stimulated Raman and Rayleigh-wing scattering as well as four-wave parametric oscillation. The low thresholds for these stimulated processes are accounted for by all waves being in resonance with high- $Q$ droplet modes and by the existence of a significant cavity QED enhancement (> 100 times) in the nonlinear gain coefficients.A variety of stimulated nonlinear optical processes are observed under relatively low intensity cw excitation in droplet spherical microcavities. These include stimulated Raman and Rayleigh-wing scattering as well as four-wave parametric oscillation. The low thresholds for these stimulated processes are accounted for by all waves being in resonance with high-$Q$ droplet modes and by the existence of a significant cavity QED enhancement (> 100 times) in the nonlinear gain coefficients.

Physical Review LettersOct 31, 1994122 citations

Optical Processes In Microcavities

Advanced series in applied physicsJan 1, 1996142 citations

Microcavity-quality-factor enhancement using nonlinear effects close to the bistability threshold and coherent population oscillations

Yannick Dumeige, Alejandro M. Yacomotti, P. Grinberg +3 more

We analytically show that inserting a driven, two-level system inside a microcavity can improve its optical properties. In this approach, the strong dispersion induced by a pump via population oscillations increases the cavity lifetime experienced by a slightly detuned probe. We further predict that if the cavity is pumped through a resonant channel, optical absorptive or dispersive bistability can be combined with the population-oscillation-induced steep material dispersion to obtain a strong quality-factor enhancement. Moreover, differential amplification coming from the nonlinear feature of the pump transfer function can be used to drastically increase the probe transmission beyond intrinsic characteristics of the resonator. The $Q$ -factor enhancement and the differential amplification can be advantageously combined with a frequency pulling effect to stabilize or readjust the microcavity resonance frequency.We analytically show that inserting a driven, two-level system inside a microcavity can improve its optical properties. In this approach, the strong dispersion induced by a pump via population oscillations increases the cavity lifetime experienced by a slightly detuned probe. We further predict that if the cavity is pumped through a resonant channel, optical absorptive or dispersive bistability can be combined with the population-oscillation-induced steep material dispersion to obtain a strong quality-factor enhancement. Moreover, differential amplification coming from the nonlinear feature of the pump transfer function can be used to drastically increase the probe transmission beyond intrinsic characteristics of the resonator. The $Q$-factor enhancement and the differential amplification can be advantageously combined with a frequency pulling effect to stabilize or readjust the microcavity resonance frequency.

Physical Review AJun 21, 201213 citations

Enhanced optical nonlinearities under collective strong light-matter coupling

Raphael F. Ribeiro, Jorge A. Campos-Gonzalez-Angulo, Noel C. Giebink +2 more

Optical microcavities and metallic nanostructures have been shown to significantly modulate the dynamics and spectroscopic response of molecular systems. We present a study of the nonlinear optics of a model consisting of $N$ anharmonic multilevel systems (e.g., Morse oscillators) undergoing collective strong coupling with a resonant infrared microcavity. We find that, under experimentally accessible conditions, molecular systems in microcavities may have nonlinear phenomena significantly intensified due to the high quality of polariton resonances and the enhanced microcavity electromagnetic energy density relative to free space. Particularly large enhancement of multiphoton absorption happens when multipolariton states are resonant with bare molecule multiphoton transitions. In particular, our model predicts two-photon absorption cross-section enhancements by several orders of magnitude relative to free space when the Rabi splitting ${\mathrm{\ensuremath{\Omega}}}_{R}$ is approximately equal to the molecular anharmonic shift $2\mathrm{\ensuremath{\Delta}}$. Our results provide rough upper bounds to resonant nonlinear-response enhancement factors as relaxation to dark states is treated phenomenologically. Notably, ensembles of two-level systems undergoing strong coupling with a cavity (described by the Tavis-Cummings model) show no such optical nonlinearity enhancements, highlighting the rich phenomenology afforded by multilevel anharmonic systems. Similar conclusions are expected to hold for excitonic systems that share features with our model (e.g., molecular dyes with accessible ${S}_{0}\ensuremath{\rightarrow}{S}_{1}\ensuremath{\rightarrow}{S}_{2}$ transitions) and strongly interact with a UV-visible cavity.Optical microcavities and metallic nanostructures have been shown to significantly modulate the dynamics and spectroscopic response of molecular systems. We present a study of the nonlinear optics of a model consisting of $N$ anharmonic multilevel systems (e.g., Morse oscillators) undergoing collective strong coupling with a resonant infrared microcavity. We find that, under experimentally accessible conditions, molecular systems in microcavities may have nonlinear phenomena significantly intensified due to the high quality of polariton resonances and the enhanced microcavity electromagnetic energy density relative to free space. Particularly large enhancement of multiphoton absorption happens when multipolariton states are resonant with bare molecule multiphoton transitions. In particular, our model predicts two-photon absorption cross-section enhancements by several orders of magnitude relative to free space when the Rabi splitting ${\mathrm{\ensuremath{\Omega}}}_{R}$ is approximately equal to the molecular anharmonic shift $2\mathrm{\ensuremath{\Delta}}$. Our results provide rough upper bounds to resonant nonlinear-response enhancement factors as relaxation to dark states is treated phenomenologically. Notably, ensembles of two-level systems undergoing strong coupling with a cavity (described by the Tavis-Cummings model) show no such optical nonlinearity enhancements, highlighting the rich phenomenology afforded by multilevel anharmonic systems. Similar conclusions are expected to hold for excitonic systems that share features with our model (e.g., molecular dyes with accessible ${S}_{0}\ensuremath{\rightarrow}{S}_{1}\ensuremath{\rightarrow}{S}_{2}$ transitions) and strongly interact with a UV-visible cavity.

arXiv:2006.08519Physical Review AJun 17, 202148 citations

Q

droplet modes and by the existence of a significant cavity QED enhancement (> 100 times) in the nonlinear gain coefficients.

Q

-factor enhancement and the differential amplification can be advantageously combined with a frequency pulling effect to stabilize or readjust the microcavity resonance frequency.

N

anharmonic multilevel systems (e.g., Morse oscillators) undergoing collective strong coupling with a resonant infrared microcavity. We find that, under experimentally accessible conditions, molecular systems in microcavities may have nonlinear phenomena significantly intensified due to the high quality of polariton resonances and the enhanced microcavity electromagnetic energy density relative to free space. Particularly large enhancement of multiphoton absorption happens when multipolariton states are resonant with bare molecule multiphoton transitions. In particular, our model predicts two-photon absorption cross-section enhancements by several orders of magnitude relative to free space when the Rabi splitting ${\mathrm{\ensuremath{\Omega}}}_{R}$ is approximately equal to the molecular anharmonic shift $2\mathrm{\ensuremath{\Delta}}$. Our results provide rough upper bounds to resonant nonlinear-response enhancement factors as relaxation to dark states is treated phenomenologically. Notably, ensembles of two-level systems undergoing strong coupling with a cavity (described by the Tavis-Cummings model) show no such optical nonlinearity enhancements, highlighting the rich phenomenology afforded by multilevel anharmonic systems. Similar conclusions are expected to hold for excitonic systems that share features with our model (e.g., molecular dyes with accessible ${S}_{0}\ensuremath{\rightarrow}{S}_{1}\ensuremath{\rightarrow}{S}_{2}$ transitions) and strongly interact with a UV-visible cavity.