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arXiv:1804.01816 · Physical review. B./Physical review. B

Vacuum-enhanced optical nonlinearities with disordered molecular photoswitches

Marina Litinskaya, Felipe Herrera

Published Jan 10, 2019• 11 citations
arXivHTMLPDF

Abstract

It is well known that nonlinear optical signals such as cross-phase modulation can be coherently enhanced in multilevel atomic gases under conditions of electromagnetically induced transparency, but analogous results in solids are challenging to obtain due to natural energetic disorder. We propose a solid-state cavity QED scheme to enable cross-phase modulation between two arbitrarily weak classical fields in the optical domain, using a highly disordered intracavity medium composed of organic molecular photoswitches. Even in the presence of strong energetic and orientational disorder, the unique spectral properties of organic photoswitches can be used to enhance the desired nonlinearity under conditions of vacuum-induced transparency, enabling cross-phase modulation signals that surpass the detection limit imposed by absorption losses. Possible applications of the scheme include integrated all-optical switching with low photon numbers.

DOI
10.1103/physrevb.99.041107

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It is well known that nonlinear optical signals such as cross-phase modulation can be coherently enhanced in multilevel atomic gases under conditions of electromagnetically induced transparency, but analogous results in solids are challenging to obtain due to natural energetic disorder. We propose a solid-state cavity QED scheme to enable cross-phase modulation between two arbitrarily weak classical fields in the optical domain, using a highly disordered intracavity medium composed of organic molecular photoswitches. Even in the presence of strong energetic and orientational disorder, the unique spectral properties of organic photoswitches can be used to enhance the desired nonlinearity under conditions of vacuum-induced transparency, enabling cross-phase modulation signals that surpass the detection limit imposed by absorption losses. Possible applications of the scheme include integrated all-optical switching with low photon numbers.
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 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/cm2 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.
Strong coupling with single molecules in plasmonic picocavities has emerged as a resource for room-temperature quantum control with nanoscale light. Tip-based nanoprobes can measure the local dynamics of individual molecular picocavities, but the overhead associated with sampling an inhomogeneous picocavity distribution can be challenging for scalability. We propose a macroscopic approach in which an ensemble of molecular picocavities acts as a nonlinear plasmonic metamaterial. Using a quantum optics perspective, we study theoretical performance limits for optical cross-phase modulation in the system, taking into account realistic distributions of picocavity volumes and molecular transition frequencies. The medium nonlinearity is mediated by local strong coupling with the lowest vibronic emission sideband of individual organic chomophores. The local vacua change the refractive index of the medium at the frequency of a weak probe field ωp\omega_pωp​, set to drive the bare zero-phonon absorption band. Refractive index variations Δn/n\Delta n/nΔn/n of a few percent, relative to a molecule-free scenario, are feasible with dilute ensembles. The probe phase evolution can be switched off in the presence of a signal field at a higher frequency ωs\omega_sωs​, for intensities as low as 10 kW/cm2^22. The mechanism for optical switching involves a novel (ωp+ωs\omega_p+\omega_sωp​+ωs​) two-photon absorption channel, assisted by local vacuum fields. Our work paves the way for future studies of plasmonic metamaterials that exploit strong light-molecule interactions, for applications in optical state preparation and control.
By mapping photons into the sample of cuprous oxide with Rydberg excitons, it is possible to obtain a significant optical phase shift due to third-order cross-Kerr nonlinearities realized under the conditions of electromagnetically induced transparency. The optimum conditions for observation of the phase shift over π in Rydberg excitons media are examined. A discussion of the application of the cross-phase modulations in the field of all-optical quantum information processing in solid-state systems is presented.
Weak-light all-optical switches would enhance photonics capabilities and enable important optical quantum information processing tasks, but optical switching based on third-order optical nonlinearity is proving to be elusive and controversial. I discuss strategies to generate large cross-phase modulation by combining double electromagnetically induced transparency, competing atomic transitions, electron population engineering for pulse speed control, and using boundary conditions to confine the transverse field beyond the diffraction limit.
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 NNN 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.